Systems and methods for quantum computing

Abstract

The present disclosure describes non-classical (e.g., quantum) computing systems and methods that utilize dopant molecules contained in host materials as qubits. The dopant molecules typically include ground state triplet (GST) molecules, such as carbenes or nitrogen alkenes. The host material typically includes an organic molecule. A precursor of the dopant molecule may be embedded in the host material and then subjected to ultraviolet (UV) or visible light to form a dilute molecular crystal that includes the dopant molecule embedded in the host material. The triplet levels of the dopant molecules may be manipulated using electromagnetic (EM) radiation, such as optical, radio frequency (RF), and / or microwave (MW) radiation, for non-classical computational operations.

Description

[0001] Cross-reference to related applications

[0002] This application claims priority to U.S. Provisional Patent Application No. 63 / 364,540 filed on May 11, 2022 and U.S. Provisional Patent Application No. 63 / 379,905 filed on October 18, 2022, each of which is incorporated herein by reference in its entirety for all purposes. Technical Field

[0003] The disclosed embodiments generally relate to non-classical (eg, quantum) computing systems and methods that utilize dopant molecules contained in a host material as qubits. Background Art

[0004] Non-classical computers (e.g., quantum computers) typically use quantum mechanical phenomena, such as superposition, entanglement, and interference, to perform computational operations on data. Compared to classical computers that use binary digits (bits) that always have a defined state (0 or 1), non-classical computers use quantum bits (qubits for short) that can exist in a superposition of basic states (i.e., a certain linear combination of the basic state |0> and the basic state |1>, where the basic states |0> and |1> are orthogonal). Individual qubits of non-classical computers can be entangled with other qubits (i.e., the quantum states of two or more qubits can be correlated so that operations on one qubit affect the state of the entangled qubit). Quantum operations can be performed to guide the state of the qubit to converge probabilistically to a specific final state, which represents a solution to a problem. For certain classes of problems, non-classical computers can converge to the solution faster than any known algorithm can achieve on a classical computer. In some cases, this "quantum advantage" can allow non-classical computers to solve problems that would be intractable using any known classical computer. These problems range from factoring large relatively prime numbers (used, for example, to crack modern cryptographic hash functions), searching for specific items in large amounts of data, and simulating the chemical behavior of drugs, materials, or other molecules. Summary of the invention

[0005] In some embodiments, the present disclosure describes non-classical (eg, quantum) computing systems and methods that utilize dopant molecules contained in a host material as qubits.

[0006] It is to be understood that both the foregoing general description and the following detailed description are exemplary and explanatory only and are not restrictive of the disclosed embodiments, as claimed. BRIEF DESCRIPTION OF THE DRAWINGS

[0007] The accompanying drawings, which comprise a part of this specification, illustrate several embodiments and, together with the description, serve to explain certain principles and features of the disclosed embodiments. In the drawings:

[0008] Figure 1A A top view of a system for performing non-classical computing is shown in accordance with various embodiments.

[0009] Figure 1B Shown according to various embodiments Figure 1A Side view of the system.

[0010] Figure 2 An example of an electronic energy level diagram of a ground state triplet (GST) molecule is shown according to various embodiments.

[0011] Figure 3 Various embodiments are shown for use Figure 1A Or a system described in 1B that performs nonclassical computation.

[0012] Figure 4 A flow chart depicting a method for performing non-classical computing is shown in accordance with various embodiments.

[0013] Figure 5 A flow chart depicting a method for generating, producing, or constructing a non-classical computer is shown, according to various embodiments.

[0014] Fig. 6A An exemplary continuous wave (cw) EPR signal associated with the stepwise photoactivation of di(naphthalene-2-yl)carbene in di(naphthalene-2-yl)methanone at a temperature of 25 K using a green laser is shown according to various embodiments.

[0015] Figure 6B FIG. 1 shows the variation of applied light energy according to various embodiments. Fig. 6A Double integration of the cw EPR signal.

[0016] Fig. 7A Exemplary cw EPR signals associated with the conversion of di(naphthalen-2-yl)carbene in freshly photoactivated di(naphthalen-2-yl)methanone to an annealed form at a temperature of 140 K are shown in accordance with various embodiments.

[0017] Figure 7B shows the change of annealing time according to various embodiments Fig. 7A Double integration of the cw EPR signal.

[0018] Fig. 8A Figure 2 shows di(naphthalene-2-yl)methanone-d at a single temperature according to various embodiments. 14 Di(naphth-2-yl)carbene-d 14An exemplary spin-lattice (T 1 ) Relaxation decay curve.

[0019] Figure 8B Di(naphthalene-2-yl)methanone-d according to various embodiments are shown. 14 Di(naphth-2-yl)carbene-d 14 T 1 Example graph of temperature dependence.

[0020] Fig. 9 1 shows an exemplary spin-spin (T) curve of a protonated and deuterated molecular crystal of di(naphthalene-2-yl)carbene in di(naphthalene-2-yl)methanone according to various embodiments. 2 ) Relaxation decay curve.

[0021] Fig.10 Partially and fully activated di(naphthalene-2-yl)methanone-d are shown according to various embodiments. 14 Di(naphth-2-yl)carbene-d 14 An exemplary double electron-electron resonance (DEER) decay curve of .

[0022] Fig.11A An exemplary cw EPR signal associated with the stepwise photoactivation of 4-nitrenebenzoic acid in 4-iodobenzoic acid using light having a wavelength of 370 nm at a temperature of 25 K according to various embodiments is shown.

[0023] Fig. 11B The following diagram shows the changes of activation time according to various embodiments. Fig.11A Double integration of the cw EPR signal.

[0024] Fig.12 Shown are exemplary cw EPR signals associated with the conversion of 4-nitrenebenzoic acid in freshly photoactivated 4-iodobenzoic acid to an annealed form at room temperature, according to various embodiments. DETAILED DESCRIPTION

[0025] Reference will now be made in detail to the exemplary embodiments discussed with respect to the accompanying drawings. Unless otherwise defined, technical and / or scientific terms have the meanings commonly understood by those of ordinary skill in the art. The disclosed embodiments are described in sufficient detail to enable those skilled in the art to practice the disclosed embodiments. It should be understood that other embodiments may be utilized and may be changed without departing from the scope of the disclosed embodiments. Therefore, materials, methods, and examples are merely illustrative and are not intended to necessarily limit.

[0026] As used herein, the term "or" shall convey both a disjunctive and a conjunctive meaning, as long as such meaning is possible. For example, the phrase "A or B" shall be interpreted as including element A alone, element B alone, and a combination of elements A and B, as long as such meaning is possible. As another example, the phrase "A, B, or C" shall be interpreted as including element A alone, element B alone, element C alone, a combination of elements A and B but not element C, a combination of elements A and C but not element B, a combination of elements B and C but not element A, and a combination of elements A, B, and C, as long as such meaning is possible.

[0027] In the drawings (ie, "FIGs." or "Figs."), like numbers refer to like elements.

[0028] Non-classical computers (e.g., quantum computers) typically use quantum mechanical phenomena, such as superposition, entanglement, and interference, to perform computational operations on data. Compared to classical computers that use binary digits (bits) that always have a defined state (0 or 1), non-classical computers use quantum bits (abbreviated as qubits) that can exist in a superposition of basic states (i.e., a certain linear combination of the basic state |0> and the basic state |1>). Individual qubits of non-classical computers can be entangled with other qubits (i.e., the quantum states of two or more qubits can be correlated so that operations on one qubit affect the state of the entangled qubit). Quantum operations can be performed to guide the state of the qubits to converge probabilistically to a solution to a problem. For certain classes of problems, non-classical computers can converge to the solution faster than any known algorithm can achieve on a classical computer. In some cases, this "quantum advantage" can allow non-classical computers to solve problems that would be intractable using any known classical computer. These problems include factoring large relatively prime numbers (e.g., for cracking modern cryptographic hash functions), searching for specific items in large amounts of data, and simulating the chemical behavior of drugs, materials, or other molecules.

[0029] Many chemical and physical systems have been proposed for use as qubits in non-classical computers. For example, a large number of resources have been directed to superconducting qubits that utilize Josephson junctions (i.e., superconductor-insulator-superconductor transitions). Such superconducting qubits use different quantum tunneling modes through the Josephson junction as basic states. These superconducting qubits can be manufactured using well-known semiconductor manufacturing techniques, allowing relatively simple circuit designs. However, superconducting qubits have many disadvantages. For example, superconducting qubits typically must be cooled to a few tenths of a degree above absolute zero, thus requiring a complex cryogenic system. The use of such complex low temperatures also makes it difficult to entangle more than a few qubits, and limits the ultimate computing power of non-classical computers based on superconducting qubits.

[0030] Many other systems have been used as qubits, including arrays of trapped ions, arrays of trapped neutral atoms, and chemical defects in solid-state lattices. One system proposed for quantum computing is the so-called nitrogen-vacancy (NV) center in diamond. The electron spin associated with the NV center can be optically initialized, and its spin state can be read out by fluorescence detection. In addition, the electron spin can be manipulated by microwave (MW) or radio frequency (RF) irradiation, and can exhibit relatively long relaxation and coherence times. However, existing NV quantum computers can only support a limited number of qubits before deleterious effects associated with increasing the number of qubits cause relaxation and coherence times to decrease, thereby negating the very properties that make NV quantum computers attractive in the first place. This is due to the high density of carbon-13 ( 13 C) The natural abundance of spin is 1.1%. 13 The number of C spins increases, increasing the 13 The isotopic concentration of C spins leads to the deterioration of NV center properties. In addition, 13 The random distribution of C spins will lead to couplings on a very wide range of scales, some of which 13 The C spin is very strongly coupled to the NV center (e.g., for adjacent 13 C spin case). This can make NV centers difficult to manipulate and control. In addition, since each NV center 13 The random distribution of C spins has different correlations 13 C spin bath, therefore, NV qubits work almost exclusively with a single NV spin, resulting in a low signal-to-noise ratio (SNR) and the need to perform nonclassical computations multiple times to achieve a measurable signal. In addition, it can be difficult to prepare diamond that can be controllably doped with NV centers, as it can be difficult to prepare highly crystalline diamond with controlled NV doping rates.

[0031] Therefore, there is a need for qubits based on chemical or physical systems that avoid the problems associated with known qubits. Ideally, such chemical or physical systems should be relatively simple to manufacture, support hundreds or thousands of qubits on a single device, allow each qubit to be manipulated independently of every other qubit, and have a coherent lifetime that is much longer than the time required to perform a quantum operation on each qubit. Systems consistent with the disclosed embodiments may meet some or all of these criteria and, therefore, provide technical improvements in performing nonclassical computing.

[0032] As used herein, the terms "non-classical computing," "non-classical programs," "non-classical operations," and "non-classical computers" generally refer to any system or method for performing computational procedures outside the classical computing paradigm. Non-classical computing, non-classical programs, non-classical operations, or non-classical computers may include quantum computing, quantum programs, quantum operations, or quantum computers.

[0033] As used herein, the terms "quantum computing," "quantum program," "quantum operation," and "quantum computer" generally refer to any method or system for performing computations on a Hilbert space represented by a quantum device using quantum mechanical operations (e.g., unitary transformations or completely positive definite trace preserving (CPTP) mappings on a quantum channel). Thus, quantum and classical (or digital) computing can be similar in that both computations can include a sequence of instructions that are performed on input information and then provide an output. Various paradigms of quantum computing can decompose quantum operations into sequences of elementary quantum operations that simultaneously affect subsets of qubits of a quantum device. Quantum operations can be selected based on, for example, their location or the ease of their physical implementation. A quantum program or computation can then consist of a sequence of such instructions that, in various applications, can represent different quantum evolutions on a quantum device. For example, programs that compute or simulate quantum chemistry can represent quantum states and annihilation and creation operators of electron spin orbits by using qubits (e.g., two-level quantum systems) and a universal set of quantum gates (e.g., Hadamard, controlled non-(CNOT), and π / 8 rotation) through the so-called Jordan-Wigner transformation or Bravyi-Kitaev transformation.

[0034] Additional examples of quantum programs or computations may include programs for optimization, such as quantum approximate optimization algorithms (QAOA) or quantum minimum discovery. QAOA may include gates that perform rotations of a single qubit and entangle multiple qubits. In quantum adiabatic computing, instructions may carry a random or non-random path for the evolution of an initial quantum system to a final quantum system. Quantum derivative programs may include simulated annealing, parallel tempering, master equation solvers, Monte Carlo programs, quantum algorithms for approximating maximum independent sets, and the like. Quantum classical or hybrid algorithms or programs may include programs such as variational quantum eigensolvers (VQE) and variational and adiabatic navigation quantum eigensolvers (VanQver).

[0035] In general, examples of quantum programs or computations can include any program or computation described in “Quantum Computation and Quantum Information” by MA Nielsen and IL Chuang, Cambridge University Press (2013), which is incorporated herein by reference in its entirety for all purposes.

[0036] A quantum computer may include one or more adiabatic quantum computers, quantum gate arrays, one-way quantum computers, topological quantum computers, quantum Turing machines, quantum annealers, Ising solvers, or gate models of quantum computing.

[0037] Doped host materials as qubits for performing nonclassical computations

[0038] Provided herein are systems and methods for performing non-classical computing. The systems and methods generally utilize dopant molecules contained in organic host materials. Dopant molecules generally act as qubits and are associated with an electronic energy level structure comprising a triple electron manifold. The triple electron manifold may include a ground state triple (GST) electron manifold. The triple electron manifold generally includes three triplets, which can be linearly combined to form a qubit basic state (e.g., with respect to a laboratory reference system, a rotating reference system, or another suitable time-independent or time-dependent reference system). The basic state generally has a long life at a temperature obtainable using a cryogenic system based on liquid helium. Dopant molecules can be arranged in the host material to allow a relatively strong coupling between the nearest neighboring dopant molecules, thereby allowing information to surge on the qubit network through entanglement. The quantum states of various dopant molecules can be manipulated individually using optical, MW, or RF techniques, thereby allowing each qubit to be individually controlled to perform non-classical computing.

[0039] Figure 1A A top view of a system 100 for performing non-classical computing according to various embodiments is shown. In the example shown, the system 100 includes at least one host material 110. In some embodiments, the host material 110 includes at least one organic molecule. In some embodiments, the host material 110 is referred to herein as a "matrix."

[0040] In some embodiments, the host material 110 comprises a crystalline host material. In some embodiments, the host material 110 comprises a single crystal host material. In some embodiments, the host material 110 comprises a polycrystalline host material. In some embodiments, the host material 110 comprises a liquid crystal host material. In some embodiments, the host material 110 comprises an amorphous host material. In some embodiments, the host material 110 comprises a powdered host material. In some embodiments, the host material 110 comprises a frozen solution host material. In some embodiments, the frozen solution host material comprises a solution frozen at a cryogenic temperature. For example, in some embodiments, the frozen solution host material is frozen at a temperature of at least about 1 Kelvin (K), 2K, 3K, 4K, 5K, 6K, 7K, 8K, 9K, 10K, 15K, 20K, 25K, 30K, 35K, 40K, 45K, 50K or greater, at most about 50K, 45K, 40K, 35K, 30K, 25K, 20K, 15K, 10K, 9K, 8K, 7K, 6K, 5K, 4K, 3K, 2K, 1K or less, or at a temperature between any two of the foregoing values.

[0041] In some embodiments, the main material 110 includes straight or branched alkanes. In some embodiments, the straight or branched alkanes include C4-C20 straight or branched alkanes. In some embodiments, the straight or branched alkanes include C4 straight or branched alkanes, C5 straight or branched alkanes, C6 straight or branched alkanes, C7 straight or branched alkanes, C8 straight or branched alkanes, C9 straight or branched alkanes, C10 straight or branched alkanes, C11 straight or branched alkanes, C12 straight or branched alkanes, C13 straight or branched alkanes, C14 straight or branched alkanes, C15 straight or branched alkanes, C16 straight or branched alkanes, C17 straight or branched alkanes, C18 straight or branched alkanes, C19 straight or branched alkanes, or C20 straight or branched alkanes. In some embodiments, the main material 110 includes aromatic hydrocarbons. In some embodiments, the host material 110 includes a polyaromatic hydrocarbon. In some embodiments, the polyaromatic hydrocarbon is optionally substituted with a methylene, nitrile, carbonyl, carboxylate, alkyl, deuterated alkyl, aryl, deuterated aryl, heteroaryl, deuterated heteroaryl, borane, imine, amine, nitro, phosphine, thioether, ether, fluorine, chlorine, bromine, iodine, or thiocarbonyl. In some embodiments, the host material 110 includes a diaryl ketone. In some embodiments, the host material 110 includes octasulfur. In some embodiments, the host material 110 includes naphthalene; anthracene; p-terphenyl; benzoic acid; fluorene; biphenyl; benzene; n-hexane; biphenylene; o-terphenylene; m-terphenylene; p-terphenylene; di(phenyl)methanone; phenanthrene; di(naphthalene-2-yl)methanone. In some embodiments, the host material 110 includes any partially or completely isotopically labeled derivative of any of the foregoing.

[0042] In some embodiments, the host material 110 is at least partially deuterated. That is, in some embodiments, the host material 110 contains one or more deuterium atoms where a hydrogen atom would otherwise be expected. In some embodiments, the host material 110 contains at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20 or more deuterium atoms, up to about 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2 or one deuterium atom, or a number of deuterium atoms within a range defined by any two of the foregoing values. In some embodiments, the host material 110 is fully deuterated. That is, in some embodiments, the host material 110 contains deuterium atoms at every site where a hydrogen atom would otherwise be expected. In some embodiments, the host material 110 is at least partially labeled with carbon-13. That is, in some embodiments, the host material 110 contains one or more carbon-13 atoms where a carbon-12 atom would otherwise be expected. In some embodiments, the host material 110 contains at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20 or more carbon-13 atoms, up to about 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, or one carbon-13 atom, or a number of carbon atoms within a range defined by any two of the foregoing values.

[0043] In some embodiments, the host material 110 comprises an isotopically enriched host material. In some embodiments, the host material 110 isotopically enriched with a specific atomic isotope. In some embodiments, the isotope comprises hydrogen ( 1 H), deuterium ( 2 H), carbon-13 ( 13 C), nitrogen-15 ( 15 N), fluorine-19 ( 19 F), Silicon-29 ( 29 Si) or phosphorus-31( 31In some embodiments, the host material 110 is isotopically enriched to have at least about 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 91%, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, or 100% isotopic enrichment. In some embodiments, the isotopic enrichment allows for improved control of the magnetic environment of the dopant molecules 120 described herein.

[0044] In some embodiments, host material 110 does not contain diamond or graphite.

[0045] In some embodiments, the host material 110 is configured to contain at least one dopant molecule 120 as described herein.

[0046] In the example shown, the system 100 includes a plurality of dopant molecules 120. In some embodiments, the plurality of dopant molecules 120 are contained in a host material 110. In some embodiments, each dopant molecule 120 includes a qubit for use in performing non-classical computing. Figure 2 The quantum state of a qubit is described in more detail in .

[0047] In some embodiments, each dopant molecule 120 comprises an organic molecule. In some embodiments, each dopant molecule 120 comprises a GST molecule; that is, in some embodiments, each dopant molecule 120 is similar to the organic molecule described herein. Figure 2 Describe the GST electronic manifold association.

[0048] In some embodiments, at least one dopant molecule 120 comprises a carbene molecule. In some embodiments, at least one dopant molecule 120 comprises a nitrene molecule. In some embodiments, at least one dopant molecule 120 comprises a diradical molecule. In some embodiments, at least one dopant molecule 120 comprises a diradical molecule. In some embodiments, at least one dopant molecule 120 comprises a diaryldiazomethane compound, di(naphthalene-2-yl)carbene, or di(phenyl)carbene. In some embodiments, at least one dopant molecule 120 comprises any partially or fully isotopically labeled derivative of any of the foregoing.

[0049] In some embodiments, at least one dopant molecule 120 is at least partially deuterated. That is, in some embodiments, at least one dopant molecule 120 contains one or more deuterium atoms where a hydrogen atom would otherwise be expected. In some embodiments, at least one dopant molecule 120 contains at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20 or more deuterium atoms, up to about 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2 or one deuterium atom, or a number of deuterium atoms within a range defined by any two of the foregoing values. In some embodiments, at least one dopant molecule 120 is fully deuterated. That is, in some embodiments, at least one dopant molecule 120 contains a deuterium atom at every site where a hydrogen atom would otherwise be expected. In some embodiments, at least one dopant molecule 120 is at least partially labeled with carbon-13. That is, in some embodiments, at least one dopant molecule 120 contains one or more carbon-13 atoms where a carbon-12 atom would otherwise be expected. In some embodiments, at least one dopant molecule 120 contains at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20 or more carbon-13 atoms, up to about 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, or one carbon-13 atom, or a number of carbon-13 atoms within a range defined by any two of the foregoing values.

[0050] In some embodiments, at least one dopant molecule 120 is coupled to at least one other dopant molecule 120 via a coupling interaction 130. In some embodiments, at least one dopant molecule 120 is coupled to at least about 1, 2, 3, 4, 5, 6, 7, 8, or more other dopant molecules 120, up to about 8, 7, 6, 5, 4, 3, 2, or 1 other dopant molecules 120, or a number of dopant molecules within a range defined by any two of the foregoing values, via a coupling interaction 130. For example, in some embodiments, at least one dopant molecule 120 is coupled to about 1 to about 2, about 1 to about 3, about 1 to about 4, about 1 to about 5, about 1 to about 6, about 1 to about 7, about 1 to about 8, about 2 to about 3, about 2 to about 4, about 2 to about 5, about 2 to about 6, about 2 to about 7, about 2 to about 8, about 3 to about 4, about 3 to about 5, about 3 to about 6, about 3 to about 7, about 3 to about 8, about 4 to about 5, about 4 to about 6, about 4 to about 7, about 4 to about 8, about 5 to about 6, about 5 to about 7, about 5 to about 8, about 6 to about 7, about 6 to about 8, or about 7 to about 8 other dopant molecules 120.

[0051] In some embodiments, each dopant molecule is coupled to at least one other dopant molecule via coupling interaction 130. In some embodiments, each dopant molecule 120 is coupled to at least about 1, 2, 3, 4, 5, 6, 7, 8, or more other dopant molecules 120, up to about 8, 7, 6, 5, 4, 3, 2, or 1 other dopant molecules 120, or a number of dopant molecules within a range defined by any two of the foregoing values, via coupling interaction 130. For example, in some embodiments, each dopant molecule 120 is coupled to about 1 to about 2, about 1 to about 3, about 1 to about 4, about 1 to about 5, about 1 to about 6, about 1 to about 7, about 1 to about 8, about 2 to about 3, about 2 to about 4, about 2 to about 5, about 2 to about 6, about 2 to about 7, about 2 to about 8, about 3 to about 4, about 3 to about 5, about 3 to about 6, about 3 to about 7, about 3 to about 8, about 4 to about 5, about 4 to about 6, about 4 to about 7, about 4 to about 8, about 5 to about 6, about 5 to about 7, about 5 to about 8, about 6 to about 7, about 6 to about 8, or about 7 to about 8 other dopant molecules 120. In some embodiments, the group of dopant molecules 120 to which each dopant molecule 120 is coupled is referred to as its "nearest neighbors."

[0052] In some embodiments, the coupling interaction 130 includes an electronic coupling interaction. In some embodiments, the coupling interaction 130 includes an electronic dipole coupling interaction. In some embodiments, the coupling interaction 130 includes a magnetic coupling interaction. In some embodiments, the coupling interaction 130 has a coupling strength. In some embodiments, the coupling strength is at least about 100 Hz, 200 Hz, 300 Hz, 400 Hz, 500 Hz, 600 Hz, 700 Hz, 800 Hz, 900 Hz, 1 kilohertz (kHz), 2 kHz, 3 kHz, 4 kHz, 5 kHz, 6 kHz, 7 kHz, 8 kHz, 9 kHz, 10 kHz, 20 kHz, 30 kHz, 40 kHz, 50 kHz, 60 kHz, 70 kHz, 80 kHz, 90 kHz, 100 kHz, 200 kHz, 300 kHz, 400 kHz, 500 kHz, 600 kHz, 700 kHz, 800 kHz, 900 kHz, 1 megahertz (MHz), 2 MHz, 3 MHz, 4 MHz, 5 MHz, 6 MHz, 7 MHz, 8 MHz, 9 MHz, 10 MHz or greater, up to about 10 MHz, 9 MHz, 8 MHz, 7 MHz, 6 MHz, 5 MHz, 4 MHz, 3 MHz, 2 MHz, 1 MHz, 900 kHz, 800 kHz, 700 kHz, 600 kHz, 500 kHz, 400 kHz, 300 kHz, 200 kHz, 100 kHz, 90 kHz, 80 kHz, 70 kHz, 60 kHz, 50 kHz, 40 kHz, 30 kHz, 20 kHz, 10 kHz, 9 kHz, 8 kHz, 7 kHz, 6 kHz, 5 kHz, 4 kHz, 3 kHz, 2 kHz, 1 kHz, 900 Hz, 800 Hz, 700 Hz, 600 Hz, 500 Hz, 400 Hz, 300 Hz, 200 Hz, 100 Hz or less, or in a range defined by any two of the foregoing values. For example, in some embodiments, the coupling strength is between about 100 Hz and about 1,000 kHz, between about 100 Hz and about 100 kHz, between about 100 Hz and about 10 kHz, between about 100 Hz and about 1 kHz, between about 1 kHz and about 1,000 kHz, between about 1 kHz and about 100 kHz, between about 1 kHz and about 10 kHz, between about 10 kHz and about 1,000 kHz, between about 10 kHz and about 100 kHz, or between about 100 kHz and about 1,000 kHz. In some embodiments, the coupling interactions 130 between each pair of dopant molecules 120 are the same. In some embodiments, the coupling interactions 130 between each pair of dopant molecules 120 are different.

[0053] In some embodiments, the plurality of dopant molecules 120 are separated by an average distance 140 . In some embodiments, the average distance 140 is at least about 0.3 nanometers (nm), 0.4 nm, 0.5 nm, 0.6 nm, 0.7 nm, 0.8 nm, 0.9 nm, 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm, 10 nm, 11 nm, 12 nm, 13 nm, 14 nm, 15 nm, 16 nm, 17 nm, 18 nm, 19 nm, 20 nm, or more, and at most about 20 nm, 19 nm, 18 nm, 17 nm, 16 nm, 15 nm, 14 nm, 13 nm, 12 nm, 11 nm, 10 nm, 9 nm, 8 nm, 7 nm, 6 nm, 5 nm, 4 nm, 3 nm, 2 nm, 1 nm, 0.9 nm, 0.8 nm, 0.7 nm, 0.6 nm, 0.5 nm, 0.4 nm, 0.3 nm, or less, or within a range defined by any two of the foregoing values. For example, in some embodiments, the average distance 140 is between about 0.3 nm and about 1 nm, between about 0.3 nm and about 10 nm, or between about 1 nm and about 10 nm.

[0054] In some embodiments, the plurality of dopant molecules 120 are present in an amount of at least about 1×10 6 Dopant molecules / cubic micrometer (μm -3 ), 2x10 6 μm -3 , 3x10 6 μm -3 , 4x10 6 μm -3 , 5x10 6 μm -3 , 6x10 6 μm -3 , 7x10 6 μm -3 , 8x10 6 μm -3 , 9x10 6 μm -3 , 1x10 7 μm -3 , 2x10 7 μm -3 , 3x10 7 μm -3 , 4x10 7 μm -3 , 5x10 7 μm -3 , 6x10 7 μm -3 , 7x10 7 μm -3 , 8x107 μm -3 、9x10 7 μm -3 、1x10 8 μm -3 、2x10 8 μm -3 、3x10 8 μm -3 、4x10 8 μm -3 、5x10 8 μm -3 、6x10 8 μm -3 、7x10 8 μm -3 、8x10 8 μm -3 、9x10 8 μm -3 、1x10 9 μm -3 、2x10 9 μm -3 、3x10 9 μm -3 、4x10 9 μm -3 、5x10 9 μm -3 、6x10 9 μm -3 、7x10 9 μm -3 、8x10 9 μm -3 、9x10 9 μm -3 、1x10 10 μm -3 、2x10 10 μm -3 、3x10 10 μm -3 、4x10 10 μm -3 、5x10 10 μm -3 、6x10 10 μm -3 、7x10 10 μm -3 、8x10 10 μm -3 、9x10 10 μm -3 、1x10 11 μm -3 、2x10 11μm -3 、 3 x 10 11 μm -3 、 4 x 10 11 μm -3 、 5 x 10 11 μm -3 、 6 x 10 11 μm -3 、 7 x 10 11 μm -3 、 8 x 10 11 μm -3 、 9 x 10 11 μm -3 、 1 x 10 12 μm -3 or greater, up to approximately 1 x 10 12 μm -3 、 9 x 10 11 μm -3 、 8 x 10 11 μm -3 、 7 x 10 11 μm -3 、 6 x 10 11 μm -3 、 5 x 10 11 μm -3 、 4 x 10 11 μm -3 、 3 x 10 11 μm -3 、 2 x 10 11 μm -3 、 1 x 10 11 μm -3 、 9 x 10 10 μm -3 、 8 x 10 10 μm -3 、 7 x 10 10 μm -3 、 6 x 10 10 μm -3 、 5 x 10 10 μm -3 、 4 x 10 10 μm -3 、 3 x 10 10 μm -3 、 2 x 10 10 μm -3 、 1 x 10 10 μm -3 、 9 x 10 9 μm -3 、 8 x 10 9 μm -3 、 7 x 10 9 μm-3 、6x10 9 μm -3 、5x10 9 μm -3 、4x10 9 μm -3 、3x10 9 μm -3 、2x10 9 μm -3 、1x10 9 μm -3 、9x10 8 μm -3 、8x10 8 μm -3 、7x10 8 μm -3 、6x10 8 μm -3 、5x10 8 μm -3 、4x10 8 μm -3 、3x10 8 μm -3 、2x10 8 μm -3 、1x10 8 μm -3 、9x10 7 μm -3 、8x10 7 μm -3 、7x10 7 μm -3 、6x10 7 μm -3 、5x10 7 μm -3 、4x10 7 μm -3 、3x10 7 μm -3 、2x10 7 μm -3 、1x10 7 μm -3 、9x10 6 μm -3 、8x10 6 μm -3 、7x10 6 μm -3 、6x10 6 μm -3 、5x10 6 μm -3 、4x10 6 μm -3, 3x10 6 μm -3 , 2x10 6 μm -3 , 1x10 6 μm -3 A concentration of 1 2 Å or less, or a concentration within a range defined by any two of the aforementioned values ​​is contained in the host material 110 .

[0055] Despite Figure 1A 100 as including nine dopant molecules 120, but the system 100 may include any number of dopant molecules 120. For example, the system 100 may include at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, 2 0,000, 30,000, 40,000, 50,000, 60,000, 70,000, 80,000, 90,000, 100,000, 200,000, 300,000, 400,000, 500,000, 600,000, 7000,000, 800,000, 900,000, 1,000,000 or more dopant molecules 120, up to about 1,000 ,000, 900,000, 800,000, 700,000, 600,000, 500,000, 400,000, 300,000, 200,000, 100,000, 90,000, 80,000, 70,000, 60,000, 50,000, 40,000, 30,000, 20,000, 10,000, 9,000, 8,000, 7,000, 6,000, 5,000, 4,000, 3,000, 2,000, 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1 dopant molecule 120, or a number of dopant molecules 120 within a range defined by any two of the foregoing values.

[0056] although Figure 1ADepicted are dopant molecules 120 arranged in an array, but this depiction is not intended to be limiting. In some embodiments, each of the dopant molecules 120 may have any number of nearest neighbors described herein. In some embodiments, different dopant molecules 120 may have different numbers of nearest neighbors. For example, one dopant molecule 120 may have 8 nearest neighbors, and another dopant molecule 120 may have 2 nearest neighbors. In some embodiments, the dopant molecules 120 are arranged in a regular, irregular, or disordered array. In some embodiments, the spatial arrangement of the nearest neighbors around each dopant molecule 120 is different. In some embodiments, the separation between each nearest neighbor and each dopant molecule 120 is different.

[0057] In some embodiments, the dopant molecule 120 is generated by cleaving (e.g., by photolysis) at least one precursor of at least one of the dopant molecules 120. In some embodiments, the at least one precursor comprises at least one cleavable moiety. In some embodiments, the at least one cleavable moiety comprises at least one photocleavable moiety. In some embodiments, the at least one photocleavable moiety comprises at least one diazo moiety. In some embodiments, the precursor comprises a derivative of a carbene molecule. In some embodiments, the precursor comprises a diazo derivative of a carbene molecule or any partially or fully isotopically labeled derivative thereof.

[0058] In some embodiments, the precursor comprises a diazo derivative of a diarylcarbene. In some embodiments, the precursor comprises (diazomethylene) dinaphthalene, (diazomethylene) diphenyl, or any partially or fully isotopically labeled derivative thereof.

[0059] In some embodiments, at least one photocleavable moiety comprises at least one azide moiety, at least one isocyanate moiety, or at least one imidoiodoalkane moiety. In some embodiments, the precursor comprises an azide derivative of a nitrene molecule, an isocyanate derivative of a nitrene molecule, or an imidoiodoalkane derivative of a nitrene molecule, or any partially or fully isotopically labeled derivative thereof.

[0060] In some embodiments, the precursor comprises 4-azidobenzoic acid or any partially or fully isotopically labeled derivative thereof.

[0061] In some embodiments, the precursor is at least partially deuterated. That is, in some embodiments, the precursor originally contains one or more deuterium atoms at the expected hydrogen atom. In some embodiments, the precursor contains at least about 1,2,3,4,5,6,7,8,9,10,11,12,13,14,15,16,17,18,19,20 or more deuterium atoms, at most about 20,19,18,17,16,15,14,13,12,11,10,9,8,7,6,5,4,3,2 or one deuterium atom, or a number of deuterium atoms in the range limited by any two of the aforementioned values. In some embodiments, the precursor is completely deuterated. That is, in some embodiments, the precursor originally contains deuterium atoms at each site of the expected hydrogen atom. In some embodiments, the precursor is at least partially labeled with carbon-13. That is, in some embodiments, the precursor originally contains one or more carbon-13 atoms at the expected carbon-13 atom. In some embodiments, the precursor contains at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, or more carbon- 13 atoms, up to about 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, or one carbon- 13 atom, or a number of carbon- 13 atoms in a range defined by any two of the foregoing values.

[0062] In some embodiments, at least one photocleavable moiety is susceptible to cleavage from at least one precursor upon exposure to cleaving (e.g., photolysis) light. In some embodiments, the cleaving light has a center wavelength of at least about 200 nanometers (nm), 210 nm, 220 nm, 230 nm, 240 nm, 250 nm, 260 nm, 270 nm, 280 nm, 290 nm, 300 nm, 310 nm, 320 nm, 330 nm, 340 nm, 350 nm, 360 nm, 370 nm, 380 nm, 390 nm, 400 nm, 410 nm, 420 nm, 430 nm, 440 nm, 450 nm, 460 nm, 470 nm, 480 nm, 490 nm, 500 nm, or more. In some embodiments, the cutting light has a center wavelength of at most about 500nm, 490nm, 480nm, 470nm, 460nm, 450nm, 440nm, 430nm, 420nm, 410nm, 400nm, 390nm, 380nm, 370nm, 360nm, 350nm, 340nm, 330nm, 320nm, 310nm, 300nm, 290nm, 280nm, 270nm, 260nm, 250nm, 240nm, 230nm, 220nm, 210nm, 200nm or less. In some embodiments, the cutting light has a center wavelength within a range defined by any two of the aforementioned values, for example, between about 300nm and about 500nm, between about 300nm and about 400nm, or between about 350nm and about 400nm.

[0063] Thus, in some embodiments, the system 100 includes at least one cutting molecule 150. In the example shown, the system 100 includes a plurality of cutting molecules 150. In some embodiments, the at least one cutting molecule 150 includes at least one nitrogen molecule, at least one carbon monoxide molecule, or at least one aryl iodide molecule. In some embodiments, the at least one cutting molecule 150 is used to increase the stability of the at least one dopant molecule 120. For example, in some embodiments, the at least one cutting molecule 150 increases the stability of the at least one dopant molecule 120 by kinetically trapping the at least one dopant molecule 120 near the originally reactive dopant molecule 120. In some embodiments, the at least one cutting molecule 150 increases the stability of the at least one dopant molecule 120 by reducing the chemical interaction between the at least one dopant molecule 120 and the host material 110.

[0064] Figure 1B A side view of a system 100 is shown according to various embodiments. In the example shown, the system 100 includes at least one host material 110 and a plurality of dopant molecules 120.

[0065] In the example shown, the body material 110 includes a thickness 160. In some embodiments, the body material 110 includes a thin film. That is, in some embodiments, the thickness 160 is at least about 0.3 nm, 0.4 nm, 0.5 nm, 0.6 nm, 0.7 nm, 0.8 nm, 0.9 nm, 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm, 10 nm, 20 nm, 30 nm, 40 nm, 50 nm, 60 nm, 70 nm, 80 nm, 90 nm, 100 nm, 200 nm, 300 nm, 400 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 1,000 nm, or more, At most about 1,000nm, 900nm, 800nm, 700nm, 600nm, 500nm, 400nm, 300nm, 200nm, 100nm, 90nm, 80nm, 70nm, 60nm, 50nm, 40nm, 30nm, 20nm, 10nm, 9nm, 8nm, 7nm, 6nm, 5nm, 4nm, 3nm, 2nm, 1nm, 0.9nm, 0.8nm, 0.7nm, 0.6nm, 0.5nm, 0.4nm, 0.3nm or less, or in a range defined by any two of the foregoing values. For example, in some embodiments, thickness 160 is between about 0.3 nm and about 1 nm, about 0.3 nm and about 10 nm, about 0.3 nm and about 100 nm, about 0.3 nm and about 1,000 nm, about 1 nm and about 10 nm, about 1 nm and about 10 nm, about 1 nm and about 100 nm, about 1 nm and about 1,000 nm, about 10 nm and about 100 nm, about 10 nm and about 1,000 nm, or about 100 nm and about 1,000 nm. In some embodiments, using a thin film host material 110 allows for the formation of a pseudo-two-dimensional (pseudo-2D) layer of dopant molecules 120, as described herein.

[0066] In some embodiments, the thin film is formed on a substrate ( Figure 1B) on top of the substrate. In some embodiments, the substrate includes a main material 110. In some embodiments, the substrate includes a micro-machining process material, such as silicon, glass, or sapphire. In some embodiments, the thin film is formed using one or more micro-machining techniques, such as wet cleaning, Piranha cleaning, RCA cleaning, surface passivation, spin coating, dip coating, chemical vapor deposition (CVD), atmospheric pressure CVD, low pressure CVD, ultra-high vacuum CVD, aerosol-assisted CVD, direct liquid jet CVD, hot wall CVD, cold wall CVD, microwave plasma-assisted CVD, plasma enhanced CVD (PECVD), remote PECVD, low energy PECVD, atomic layer CVD, combustion CVD, rapid thermal CVD, photoinduced CVD, laser CVD, vapor phase epitaxy, physical vapor deposition, sputtering deposition, evaporative deposition, pulsed laser deposition, pulsed electron deposition, atomic layer deposition, molecular beam epitaxy, etching, wet etching, dry etching, reactive ion etching (RIE), deep RIE, atomic layer etching, or self-assembly (to form a self-assembled monolayer).

[0067] In some embodiments, the thickness 160 of the body material 110 is at least about 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm, 10 nm, 20 nm, 30 nm, 40 nm, 50 nm, 60 nm, 70 nm, 80 nm, 90 nm, 100 nm, 200 nm, 300 nm, 400 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 100 nm, 200 nm, 300 nm, 400 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 1 micrometer (μm), 2 μm, or more. m, 3μm, 4μm, 5μm, 6μm, 7μm, 8μm, 9μm, 10μm, 20μm, 30μm, 40μm, 50μm, 60μm, 70μm, 80μm, 90μm, 100μm, 200μm m, 300μm, 400μm, 500μm, 600μm, 700μm, 800μm, 900μm, 1 millimeter (mm), 2mm, 3mm, 4mm, 5mm, 6mm, 7mm, 8mm, 9mm, 10 mm or larger, up to about 10mm, 9mm, 8mm, 7mm, 6mm, 5mm, 4mm, 3mm, 2mm, 1mm, 900μm, 800μm, 700μm, 600μm, 500μm, 400μm , 300μm, 200μm, 100μm, 90μm, 80μm, 70μm, 60μm, 50μm, 40μm, 30μm, 20μm, 10μm, 9μm, 8μm, 7μm, 6μm, 5μm, 4μ In some embodiments, the body material 110 is not formed on the substrate.

[0068] In the example shown, a plurality of dopant molecules 120 are arranged in a pseudo-2D layer. In some embodiments, the pseudo-2D layer includes a sheet of space to which the plurality of dopant molecules 120 are confined. In some embodiments, a carrier may be drawn between each pair of dopant molecules 120 in the pseudo-2D layer. In some embodiments, the carrier is angled with respect to a plane defined by the host material 110. In some embodiments, the angle is at least about 0, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, or 90 degrees, at most about 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, or 0 degrees, or within a range defined by any two of the foregoing values. In some embodiments, the pseudo-2D layer comprises a self-assembled monolayer (SAM). In some embodiments, arranging the plurality of dopant molecules 120 in a pseudo-2D layer reduces the extent to which each of the plurality of dopant molecules 120 must interact with its nearest neighbors located substantially above or below it, thereby simplifying the quantum dynamics of the plurality of dopant molecules 120 .

[0069] Although Figure 1B A pseudo-2D layer of a thin sheet of space to which the various dopant molecules 120 are confined is depicted, but the disclosed embodiments are not limited thereto. In some embodiments, the various dopant molecules 120 may be disposed within a thicker layer. In such a thicker layer, each of the various dopant molecules 120 may interact with a nearest neighbor located substantially above or below it.

[0070] Electron triplet states used as fundamental states of qubits

[0071] Figure 2 An example of an electronic energy level diagram 200 of a GST molecule is shown. In some embodiments, a GST molecule is used as a qubit (e.g., as described herein with respect to Figure 1A and 1B qubits described). In the example shown, the GST molecule is associated with a GST electron manifold 210, a first singlet electronic state 220, a second singlet electronic state 230, and an excited state triplet (EST) electron manifold 240. In some embodiments, the GST electron manifold 210 includes a first triplet state 211, a second triplet state 212, and a third triplet state 213. In some embodiments, the first triplet state 211, the second triplet state 212, and the third triplet state 213 represent the lowest energy electronic states of the GST molecule. In some embodiments, the first triplet state 211 is represented by |T 1> indicates that the second triplet state 212 is represented by |T 2 >, and the third triplet state 213 is represented by |T 3 > represents. In some embodiments, the EST electron manifold 240 includes a first triplet state 241, a second triplet state 242, and a third triplet state 243. In some embodiments, the first singlet electronic state 220, the second singlet electronic state 230, and the EST electron manifold 240 each represent a higher energy electronic state than the GST molecule. Figure 2 As depicted in , in some embodiments, the energy of the second singlet electronic state 230 is lower than the EST electron manifold 240. However, in other embodiments, the energy of the second singlet electronic state 230 is higher than the EST electron manifold 240.

[0072] In some embodiments, under thermal equilibrium, the GST electronic state 210 is highly populated (i.e., the electronic wave function of the GST molecule is heavily biased to the GST electronic state 210, with relatively equal contributions to the first triplet state 211, the second triplet state 212, and the third triplet state 213), while the first singlet electronic state 220, the second singlet electronic state 230, the first triplet state 241, the second triplet state 242, and the third triplet state 243 are not highly populated.

[0073] In some embodiments, the GST molecules are configured to absorb electromagnetic energy to drive the population from the first triplet state 211, the second triplet state 212, or the third triplet state 213 to the first singlet state 220, the second singlet state 230, the first triplet state 241, the second triplet state 242, or the third triplet state 243. In some embodiments, the GST molecules are configured to relax back to the first triplet state 211, the second triplet state 212, or the third triplet state 213 via radiative decay; or relax back to the first singlet state 220 or the second singlet state 230 via intersystem crossing (ISC). In some embodiments, continuous absorption of electromagnetic energy selectively drives the population into any combination of the first triplet state 211, the second triplet state 212, and the third triplet state 213, thereby generating a non-equilibrium electronic state distribution. In this way, any combination of the first triplet state 211, the second triplet state 212, and the third triplet state 213 can be "hyperpolarized" as described herein.

[0074] In some embodiments, the first triplet state |T 1 >, the second triplet state |T 2 > and the third triplet state |T 3 > can be used as a qubit basis state for non-classical computing. Thus, a qubit may include: a first qubit basis state, wherein the first qubit basis state is a first triplet state |T 1 >, the second triplet state |T 2 > and the third triplet state |T 3> (e.g., with respect to a laboratory reference frame, a rotating reference frame, or another suitable time-independent or time-dependent reference frame) (e.g., a first qubit basis state |0>=α 1 |T 1 >+α 2 |T 2 >+α 3 |T 3 >); and a second qubit base state, wherein the second qubit base state is the first triplet state |T 1 >, the second triplet state |T 2 > and the third triplet state |T 3 > (e.g., the second qubit basis state |1>=β 1 |T 1 >+β 2 |T 2 >+β 3 |T 3 >). Usually, α 1 , α 2 , α 3 , β 1 , β 2 and β 3 They can each satisfy the normalization condition |α 1 | 2 +|α 2 | 2 +|α 3 | 2 =1 and |β 1 | 2 +|β 2 | 2 +|β 3 | 2 = 1. In addition, α should usually be chosen 1 , α 2 , α 3 , β 1 , β 2 and β 3 Such that the first qubit basis state and the second qubit basis state are different from each other (eg, orthogonal).

[0075] In some embodiments, the lifetime (e.g., coherence lifetime or relaxation lifetime) of the first qubit basis state or the second qubit basis state is at least about 100 microseconds (μs), 200 μs, 300 μs, 400 μs, 500 μs, 600 μs, 700 μs, 800 μs, 900 μs, 1 millisecond (ms), 2 ms, 3 ms, 4 ms, 5 ms, 6 ms, 7 ms, 8 ms, 9 ms, 10 ms, 15 ms, 20 ms, 25 ms, 30 ms, 35 ms, 40 ms, 45 ms, 50 ms, 55 ms, 60 ms, 65 ms, 70 ms, 75 ms, 80 ms, 85 ms, 90 ms, 95 ms, 100 ms, 125 ms, 150 ms, 175 ms, 200 ms, 225 ms, 250 ms, 275 ms, 300 ms, 325 ms, 350 ms , 375ms, 400ms, 425ms, 450ms, 475ms, 500ms, 525ms, 550ms, 575ms, 600ms, 625ms, 650ms, 67 5ms, 700ms, 725ms, 800ms, 825ms, 850ms, 875ms, 900ms, 925ms, 950ms, 975ms, 1 second (s), 2 seconds, 3 seconds, 4 seconds, 5 seconds, 6 seconds, 7 seconds, 8 seconds, 9 seconds, 10 seconds, 20 seconds, 30 seconds, 40 seconds, 50 seconds, 1 minute (min), 2 minutes, 3 minutes, 4 minutes, 5 minutes, 6 minutes, 7 minutes, 8 minutes, 9 minutes, 10 minutes, 20 minutes, 30 minutes, 40 minutes, 50 minutes, 1 hour (h), 2 hours, 3 hours, 4 hours, 5 hours, 6 hours, 7 hours, 8 hours, 9 hours, 10 hours or more,Up to about 10 hours, 9 hours, 8 hours, 7 hours, 6 hours, 5 hours, 4 hours, 3 hours, 2 hours, 1 hour, 50 minutes, 40 minutes, 30 minutes, 20 minutes, 10 minutes, 9 minutes, 8 minutes, 7 minutes, 6 minutes, 5 minutes, 4 minutes, 3 minutes, 2 minutes, 1 minute, 50 seconds, 40 seconds, 30 seconds, 20 seconds, 10 seconds, 9 seconds, 8 seconds, 7 seconds, 6 seconds, 5 seconds, 4 seconds, 3 seconds, 2 seconds, 1 second, 975ms, 950ms, 925ms, 900ms, 875ms, 850ms, 825ms, 800ms, 775ms, 750ms, 725ms, 700ms, 675ms, 650ms, 625ms, 600ms, 575ms, 550ms, 525ms, 500ms, 475ms, 450ms, 42 s, 5ms, 400ms, 375ms, 350ms, 325ms, 300ms, 275ms, 250ms, 225ms, 200ms, 175ms, 150ms, 125ms, 100ms, 95ms, 90ms, 85ms, 80ms, 75ms, 70ms, 65ms, 60ms, 55ms, 50ms, 45ms, 40ms, 35ms, 30ms, 25ms, 20ms, 15ms, 10ms, 9ms, 8ms, 7ms, 6ms, 5ms, 4ms, 3ms, 2ms, 1ms, 900μs, 800μs, 700μs, 600μs, 500μs, 400μs, 300μs, 200μs, 100μs or less, or the lifetime is within the range defined by any two of the preceding values. ,

[0076] In some embodiments, the lifetime is defined as the half-life of the electronic state of the qubit returning from a hyperpolarized electronic state distribution to a thermal equilibrium electronic state distribution. In some embodiments, the lifetime is measured at the intended operating temperature of the qubit, e.g., at least about 1 K, 2 K, 3 K, 4 K, 5 K, 6 K, 7 K, 8 K, 9 K, 10 K, 15 K, 20 K, 25 K, 30 K, 35 K, 40 K, 45 K, 50 K or more, at most about 50 K, 45 K, 40 K, 35 K, 30 K, 25 K, 20 K, 15 K, 10 K, 9 K, 8 K, 7 K, 6 K, 5 K, 4 K, 3 K, 2 K, 1 K or less, or at a temperature between any two of the foregoing values ​​(e.g., between about 4 K and about 20 K). In some embodiments, lifetime is measured at a temperature of at least about 1 K, 2 K, 3 K, 4 K, 5 K, 6 K, 7 K, 8 K, 9 K, 10 K, 15 K, 20 K, 25 K, 30 K, 35 K, 40 K, 45 K, 50 K or more, at most about 50 K, 45 K, 40 K, 35 K, 30 K, 25 K, 20 K, 15 K, 10 K, 9 K, 8 K, 7 K, 6 K, 5 K, 4 K, 3 K, 2 K, 1 K or less. Figure 1A and 1B Describing the dipole coupling strength (e.g., Figure 1A and 1BThe coupling interaction 130 depicted in Figure 1 is greater than a multiple of the reciprocal of the lifetime. In some embodiments, the multiple is at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10 or more, at most about 10, 9, 8, 7, 6, 5, 4, 3, 2, 1 or less, or within a range defined by any two of the foregoing values.

[0077] Optical hyperpolarization and initialization of qubit states

[0078] In some embodiments, hyperpolarization allows non-classical computations to be performed with high signal-to-noise ratios (SNRs). In some embodiments, hyperpolarization allows qubits to be initialized in a first qubit basis state or a second qubit basis state (or any linear combination thereof), thereby initializing non-classical computations. In some embodiments, hyperpolarization allows coherent manipulation of the quantum states of qubits to perform non-classical computations.

[0079] In some embodiments, hyperpolarization allows one or more qubits to be placed in a particular quantum state (e.g., a first qubit basis state, a second qubit basis state, or any linear combination thereof). In some embodiments, the qubits are initialized after such hyperpolarization.

[0080] In the case of a GST molecule, in some embodiments, hyperpolarization describes a condition where the electronic state population in one state (e.g., the first singlet electronic state of the GST molecule) is relatively close to that in another state (e.g., the first triplet electronic state of the GST molecule). 1 >, the second triplet state |T 2 > and the third triplet state |T 3 >any combination) exceeds the absolute value of the corresponding differences in thermal equilibrium.

[0081] In some embodiments, the population difference between two electronic states is the difference between the populations of the two electronic states divided by the total population of the two electronic states. The population difference can be expressed as a fractional population difference or a percentage population difference. In some embodiments, the population difference (expressed as a percentage) is at least about 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 95% or more, at most about 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15%, 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3%, 2%, 1% or less, or within a range defined by any two of the foregoing values.

[0082] As described herein, in some embodiments, the qubit is configured to absorb electromagnetic energy to drive the population into a first triplet state |T 1 >, the second triplet state |T 2 > and the third triplet state |T 3 >, thereby generating hyperpolarization. In some embodiments, the electromagnetic energy has a central wavelength selected to drive the population to the first triplet state |T 1 >, the second triplet state |T 2 > and the third triplet state |T 3> any combination of. In some embodiments, the central wavelength is within the infrared (IR), visible, or ultraviolet (UV) portion of the electromagnetic spectrum. In some embodiments, the central wavelength is at least about 200 nm, 210 nm, 220 nm, 230 nm, 240 nm, 250 nm, 260 nm, 270 nm, 280 nm, 290 nm, 300 nm, 310 nm, 320 nm, 330 nm, 340 nm, 350 nm, 360 nm, 370 nm, 380 nm, 390 nm, 400 nm, 410 nm, 420 nm, 430 nm, 440 nm, 450 nm, 460 nm, 470 nm, 480 nm, 490 nm, 500 nm, 510 nm, 520 nm, 530 nm, 540 nm, 550 nm, 560 nm, 570 nm, 580 nm, 590 nm, 600 nm, 610 nm, 620 nm, 630 nm, 640 nm, 650 nm, 660 nm, 670 nm, 680 nm, 690 nm, 700 nm, 710 nm, 720 nm, 730 nm, 740 nm, 750 nm, 760 nm, 770 nm, 780 nm, 790 nm, 800 nm, 1000 nm, 1010 nm, 1020 nm, 1030 nm, 1040 nm, 1050 nm, 1060 nm, 1070 nm, 1080 nm, 1090 nm, 1100 nm, 1110 nm, 1120 nm, 1130 nm, 1140 nm, 1150 nm, 1160 nm, 1170 nm, 1180 nm, 1190 nm, 2000 nm, 2010 nm, 2020 nm, 2030 nm, 2040 nm, 2050 nm, 2060 nm, 2070 nm, 2080 nm, 2090 nm, 2100 nm, 2110 nm, 2120 nm, 2130 nm, 2140 nm, 2150 nm, 2160 nm, 2170 nm, 2180 nm,000nm, 990nm, 980nm, 970nm, 960nm, 950nm, 940nm, 930nm, 920nm, 910nm, 900 nm, 890nm, 880nm, 870nm, 860nm, 850nm, 840nm, 830nm, 820nm, 810nm, 800nm, 7 90nm, 780nm, 770nm, 760nm, 750nm, 740nm, 730nm, 720nm, 710nm, 700nm, 690n m, 680nm, 670nm, 660nm, 650nm, 640nm, 630nm, 620nm, 610nm, 600nm, 590nm, 58 0nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm, 100nm,

[0083] Optical initialization of individual qubits

[0084] return Figure 1A and 1B In some embodiments, different dopant molecules 120 experience different physicochemical environments due to their different positions or orientations in the host material 110. In some embodiments, different physicochemical environments cause different dopant molecules 120 to have slightly different electronic energy level structures. For example, Figure 2 As discussed in the foregoing, the energy difference between any two of the first triplet state 211, the second triplet state 212, the third triplet state 213, the first singlet electronic state 220, the second singlet state 230, the first triplet state 241, the second triplet state 242 and the third triplet state 243 can depend on the physicochemical environment of the associated dopant molecules, thereby changing the wavelength or frequency of the electromagnetic energy required to drive the transition between the two states.

[0085] return Figure 1A and 1BAs discussed above, in some embodiments, the different electronic energy level structures of the dopant molecules 120 may allow for individual addressing of each dopant molecule 120. For example, if the bandwidth of the optical energy used to initialize each dopant molecule is sufficiently narrow (e.g., the bandwidth is small compared to the difference between the wavelength required to initialize a given dopant molecule 120 and the wavelength required to initialize other dopant molecules 120), each dopant molecule 120 may be individually optically addressed.

[0086] For example, the first dopant molecule 120 and the second dopant molecule 120 may have different electronic energy level structures. Therefore, in some embodiments, the first dopant molecule 120 may be configured to absorb a first electromagnetic energy having a first central wavelength, and the second dopant molecule 120 may be configured to absorb a second electromagnetic energy having a second central wavelength. In some embodiments, the first central wavelength or the second central wavelength includes any central wavelength described herein. In some embodiments, the first central wavelength and the second central wavelength are different from each other.

[0087] In some embodiments, the first center wavelength is associated with a first wavelength range having a first bandwidth. In some embodiments, the first bandwidth is measured as a first full width at half maximum (FWHM). In some embodiments, the second center wavelength is associated with a second wavelength range having a second bandwidth. In some embodiments, the second bandwidth is measured as a second FWHM bandwidth. In some embodiments, the first bandwidth or the second bandwidth is at least about 1 MHz, 2 MHz, 3 MHz, 4 MHz, 5 MHz, 6 MHz, 7 MHz, 8 MHz, 9 MHz, 10 MHz, 15 MHz, 20 MHz, 25 MHz, 30 MHz, 35 MHz, 40 MHz, 45 MHz, 50 MHz, 55 MHz, 60 MHz, 65 MHz, 70 MHz, 75 MHz, 80 MHz, 85 MHz, 90 MHz, 95 MHz, 100 MHz or more and at most about 100 MHz, 95 MHz, 90 MHz, 85 MHz, 80 MHz, 75 MHz, 70 MHz, 65 MHz, 60 MHz, 55 MHz, 50 MHz, 45 MHz, 40 MHz, 35 MHz, 30 MHz, 25 MHz, 20 MHz, 15 MHz, 10 MHz, 9 MHz, 8 MHz, 7 MHz, 6 MHz, 5 MHz, 4 MHz, 3 MHz, 2 MHz, 1 MHz or less, or within a range defined by any two of the foregoing values.

[0088] In some embodiments, the first wavelength range and the second wavelength range are different. In some embodiments, the first wavelength range and the second wavelength range (e.g., within the first FWHM and the second FWHM) do not overlap. In some embodiments, the first FWHM and the second FWHM are similar to or wider than the bandwidth of the light source directed to the first dopant molecule 120 and the second dopant molecule 120. In some embodiments, the non-overlapping nature of the first wavelength range and the second wavelength range allows the first dopant molecule 120 to absorb light energy while the second dopant molecule 120 does not absorb light energy. In some embodiments, the non-overlapping nature of the first wavelength range and the second wavelength range allows the second dopant molecule 120 to absorb light energy while the first dopant molecule 120 does not absorb light energy. This procedure may be referred to as "separate optical initialization" of the first dopant molecule and the second dopant molecule 120. In some embodiments, the separate optical initialization of the first dopant molecule and the second dopant molecule 120 causes the first dopant molecule and the second dopant molecule 120 to emit different amounts of light energy. In some embodiments, measuring the light energy collapses the quantum state of at least one dopant molecule into an electronic energy eigenstate of at least one dopant molecule, thereby initializing the dopant molecule to a desired initial quantum state.

[0089] Although discussed from the perspective of two dopant molecules 120, the principles of separate optical initialization described herein can be extended to any number of dopant molecules 120. For example, separate optical initialization can be applied to at least about 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, or more dopant molecules 120, Up to about 10,000, 9,000, 6,000, 5,000, 4,000, 3,000, 2,000, 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3 or 2 dopant molecules 120, or a number of dopant molecules 120 within a range defined by any two of the foregoing values.

[0090] Such individual optical initialization may be particularly useful for qubits based on dopant molecules 120. As described herein, such dopant molecules 120 may be separated from each other by a relatively small distance compared to a typical beam waist. For example, in some embodiments, the dopant molecules 120 are separated from each other by a distance of less than 10 nm (or any other separation distance described herein) in order to ensure proper coupling between nearest neighboring dopant molecules 120. In some embodiments, a typical beam waist may be approximately 500 nm, such that the optical energy will hit approximately 5,000 qubits. Thus, even when the optical energy is directed to hundreds or thousands of qubits, individual optical initialization may allow manipulation of individual qubits.

[0091] In some embodiments, individual optical initialization of qubits may allow for individual initialization of qubits in a first qubit basis state or a second qubit basis state (or any linear combination thereof), thereby initializing non-classical computation.

[0092] RF or MW manipulation of individual qubits

[0093] In some embodiments, the first qubit state and the second qubit state described herein are separated by an energy difference in the RF or MW portion of the electromagnetic spectrum. Thus, in some embodiments, manipulation of the quantum state of each qubit can be performed using RF or MW energy. Furthermore, in some embodiments, the different physicochemical environments of the different dopant molecules 120 produce a wavelength or frequency shift that is insufficient to allow optical initialization of each qubit individually. In such embodiments, multiple qubits can first be optically initialized simultaneously using, for example, a broadband light source, as described herein. In some embodiments, the quantum state of each qubit is then manipulated individually using RF or MW energy.

[0094] In some embodiments, the first dopant molecule 120 can be configured to absorb first electromagnetic energy having a first center frequency, and the second dopant molecule 120 can be configured to absorb second electromagnetic energy having a second center frequency. In some embodiments, the first center frequency or the second center frequency is at least about 1 MHz, 2 MHz, 3 MHz, 4 MHz, 5 MHz, 6 MHz, 7 MHz, 8 MHz, 9 MHz, 10 MHz, 20 MHz, 30 MHz, 40 MHz, 50 MHz, 60 MHz, 70 MHz, 80 MHz, 90 MHz, 100 MHz, 200 MHz, 300 MHz, 400 MHz, 500 MHz, 600 MHz, 700 MHz, 800 MHz, 900 MHz, 1 gigahertz (GHz), 2 GHz, 3 GHz, 4 GHz, 5 GHz, 6 GHz, 7 GHz, 8 GHz, 9 GHz, 10 GHz, 20 GHz, 30 GHz, 40 GHz, 50 GHz, 60 GHz, 70 GHz, 80 GHz, 90 GHz, 100 GHz In some embodiments, the first center frequency or the second center frequency is in the RF or MW portion of the electromagnetic spectrum.

[0095] In some embodiments, the first center frequency and the second center frequency are different from each other. In some embodiments, the first center frequency is associated with a first frequency range having a first bandwidth. In some embodiments, the first bandwidth is measured as a first FWHM bandwidth. In some embodiments, the second center frequency is associated with a second frequency range having a second bandwidth. In some embodiments, the second bandwidth is measured as a second FWHM bandwidth. In some embodiments, the first bandwidth or the second bandwidth depends on the power of the RF or MW energy supplied to the first dopant molecule or the second dopant molecule 120. In some embodiments, the first bandwidth or the second bandwidth includes a natural bandwidth of the first dopant molecule or the second dopant molecule 120. For example, in some embodiments, the first bandwidth or the second bandwidth is at least about 100 Hz, 200 Hz, 300 Hz, 400 Hz, 500 Hz, 600 Hz, 700 Hz, 800 Hz, 900 Hz, 1 kHz, 2 kHz, 3 kHz, 4 kHz, 5 kHz, 6 kHz, 7 kHz, 8 kHz, 9 kHz, 10 kHz, 20 kHz, 30 kHz, 40 kHz, 50 kHz, 60 kHz, 70 kHz, 80 kHz, 90 kHz, 100 kHz, 200 kHz, 300 kHz, 400 kHz, 500 kHz, 600 kHz, 700 kHz, 800 kHz, 900 kHz, 1 MHz, 2 MHz, 3 MHz, 4 MHz, 5 MHz, 6 MHz, 7 MHz, 8 MHz, 9 MHz, 10 MHz, 20 MHz, 30 MHz, 40 MHz, 50 MHz, 60 MHz, 70 MHz, 80 MHz, 90 MHz, 100 MHz, or more. , up to about 100 MHz, 90 MHz, 80 MHz, 70 MHz, 60 MHz, 50 MHz, 40 MHz, 30 MHz, 20 MHz, 10 MHz, 9 MHz, 8 MHz, 7 MHz, 6 MHz, 5 MHz, 4 MHz, 3 MHz, 2 MHz, 1 MHz, 900 kHz, 800 kHz, 700 kHz, 600 kHz, 500 kHz, 400 kHz, 300 kHz, 200 kHz, 100 kHz, 90 kHz, 80 kHz, 70 kHz, 60 kHz, 50 kHz, 40 kHz, 30 kHz, 20 kHz, 10 kHz, 9 kHz, 8 kHz, 7 kHz, 6 kHz, 5 kHz, 4 kHz, 3 kHz, 2 kHz, 1 kHz, 900 Hz, 800 Hz, 700 Hz, 600 Hz, 500 Hz, 400 Hz, 300 Hz, 200 Hz, 100 Hz or less, or in a range defined by any two of the foregoing values.

[0096] In some embodiments, the first frequency range and the second frequency range are different. In some embodiments, the first frequency range and the second frequency range (e.g., within the first FWHM and the second FWHM) do not overlap. In some embodiments, the first FWHM and the second FWHM are similar to or narrower than the bandwidth of the RF or MW energy directed to the first dopant molecule 120 and the second dopant molecule 120. In some embodiments, the non-overlapping nature of the first frequency range and the second frequency range allows the first dopant molecule 120 to absorb RF or MW energy while the second dopant molecule 120 does not absorb RF or MW energy. In some embodiments, the non-overlapping nature of the first frequency range and the second frequency range allows the second dopant molecule 120 to absorb RF or MW energy while the first dopant molecule 120 does not absorb RF or MW energy. This procedure can be referred to as "separate RF or MW manipulation" of the first dopant molecule and the second dopant molecule 120.

[0097] Although discussed from the perspective of two dopant molecules 120, the principles of separate RF or MW manipulation described herein can be extended to any number of dopant molecules 120. For example, separate RF or MW manipulation can be applied to at least about 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, or more dopant molecules 120, up to about 10 ,000, 9,000, 8,000, 7,000, 6,000, 5,000, 4,000, 3,000, 2,000, 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3 or 2 dopant molecules 120, or a number of dopant molecules 120 within a range defined by any two of the foregoing values.

[0098] Such separate RF or MW manipulation may be particularly useful for qubits based on dopant molecules 120. As described herein, such dopant molecules 120 may be separated from each other by a relatively small distance compared to a typical beam waist. For example, in some embodiments, the dopant molecules 120 are separated from each other by a distance less than 10 nm (or any other separation distance described herein) in order to ensure proper coupling between nearest neighboring dopant molecules 120. In some embodiments, a typical beam waist may hit hundreds or thousands of qubits, as described herein.

[0099] Thus, following optical initialization of the qubits (either individually or simultaneously), individual RF or MW manipulations can allow individual coherent manipulation of the quantum state of each qubit. In some embodiments, the coherent manipulations include the implementation of at least one non-classical operation. In some embodiments, the non-classical operations include any of the non-classical operations described herein.

[0100] Storing nonclassical information in nuclear spin degrees of freedom

[0101] In some embodiments, nonclassical information (e.g., information obtained during or after implementation of any nonclassical operation described herein) can be transferred from the electronic state of at least one dopant molecule 120 to the nuclear spin state of at least one dopant molecule 120 or at least one nearby molecule (referred to as a "nearby host molecule") contained within the host material 110. In some embodiments, the information can be transferred by implementing an exchange gate between the electronic state and the nuclear spin state of at least one dopant molecule 120. In some embodiments, the exchange gate can be implemented by applying RF or MW energy to the at least one dopant molecule 120 and the nuclear spin state, as described herein.

[0102] In some embodiments, transferring nonclassical information to nuclear spin states provides an increase in readout fidelity, initialization fidelity, or lifetime, thereby improving the overall fidelity of nonclassical computing.

[0103] Optical readout of individual qubits

[0104] In some embodiments, the different electronic energy level structures of the dopant molecules 120 can allow for the individual optical readout of the quantum state of each dopant molecule 120 after non-classical operations. For example, the quantum state of each dopant molecule 120 can be individually optically readout based on the wavelength of light emitted by the dopant molecule 120, which can vary based on the physicochemical environment of each dopant molecule 120.

[0105] In some embodiments, each dopant molecule 120 is configured to absorb light and emit light. In some embodiments, the optical properties of the light emitted by each dopant molecule 120 are related to the quantum state of the associated dopant molecule 120. For example, in some embodiments, the dopant molecule 120 in the first qubit state absorbs and emits light having a first property, while the dopant molecule 120 in the second qubit state absorbs and emits light having a second property. In some embodiments, the dopant molecule in a linear superposition between the first qubit state and the second qubit state absorbs and emits light having a linear superposition of the first property and the second property. In some embodiments, the first property is different from the second property. Therefore, in some embodiments, measuring the light emitted by the dopant molecule 120 allows the quantum state of the dopant molecule 120 to be determined at the time of measurement. In some embodiments, the first property or the second property includes the intensity of the light emitted by the dopant molecule 120. In some embodiments, the first property or the second property includes the polarization state of the light emitted by the dopant molecule 120. In some embodiments, the first property or the second property includes the wavelength of the light emitted by the dopant molecule 120. In some embodiments, the first property or the second property includes the frequency of the light emitted by the dopant molecule 120.

[0106] System for initializing, manipulating and reading out dopant molecular quantum bit states

[0107] Figure 3 Various embodiments are shown for use Figure 1A In the example shown, the system 300 includes at least one cryogenic unit 310. In some embodiments, the cryogenic unit 310 is configured to include the system 100 of the present invention. Figure 1A and 1B In some embodiments, the cryogenic unit 310 comprises the system 100. In some embodiments, the cryogenic unit 310 does not comprise the system 100. In some embodiments, the cryogenic unit 310 is configured to cool the system 100 to an operating temperature, such as a temperature of at least about 1K, 2K, 3K, 4K, 5K, 6K, 7K, 8K, 9K, 10K, 15K, 20K, 25K, 30K, 35K, 40K, 45K, 50K or greater, at most about 50K, 45K, 40K, 35K, 30K, 25K, 20K, 15K, 10K, 9K, 8K, 7K, 6K, 5K, 4K, 3K, 2K, 1K or less, or a temperature between any two of the foregoing values ​​(e.g., between about 4K and about 20K). In some embodiments, the cryogenic unit 310 comprises at least one helium cryocooler. In some embodiments, the cryogenic unit 310 comprises at least one closed cycle helium cryocooler. In some embodiments, the cryogenic unit 310 includes at least one window ( Figure 3), the at least one window being configured to allow electromagnetic energy (e.g., light energy) to pass therethrough. In some embodiments, the cryogenic unit 310 includes at least one electrical feedthrough ( Figure 3 ), the at least one electrical feedthrough being configured to allow electromagnetic energy (eg, RF or MW energy) to pass therethrough.

[0108] In the example shown, the system 300 includes at least one initialization unit 320. In some embodiments, the initialization unit 320 is configured to direct the third electromagnetic energy 322 to at least one dopant molecule ( Figure 3 In some embodiments, the third electromagnetic energy 322 is configured to initialize the quantum state of at least one dopant molecule to any linear combination of the first qubit state and the second qubit state, as described herein with respect to Figure 1A , 1B and 2. In some embodiments, the third electromagnetic energy 322 includes at least one IR, visible, or UV wavelength as described herein. For example, in some embodiments, the third electromagnetic energy 322 includes at least one wavelength between about 200 nm and about 1,000 nm. In some embodiments, the initialization unit 320 is configured to Figure 1A , 1B or any of the methods described in 2. In some embodiments, the initialization unit 320 comprises a confocal optical system, a confocal microscope, or a wide-field microscope. In some embodiments, the initialization unit 320 is configured to measure the electromagnetic energy (e) emitted by the at least one dopant molecule in response to the third electromagnetic energy 322. Figure 3 320 ). In some embodiments, the measured electromagnetic energy indicates whether the quantum state of the at least one dopant molecule is correctly initialized. In some embodiments, the emitted electromagnetic energy is measured to collapse the quantum state of the at least one dopant molecule into the electronic energy eigenstate of the at least one dopant molecule, thereby initializing the dopant molecule to a desired initial quantum state. In some embodiments, the initialization unit 320 is configured to reapply the third electromagnetic energy 322 in response to the measured electromagnetic energy. For example, in some embodiments, the initialization unit 320 is configured to reapply the third electromagnetic energy 322 to the at least one dopant molecule if the measured electromagnetic energy indicates that the at least one dopant molecule is not correctly initialized.

[0109] In the example shown, the system 300 includes a single initialization unit 320. However, in some embodiments, the system 300 includes a plurality of initialization units 320. In some embodiments, system 300 includes at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, 20,000, 30,000, 40,000, 50,000, 60,000, 70,000, 80,000, 90,000, 100,000, or more initialization units 320, up to about 100, 7, 6, 5, 4, 3, 2, or 1 initialization unit 320, or a number of initialization units 320 within a range defined by any two of the foregoing values. In some embodiments, each initialization unit 320 is configured to initialize the quantum states of at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, or more qubits to a value greater than or equal to 1. 7, 6, 5, 4, 3, 2, or 1 qubit, or a number of qubits in a range defined by any two of the foregoing values.

[0110] In the example shown, the system 300 includes at least one non-classical operation unit 330. In some embodiments, the non-classical operation unit 330 is configured to apply fourth electromagnetic energy 332 to at least one dopant molecule of the system 100. In some embodiments, the fourth electromagnetic energy 332 is configured to perform at least one non-classical operation on the at least one dopant molecule, as described herein with respect to Figure 1A , 1B and 2. In some embodiments, the fourth electromagnetic energy 332 includes at least one RF or MW frequency as described herein. For example, in some embodiments, the fourth electromagnetic energy 332 includes at least one frequency between about 1 MHz and about 100 GHz. In some embodiments, the non-classical operating unit is configured to perform the operations described herein with respect to Figure 1A , 1B or any non-classical operation described in any manner as described in 2. In some embodiments, the non-classical operation unit 330 includes at least one RF cavity, MW cavity, RF stripline, MW stripline, RF antenna, MW antenna, microscopic RF antenna, microscopic MW antenna, nanomirror RF antenna, or nanomirror MW antenna.

[0111] In the example shown, the system 300 includes a single non-classical operating unit 330. However, in some embodiments, the system 300 includes multiple non-classical operating units 330. In some embodiments, the system 300 includes at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, or more non-classical operating units 330, at most about 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1 non-classical operating unit 330, or a number of non-classical operating units 330 within a range defined by any two of the foregoing values. In some embodiments, each non-classical operation unit 330 is configured to perform a non-classical operation on at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, or more qubits, at most about 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1 qubit, or a number of qubits in a range defined by any two of the foregoing values.

[0112] In the example shown, the system 300 includes at least one storage unit 340. In some embodiments, the at least one storage unit 340 is configured to apply the fifth electromagnetic energy 342 and the sixth electromagnetic energy 344 to the at least one dopant molecule. In some embodiments, the fifth electromagnetic energy 342 and the sixth electromagnetic energy 344 are collectively configured to transfer information from the electronic state of the at least one dopant molecule to the nuclear spin state of the at least one dopant molecule, as described herein with respect to Figure 1A , 1B In some embodiments, the fifth electromagnetic energy 342 and the sixth electromagnetic energy 344 are configured to collectively apply a switching gate to at least one dopant molecule, as described herein with respect to Figure 1A , 1B and 2. In some embodiments, the fifth electromagnetic energy 342 includes at least one RF or MW frequency described herein. For example, in some embodiments, the fifth electromagnetic energy 342 includes at least one frequency between about 1 kHz and about 100 MHz. In some embodiments, the sixth electromagnetic energy 344 includes at least one RF or MW frequency described herein. For example, in some embodiments, the sixth electromagnetic energy 344 includes at least one frequency between about 1 MHz and about 100 GHz. In some embodiments, the storage unit 340 includes at least one RF cavity, MW cavity, RF stripline, MW stripline, RF antenna, MW antenna, microscopic RF antenna, microscopic MW antenna, nanomirror RF antenna, or nanomirror MW antenna.

[0113] In the example shown, the system 300 includes a single storage unit 340. However, in some embodiments, the system 300 includes a plurality of storage units 340. In some embodiments, the system 300 includes at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000 or more storage units 340, at most about 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2 or 1 storage unit 340, or a number of storage units 340 within a range defined by any two of the foregoing values. In some embodiments, each storage cell 340 is configured to transfer information from an electronic state to a nuclear spin state of at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, or more qubits, at most about 1,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1 qubit, or a number of qubits in a range defined by any two of the foregoing values.

[0114] In some embodiments, system 300 does not include storage unit 340 .

[0115] In the example shown, the system 300 includes at least one detection unit 350. In some embodiments, the detection unit 350 is configured to detect the electronic state of at least one dopant molecule, as described herein with respect to Figure 1A , 1B In some embodiments, the detection unit 350 is configured to detect the nuclear spin state of at least one dopant molecule, as described herein with respect to Figure 1A , 1B In some embodiments, the detection unit 350 is configured to direct the seventh electromagnetic energy 352 to at least one dopant molecule, thereby obtaining the result of at least one non-classical operation, as described herein with respect to Figure 1A , 1Band 2. In some embodiments, the seventh electromagnetic energy 352 includes at least one IR, visible or UV wavelength as described herein. For example, in some embodiments, the seventh electromagnetic energy 352 includes at least one wavelength between about 200nm and about 1,000nm. In some embodiments, the detection unit 350 includes at least one optical detector configured to detect light emitted by at least one dopant molecule in response to the seventh electromagnetic energy 352. In some embodiments, the detection unit 350 includes a confocal optical system, a confocal microscope, a wide-field microscope, a spectrometer, an optical spectrometer, a fluorescence spectrometer, a UV visible spectrometer, a polarimeter, or a polarization camera.

[0116] In the example shown, the system 300 includes a single detection unit 350. However, in some embodiments, the system 300 includes a plurality of detection units 350. In some embodiments, system 300 includes at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, 20,000, 30,000, 40,000, 50,000, 60,000, 70,000, 80,000, 90,000, 100,000 or more detection units 350, up to about 100 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2 or 1 detection unit 350, or a number of detection units 350 within a range defined by any two of the foregoing values. In some embodiments, each detection unit 350 is configured to detect at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 2,000, 3,000, 4,000, 5,000, 6,000, 7,000, 8,000, 9,000, 10,000, or more qubits, up to about 1 7, 6, 5, 4, 3, 2, or 1 qubit, or an electronic or nuclear spin state of a number of qubits in a range defined by any two of the foregoing values.

[0117] In some embodiments, system 300 includes at least one polarizing beam splitter 360. In some embodiments, polarizing beam splitter 360 is configured to direct third electromagnetic energy 322 from initialization unit 320 to system 100. In some embodiments, polarizing beam splitter 360 is configured to direct seventh electromagnetic energy 352 from detection unit 350 to system 100, and direct light emitted by at least one dopant molecule in response to seventh electromagnetic energy 352 from system 100 to detection unit 350.

[0118] In some embodiments, system 300 includes one or more magnetic field sources ( Figure 3100). In some embodiments, the magnetic field sources are configured to generate one or more magnetic fields or magnetic field gradients near the system 100. In some embodiments, the magnetic field sources each include a permanent magnet, an electromagnet, or a superconducting magnet. In some embodiments, the magnetic field sources include one or more solenoids, Helmholtz coils, anti-Helmholtz coils, saddle coils, Halbach arrays, etc. In some embodiments, one or more of the magnetic field sources are contained in the cryogenic unit 310. In some embodiments, one or more of the magnetic field sources are configured to generate at least about 1 microTesla (μT), 2μT, 3μT, 4μT, 5μT, 6μT, 7μT, 8μT, 9μT, 10μT, 20μT, 30μT, 40μT, 50μT, 60μT, 70μT, 80μT, 90μT, 100μT, 200μT, 300μT, 400μT, 500μT, 600μT, 700μT, 800μT, T, 900μT, 1 millitesla (mT), 2mT, 3mT, 4mT, 5mT, 6mT, 7mT, 8mT, 9mT, 10mT, 20mT, 30mT, 40mT, 50mT, 60mT, 70mT, 80mT, 90mT, 100mT, 200mT, 300mT, 400mT, 500mT, 600mT, 700mT, 800mT, 900mT, 1 Tesla (T) or more, Up to about 1T, 900mT, 800mT, 700mT, 600mT, 500mT, 400mT, 300mT, 200mT, 100mT, 90mT, 80mT, 70mT, 60mT, 50mT, 40mT, 30mT, 20mT, 10mT, 9mT, 8mT, 7mT, 6mT, 5mT, 4mT, 3mT, 2mT, 1mT, 900μT, 800μT, 700μT, 6 In some embodiments, the magnetic field sources are configured to provide an average magnetic field strength (on system 100) of at least about 100 μT, 500 μT, 400 μT, 300 μT, 200 μT, 100 μT, 90 μT, 80 μT, 70 μT, 60 μT, 50 μT, 40 μT, 30 μT, 20 μT, 10 μT, 9 μT, 8 μT, 7 μT, 6 μT, 5 μT, 4 μT, 3 μT, 2 μT, 1 μT, or less. In some embodiments, one or more of the magnetic field sources are configured to provide an average magnetic field strength (on system 100) of at least about 100 μT, 500 μT, 400 μT, 300 μT, 200 μT, 100 μT, 90 μT, 80 μT, 70 μT, 60 μT, 50 μT, 40 μT, 30 μT, 20 μT, 10 μT, 9 μT, 8 μT, 7 μT, 6 μT, 5 μT, 4 μT, 3 μT, 2 μT, 1 μT, or less. -1 )、2μTm -1 、3μTm -1 , 4μTm -1 , 5μTm -1 , 6μTm -1 、7μTm -1 , 8μTm -1 , 9μTm -1 、10μTm-1 , 20μTm -1 、30μTm -1 , 40μTm -1 , 50μTm -1 、60μTm -1 、70μTm -1 、80μTm -1 、90μTm -1 、100μTm -1 , 200μTm -1 、300μTm -1 、400μTm -1 、500μTm -1 、600μTm -1 、700μTm -1 、800μTm -1 、900μTm -1 , 1 microtesla / meter (mTm -1 )、2mTm -1 、3mTm -1 , 4mTm -1 , 5mTm -1 、6mTm -1 7mTm -1 , 8mTm -1 , 9mTm -1 , 10mTm -1 , 20mTm -1 、30mTm -1 , 40mTm -1 、50mTm -1 、60mTm -1 、70mTm -1 、80mTm -1 、90mTm -1 、100mTm -1 、200mTm -1 、300mTm -1 、400mTm -1 、500mTm -1 、600mTm -1 、700mTm -1 、800mTm -1 、900mTm -1 、1,000mTm -1 or greater, up to about 1,000 mTm -1 、900mTm -1 、800mTm -1 、700mTm -1 、600mTm -1 、500mTm-1 、400mTm -1 、300mTm -1 、200mTm -1 、100mTm -1 、90mTm -1 、80mTm -1 、70mTm -1 、60mTm -1 、50mTm -1 , 40mTm -1 、30mTm -1 , 20mTm -1 , 10mTm -1 , 9mTm -1 , 8mTm -1 7mTm -1 、6mTm -1 , 5mTm -1 , 4mTm -1 、3mTm -1 , 2mTm -1 , 1mTm -1 、900μTm -1 、800μTm -1 、700μTm -1 、600μTm -1 、500μTm -1 、400μTm -1 、300μTm -1 , 200μTm -1 、100μTm -1 、90μTm -1 、80μTm -1 、70μTm -1 、60μTm -1 , 50μTm -1 , 40μTm -1 、30μTm -1 , 20μTm -1 、10μTm -1 , 9μTm -1 , 8μTm -1 、7μTm -1 , 6μTm -1 , 5μTm -1 , 4μTm -1 、3μTm -1 , 2μTm -1 , 1μTm -1 An average magnetic field gradient (on system 100) of 50° or less, or an average magnetic field gradient within a range defined by any two of the aforementioned values.

[0119] Methods for performing nonclassical computations

[0120] Figure 4 A flowchart depicting a method 400 for performing non-classical computing is shown according to various embodiments. In some embodiments, the method 400 uses Figure 1A or 1B system 100 or Figure 3 At 410, a plurality of dopant molecules contained in at least one host material is obtained. In some embodiments, the plurality of dopant molecules include Figure 1A , 1B , 2 or 3. In some embodiments, the host material includes any dopant molecule described herein Figure 1A , 1B , 2 or 3. In some embodiments, each dopant molecule is combined with a Figure 2 In some embodiments, the triple electron manifold includes the electron energy level structure described herein. Figure 2 The first triplet state, the second triplet state and the third triplet state are described.

[0121] At 420, each dopant molecule is configured to have Figure 1A , 1B , 2, or 3. In some embodiments, the first qubit state comprises a first linear combination of a first triplet state, a second triplet state, and a third triplet state, as described herein. In some embodiments, the second qubit state comprises a second linear combination of a first triplet state, a second triplet state, and a third triplet state, as described herein, wherein the first qubit state is different from the second qubit state. In some embodiments, the first qubit state or the second qubit state is different from the second qubit state as described herein with respect to Figure 1A , 1B , 2 or 3 at any temperature described herein Figure 1A , 1B In some embodiments, at least one dopant molecule has any lifetime described herein. Figure 1A , 1B , 2 or 3 described by any dipole or magnetic coupling strength is coupled to at least one other dopant molecule by an electronic or magnetic dipole coupling interaction.

[0122] At 430, non-classical computing is performed on the at least one dopant molecule. In some embodiments, performing non-classical computing includes: directing third electromagnetic energy to the at least one dopant molecule, thereby initializing a quantum state of the at least one dopant molecule to a first qubit state or a second qubit state; applying fourth electromagnetic energy to the at least one dopant molecule, thereby performing at least one non-classical operation on the at least one dopant molecule; and detecting an electronic state of the at least one dopant molecule or a nuclear spin state of the at least one dopant molecule, thereby obtaining a result of the at least one non-classical operation, as described herein with respect to Figure 1A , 1B , 2 or 3. In some embodiments, the third electromagnetic energy comprises any third electromagnetic energy described herein. In some embodiments, the fourth electromagnetic energy comprises any fourth electromagnetic energy described herein. In some embodiments, at least one non-classical operation comprises any non-classical operation described herein.

[0123] In some embodiments, performing non-classical computing further comprises applying fifth electromagnetic energy and sixth electromagnetic energy to at least one dopant molecule prior to detecting the nuclear spin state of the at least one dopant molecule, as described herein with respect to Figure 1A , 1B , 2 or 3. In some embodiments, the fifth electromagnetic energy and the sixth electromagnetic energy are collectively configured to transfer information from the electronic state of at least one dopant molecule to the nuclear spin state of at least one dopant molecule, as described herein with respect to Figure 1A , 1B , 2 or 3. In some embodiments, the fifth electromagnetic energy comprises any fifth electromagnetic energy described herein. In some embodiments, the sixth electromagnetic energy comprises any sixth electromagnetic energy described herein.

[0124] In some embodiments, detecting the electronic state of at least one dopant molecule or the nuclear spin state of at least one dopant molecule comprises applying seventh electromagnetic energy to the at least one dopant molecule, thereby obtaining a result of at least one non-classical operation, as described herein with respect to Figure 1A , 1B , 2 or 3. In some embodiments, the seventh electromagnetic energy comprises any seventh electromagnetic energy described herein. In some embodiments, detecting the electronic state of at least one dopant molecule or the nuclear spin state of at least one dopant molecule further comprises detecting light emitted by at least one dopant molecule in response to the seventh electromagnetic energy, as described herein with respect to Figure 1A , 1B , 2, or 3 described.

[0125] Method for generating, producing or constructing a non-classical computer

[0126] Figure 5A flowchart depicting a method 500 for generating, producing, or constructing a non-classical computer is shown according to various embodiments. In some embodiments, the method 500 is used to generate Figure 1A or 1B system 100 or Figure 3 At 510, at least one host material is prepared or obtained. In some embodiments, the at least one host material includes any host material described herein. Figure 1A , 1B Any subject material described in , 2 or 3.

[0127] At 520, at least one precursor of at least one dopant molecule is embedded in at least one host material. For example, in some embodiments, at least one precursor is embedded in at least one host material by solution-based growth of dilute molecular crystals. In some embodiments, at least one dopant molecule includes Figure 1A , 1B , 2 or 3. In some embodiments, at least one precursor comprises at least one cleavable moiety. In some embodiments, at least one cleavable moiety comprises any of the dopant molecules described herein. Figure 1A Any cuttable portion of the description.

[0128] In some embodiments, at least one dopant molecule is combined with a Figure 2 In some embodiments, the triple electron manifold includes the electron energy level structure described herein. Figure 2 The first triplet state, the second triplet state and the third triplet state are described.

[0129] At 530, at least one cuttable portion is cut, as described herein with respect to Figure 1A In some embodiments, cleaving the at least one cleavable portion generates at least one dopant molecule and at least one cleaving molecule in at least one host material, as described herein with respect to Figure 1A In some embodiments, at least one cleavage molecule comprises Figure 1A In some embodiments, at least one cleavable moiety is cleaved by exposing at least one precursor to light, as described herein for Figure 1A In some embodiments, the light includes Figure 1A Any light of description.

[0130] Description of Embodiments

[0131] Non-limiting examples of the foregoing disclosed herein include:

[0132] Embodiment 1. A method for generating a non-classical computer, comprising:

[0133] preparing at least one host material;

[0134] embedding at least one precursor of at least one dopant molecule into the at least one host material, the at least one precursor comprising at least one cleavable moiety;

[0135] and cutting the at least one cleavable portion to generate the at least one dopant molecule and the at least one cleaving molecule in the at least one host material, wherein:

[0136] The at least one dopant molecule includes a qubit having at least a first qubit state and a second qubit state;

[0137] The at least one dopant molecule is associated with an electronic energy level structure comprising a triplet electron manifold;

[0138] The triplet electron manifold includes a first triplet state, a second triplet state, and a third triplet state;

[0139] the first qubit state comprises a first linear combination of the first triplet state, the second triplet state, and the third triplet state;

[0140] the second qubit state comprises a second linear combination of the first triplet state, the second triplet state, and the third triplet state; and

[0141] The first qubit state is different from the second qubit state.

[0142] Embodiment 2. The method of Embodiment 1, wherein the at least one cleavable portion comprises at least one photocleavable portion.

[0143] Embodiment 3. The method of embodiment 1, wherein the at least one photocleavable moiety comprises at least one diazo moiety, an azide moiety, an isocyanate moiety, or an iminoiodinane moiety.

[0144] Embodiment 4. The method of embodiment 3, wherein the at least one cleavage molecule comprises at least one dinitrogen molecule, a carbon monoxide molecule, or an aryl iodide molecule.

[0145] Embodiment 5. The method of any one of embodiments 1 to 4, wherein cleaving the at least one cleavable moiety comprises exposing the at least one precursor to light.

[0146] Embodiment 6. The method of Embodiment 5, wherein the light has a central wavelength between about 200 nanometers (nm) and about 500 nm.

[0147] Embodiment 7. The method of any one of embodiments 1 to 6, wherein the at least one dopant molecule comprises a plurality of dopant molecules.

[0148] Embodiment 8. The method of any one of embodiments 1 to 7, wherein the host material comprises at least one organic molecule.

[0149] Embodiment 9. The method according to any one of embodiments 1 to 8, wherein the host material comprises a crystalline host material, a single crystal host material, a polycrystalline host material, a liquid crystal host material, a powder host material, an amorphous host material or a frozen solution host material.

[0150] Embodiment 10. A method according to any one of embodiments 1 to 9, wherein the host material includes C4-C20 straight or branched alkanes; aromatic hydrocarbons; polyaromatic hydrocarbons optionally substituted with methylene, nitrile, carbonyl, carboxylate, alkyl, deuterated alkyl, aryl, deuterated aryl, heteroaryl, deuterated heteroaryl, borane, imine, amine, nitro, phosphine, thioether, ether, fluorine, chlorine, bromine, iodine or thiocarbonyl; diaryl ketones; naphthalene; anthracene; p-terphenyl; benzoic acid; fluorene; biphenyl; benzene; n-hexane; biphenylene; o-terphenylene; m-terphenylene; p-terphenylene; phenanthrene; di(naphthalene-2-yl)ketone; di(phenyl)ketone; or any partially or fully isotopically labeled derivatives thereof.

[0151] Embodiment 11. The method of any one of embodiments 1 to 10, wherein the host material comprises a thin film having a thickness of at most 100 nanometers (nm).

[0152] Embodiment 12. The method of any one of embodiments 1 to 11, wherein the at least one dopant molecule comprises an organic molecule.

[0153] Embodiment 13. A method according to any one of embodiments 1 to 12, wherein the at least one precursor comprises a derivative of a carbene molecule; a derivative of a nitrene molecule; a diazo derivative of a carbene molecule; an azide derivative of a nitrene molecule; an isocyanate derivative of a nitrene molecule; an imidoiodinane derivative of a nitrene; (diazomethylene) dinaphthalene; (diazomethylene) diphenyl; 4-azidobenzoic acid; or any partially or fully isotopically labeled derivative thereof.

[0154] Embodiment 14. A method according to any one of embodiments 1 to 13, wherein the at least one dopant molecule comprises a carbene molecule; a nitrene molecule; a di(naphthalene-2-yl)carbene molecule; a di(phenyl)carbene molecule; or any partially or fully isotopically labeled derivative thereof.

[0155] Embodiment 15. The method of any one of embodiments 1 to 14, wherein the plurality of dopant molecules are arranged in a pseudo two-dimensional (pseudo-2D) layer.

[0156] Embodiment 16. The method of embodiment 15, wherein the pseudo-2D layer comprises a self-assembled monolayer (SAM).

[0157] Embodiment 17. The method of any one of embodiments 1 to 16, wherein the average distance between dopant molecules is at most 20 nm.

[0158] Embodiment 18. The method according to any one of embodiments 1 to 17, wherein the at least one dopant molecule is present in an amount of at least 10 6 Dopant molecules / cubic micrometer (μm 3 ) is contained in the at least one host material.

[0159] Embodiment 19. The method according to any one of embodiments 1 to 18, wherein:

[0160] The at least one dopant molecule comprises a plurality of dopant molecules;

[0161] A first dopant molecule of the plurality of dopant molecules is configured to absorb first electromagnetic energy having a first center wavelength or a first center frequency;

[0162] A second dopant molecule of the plurality of dopant molecules is configured to absorb second electromagnetic energy having a second center wavelength or a second center frequency; and

[0163] The first center wavelength or the first center frequency is different from the second center wavelength or the second center frequency.

[0164] Embodiment 20. The method according to embodiment 19, wherein:

[0165] The first center wavelength or the first center frequency is associated with a first wavelength range or a first frequency range having a first full width at half maximum (FWHM) bandwidth;

[0166] The second center wavelength or the second center frequency is associated with a second wavelength range or a second frequency range having a second FWHM bandwidth; and

[0167] The first wavelength range or the first frequency range within the first FWHM bandwidth and the second wavelength range or the second frequency range within the second FWHM bandwidth do not overlap.

[0168] Embodiment 21. The method of Embodiment 20, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 megahertz (MHz).

[0169] Embodiment 22. The method of any one of Embodiments 19 to 21, wherein the first center wavelength or the second center wavelength is between 200 nm and 1,000 nm.

[0170] Embodiment 23. The method of Embodiment 21, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 gigahertz (GHz).

[0171] Embodiment 24. The method of Embodiment 23, wherein the first center frequency or the second center frequency is between 1 MHz and 100 GHz.

[0172] Embodiment 25. The method of any one of Embodiments 1 to 24, wherein the triplet electron manifold comprises a ground state triplet (GST) electron manifold.

[0173] Embodiment 26. A system for performing non-classical computing, comprising:

[0174] at least one host material;

[0175] at least one dopant molecule, the at least one dopant molecule contained in the at least one host material; and

[0176] at least one cleaving molecule, the at least one cleaving molecule being contained in the at least one host material, wherein:

[0177] The at least one dopant molecule includes a qubit having at least a first qubit state and a second qubit state;

[0178] The at least one dopant molecule is associated with an electronic energy level structure comprising a triplet electron manifold;

[0179] The triplet electron manifold includes a first triplet state, a second triplet state, and a third triplet state;

[0180] the first qubit state comprises a first linear combination of the first triplet state, the second triplet state, and the third triplet state;

[0181] the second qubit state comprises a second linear combination of the first triplet state, the second triplet state, and the third triplet state; and

[0182] The first qubit state is different from the second qubit state.

[0183] Embodiment 27. The system of Embodiment 26, wherein the at least one dopant molecule and the at least one cleaving molecule are generated by cleaving at least one precursor of the at least one dopant molecule, the at least one precursor comprising at least one cleavable portion.

[0184] Embodiment 28. The system of Embodiment 27, wherein the at least one cleavable portion comprises at least one photocleavable portion.

[0185] Embodiment 29. The system of Embodiment 28, wherein the at least one photocleavable moiety comprises at least one diazo moiety, an azide moiety, an isocyanate moiety, or an imidoiodoalkane moiety.

[0186] Embodiment 30. The system of Embodiment 29, wherein the cleavage molecule comprises at least one dinitrogen molecule, a carbon monoxide molecule, or an aryl iodide molecule.

[0187] Embodiment 31. The system of any one of Embodiments 27 to 30, wherein cutting the at least one precursor comprises exposing the at least one precursor to light.

[0188] Embodiment 32. The system of Embodiment 31, wherein the light has a central wavelength between approximately 200 nanometers (nm) and approximately 500 nm.

[0189] Embodiment 33. The system of any one of Embodiments 26 to 32, wherein the at least one dopant molecule comprises a plurality of dopant molecules.

[0190] Embodiment 34. The system of any one of Embodiments 26 to 33, wherein the host material comprises at least one organic molecule.

[0191] Embodiment 35. A system according to any one of embodiments 26 to 34, wherein the host material comprises a crystalline host material, a single crystal host material, a polycrystalline host material, a liquid crystal host material, a powder host material, an amorphous host material, or a frozen solution host material.

[0192] Embodiment 36. A system according to any one of embodiments 26 to 35, wherein the main material includes C4-C20 straight chain or branched alkanes; aromatic hydrocarbons; polyaromatic hydrocarbons optionally substituted with methylene, nitrile, carbonyl, carboxylate, alkyl, deuterated alkyl, aryl, deuterated aryl, heteroaryl, deuterated heteroaryl, borane, imine, amine, nitro, phosphine, thioether, ether, fluorine, chlorine, bromine, iodine or thiocarbonyl; diaryl ketones; naphthalene; anthracene; p-terphenyl; benzoic acid; fluorene; biphenyl; benzene; n-hexane; diphenylene; o-terphenylene; m-terphenylene; p-terphenylene; phenanthrene; di(naphthalene-2-yl)methanone; di(phenyl)methanone; or any partially or fully isotopically labeled derivatives thereof.

[0193] Embodiment 37. The system of any one of Embodiments 26 to 36, wherein the host material comprises a thin film having a thickness of at most 100 nanometers (nm).

[0194] Embodiment 38 The system of any one of Embodiments 26 to 37, wherein the at least one dopant molecule comprises an organic molecule.

[0195] Embodiment 39. A system according to any one of embodiments 26 to 38, wherein at least one of the precursors comprises a derivative of a carbene molecule; a derivative of a nitrene molecule; a diazo derivative of a carbene molecule; an azide derivative of a nitrene molecule; an isocyanate derivative of a nitrene molecule; an imidoiodoalkane derivative of a nitrene molecule; (diazomethylene) dinaphthalene; (diazomethylene) diphenyl; 4-azidobenzoic acid; or any partially or fully isotopically labeled derivative thereof.

[0196] Embodiment 40. A system according to any one of Embodiments 26 to 39, wherein the at least one dopant molecule comprises a carbene molecule; a nitrene molecule; a di(naphthalene-2-yl)carbene molecule; a di(phenyl)carbene molecule; or any partially or fully isotopically labeled derivative thereof.

[0197] Embodiment 41. The system of any one of Embodiments 26 to 40, wherein the plurality of dopant molecules are arranged in a pseudo two-dimensional (pseudo-2D) layer.

[0198] Embodiment 42. The system of Embodiment 41, wherein the pseudo-2D layer comprises a self-assembled monolayer (SAM).

[0199] Embodiment 43. The system of any one of Embodiments 26 to 42, wherein the average distance between dopant molecules is at most 20 nm.

[0200] Embodiment 44. The system of any one of Embodiments 26 to 43, wherein the at least one dopant molecule is present in an amount of at least 10 6 Dopant molecules / cubic micrometer (μm3 ) is contained in the at least one host material.

[0201] Embodiment 45. A system according to any one of embodiments 26 to 44, wherein:

[0202] The at least one dopant molecule comprises a plurality of dopant molecules;

[0203] A first dopant molecule of the plurality of dopant molecules is configured to absorb first electromagnetic energy having a first center wavelength or a first center frequency;

[0204] A second dopant molecule of the plurality of dopant molecules is configured to absorb second electromagnetic energy having a second center wavelength or a second center frequency; and

[0205] The first center wavelength or the first center frequency is different from the second center wavelength or the second center frequency.

[0206] Embodiment 46. The system of embodiment 45, wherein:

[0207] The first center wavelength or the first center frequency is associated with a first wavelength range or a first frequency range having a first full width at half maximum (FWHM) bandwidth;

[0208] The second center wavelength or the second center frequency is associated with a second wavelength range or a second frequency range having a second FWHM bandwidth; and

[0209] The first wavelength range or the first frequency range within the first FWHM bandwidth and the second wavelength range or the second frequency range within the second FWHM bandwidth do not overlap.

[0210] Embodiment 47. The system of Embodiment 46, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 megahertz (MHz).

[0211] Embodiment 48. The system of any one of Embodiments 45 to 47, wherein the first center wavelength or the second center wavelength is between 200 nm and 1,000 nm.

[0212] Embodiment 49. The system of Embodiment 48, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 gigahertz (GHz).

[0213] Embodiment 50. The system of Embodiment 49, wherein the first center frequency or the second center frequency is between 1 MHz and 100 GHz.

[0214] Embodiment 51. The system of any one of Embodiments 26 to 50, wherein the triplet electron manifold comprises a ground state triplet (GST) electron manifold.

[0215] Embodiment 52. A system according to any one of Embodiments 26 to 51, further comprising at least one initialization unit, wherein the at least one initialization unit is configured to direct a third electromagnetic energy to the at least one dopant molecule, thereby initializing the quantum state of the at least one dopant molecule to the first quantum bit state or the second quantum bit state.

[0216] Embodiment 53. The system of Embodiment 52, wherein the third electromagnetic energy comprises at least one wavelength between 200 nm and 1,000 nm.

[0217] Embodiment 54. A system according to any one of Embodiments 26 to 53, further comprising at least one non-classical operation unit, wherein the at least one non-classical operation unit is configured to apply fourth electromagnetic energy to the at least one dopant molecule, thereby performing at least one non-classical operation on the at least one dopant molecule.

[0218] Embodiment 55. A system according to Embodiment 54, wherein the at least one non-classical operation includes at least one quantum operation, at least one quantum computing operation, at least one quantum gate operation, at least one quantum simulation operation, or at least one quantum annealing operation.

[0219] Embodiment 56. The system of Embodiment 54 or 55, wherein the fourth electromagnetic energy comprises at least one frequency between 1 MHz and 100 GHz.

[0220] Embodiment 57. A system according to any one of Embodiments 54 to 56, wherein after performing the at least one non-classical operation, a result of the at least one non-classical operation is related to an electronic state of the at least one dopant molecule.

[0221] Embodiment 58. The system according to embodiment 57 further includes at least one storage unit, wherein the at least one storage unit is configured to apply fifth electromagnetic energy and sixth electromagnetic energy to the at least one dopant molecule, wherein the fifth electromagnetic energy and the sixth electromagnetic energy are collectively configured to transfer information from the electronic state of the at least one dopant molecule to the nuclear spin state.

[0222] Embodiment 59. A system according to Embodiment 58, wherein the fifth electromagnetic energy and the sixth electromagnetic energy are configured to jointly apply a swap gate to the at least one dopant molecule, thereby transferring the information from the electronic state of the at least one dopant molecule to the nuclear spin state.

[0223] Embodiment 60. The system of Embodiment 58 or 59, wherein the fifth electromagnetic energy comprises at least one frequency between 1 kHz and 100 MHz, and wherein the sixth electromagnetic energy comprises at least one frequency between 1 MHz and 100 GHz.

[0224] Embodiment 61. According to any one of Embodiments 26 to 60, the system further includes at least one detection unit, wherein the at least one detection unit is configured to detect the electronic state of the at least one dopant molecule or the nuclear spin state of the at least one dopant molecule, thereby obtaining the result of the at least one non-classical operation.

[0225] Embodiment 62. The system of Embodiment 61, wherein the at least one detection unit is configured to apply a seventh electromagnetic energy to the at least one dopant molecule to obtain the result of the at least one non-classical operation.

[0226] Embodiment 63. A system according to embodiment 61 or 62, wherein the at least one detection unit comprises at least one optical detector, and the at least one optical detector is configured to detect light emitted by the at least one dopant molecule in response to the seventh electromagnetic energy.

[0227] Embodiment 64. A system as described in Embodiment 63, wherein the light emitted by the at least one dopant molecule has a first optical property associated with the first qubit state and a second optical property associated with the second qubit state, and wherein the first optical property is different from the second optical property.

[0228] Embodiment 65. A system according to Embodiment 64, wherein the first optical characteristic or the second optical characteristic comprises an intensity, polarization, wavelength, or frequency of the light.

[0229] Embodiment 66. The system of any one of Embodiments 26 to 65, further comprising a cryogenic unit configured to contain the at least one bulk material and cool the at least one bulk material to a temperature of at most 20K.

[0230] Embodiment 67. A system according to Embodiment 66, wherein the cryogenic unit comprises a helium cryocooler or a closed cycle helium cryocooler.

[0231] Examples

[0232] Example 1: General synthesis and characterization procedures

[0233] Commercially available materials were used without purification unless otherwise noted. Moisture and oxygen sensitive reactions were performed using syringe / septum techniques in flame-dried glassware and under an inert atmosphere of purified argon. 254 Thin layer chromatography (TLC) was performed on aluminum plates. The plates were visualized using ultraviolet (UV) light at wavelengths of 254 nm and 365 nm. 1 H at 400.13MHz and for 13 C at 100.61MHz or for 1 H at 600.15MHz and for 13 C NMR spectra were recorded on a Bruker Avance Neo 400 MHz or Bruker Avance Neo 600 MHz spectrometer operating at 150.94 MHz. NMR chemical shifts (δ) are reported in parts per million (ppm). 1 H and 13 C spectra, the solvent signal was used for internal calibration ( 1 H NMR: δ(CHCl 3 )=7.26; 13 C NMR: δ(CDCl 3 )=77.16). Recorded in proton decoupling mode 13 C NMR spectra. Coupling constants (J) are given in Hz and apparent resonance multiplicities are reported as s (singlet), d (doublet), t (triplet), q (quartet), quint (quintet), or m (multiplet). HC Duo column was used as solid phase. The Selekt rapid purification system was used for rapid chromatography. Electron paramagnetic resonance (EPR) spectra were recorded on an X-band EPR spectrometer (Bruker ELEXSYSE580), with software xEPR used for data acquisition. Measurements were made using a dielectric ring resonance (Bruker model 4118X-MD5, typical microwave frequency of about 9.7 GHz), which was installed in a helium flow cryostat (Oxford CF935) with an optical access. When operated in continuous wave (cw) mode, a typical quality factor of about 10,000 was achieved, and the typical modulation amplitude and frequency were 1 Gauss (G) and 100 kHz, respectively. In the pulsed model, a Bruker SpinJet arbitrary waveform generator (Applied Systems Engineering Model 117) with a 1 kW traveling wave tube (TWT) amplifier was used. Prior to measurement, the sample was inserted into an EPR tube (Wilmade Quartz CFQ) with an outer diameter (OD) of 4 millimeters (mm) and aligned on a homemade Teflon sample stage. The sample can be rotated using a single-axis goniometer stage (Bruker E218G1).

[0234] Example 2: General synthetic route for forming carbene dopant molecules

[0235] The general synthetic route for forming carbene dopant molecules in organic host materials is shown below.

[0236]

[0237] Carbenes are designed to have a triplet ground state in which two unpaired electrons are confined to nearby molecular orbitals. As a result, electronic coupling is maximized and the zero-field partitioning parameters D and E of the electron spins are large. In addition, the spin-lattice relaxation times benefit from the weak spin-orbit coupling that is typically present in pure organic materials. Carbenes can be contained in a cyclic structure (1) and include two (2) or one (3) aryl or heteroaryl π 1-3 , which may be substituted with one or more nitrile, carbonyl, carboxylic acid, ester, alkyl, aryl, heteroaryl, amine, nitro, phosphine, alcohol, ether, thioether, or halogen groups. Such groups may be selected (e.g., using computational molecular modeling, high throughput synthesis and screening, etc.) to fine tune electronic properties, such as ZFS, zero phonon lines, spectral stability, and / or thermodynamic / kinetic stability.

[0238] Since carbenes are generally not stable enough to prepare dilute molecular crystals directly, a stable carbenes precursor is instead embedded in a molecular matrix (compounds 4-6) and then activated (i.e., converted from the carbenes precursor form to the activated carbenes form). The carbenes precursor generally includes a diaryldiazo group (R 2 C=N- - =N), which can be photoactivated with light (λ = 200 to 500 nm) to generate dinitrogen N 2 An example of such activation is shown below.

[0239]

[0240] The host materials (compounds 6-9) in which carbenes are embedded are generally designed so that they are structurally similar to carbenes precursors 1-3, respectively, and can form rare molecule crystals by replacing the host material (i.e., matrix) molecules by the carbenes precursors. This isostructural relationship allows the preparation of high-quality rare molecule crystals by reducing the amount of strain imparted by the dopant molecules (i.e., carbenes). Both carbenes and host materials can be partially or completely deuterated to reduce magnetic noise in rare molecule crystals, and thus enhance the spin-spin coherence time T 2 Using bottom-up synthetic chemistry, molecules can also be selectively 13 C (e.g., at the carbene carbon) labeling, adding a nuclear spin manifold that can be used for quantum state preparation. The close packing of molecules in the supramolecular arrangement helps by placing the inert N2 Molecular trapping in close proximity to the reactive carbene center stabilizes the carbene and thereby isolates it from any nearby reaction partners.

[0241] Example 3: Synthesis of compounds required for inserting di(naphthalene-2-yl)carbene into di(naphthalene-2-yl)methanone

[0242] The synthetic route for forming the di(naphthalene-2-yl)carbene dopant molecule in the di(naphthalene-2-yl)methanone host material is shown below.

[0243]

[0244] a) Formation of di(naphthalene-2-yl)methanone

[0245]

[0246] Di(naphthalene-2-yl)methanone was prepared by modifying the procedure described in the following document: B. Kozankiewicz, M. Aloshyna, AD Gudmundsdottir, MS Platz, M. Orrit, P. Tamarat, Journal of Physical Chemistry A (J. Phys. Chem. A) 1999, 103, 3155. A solution of 2-bromonaphthalene (25.0 grams (g), 0.12 moles (mol)) in diethyl ether (anhydrous, 400 milliliters (mL), 0.3 moles (M)) was cooled to -78 degrees Celsius (°C), and n-butyllithium (2.5M in hexanes, 48.3 mL, 1.00 equiv) was added via a dropping funnel over 10 minutes (min). The solution was stirred at -78°C for 1 hour (h). To the resulting yellow dispersion was added a solution of N-ethoxycarbonylpiperidine (9.49 g, 0.12 mol, 1.00 equiv) in diethyl ether (anhydrous, 50 mL) at -78 °C within 5 minutes, and the cooling bath was removed after the addition was complete. The reaction mixture was allowed to warm to room temperature (RT) within 1 hour. The reactants were quenched by adding 10% aqueous HCl (150 mL). The organic phase was separated and the aqueous phase was extracted with diethyl ether (2 × 100 mL). The combined organic phase was washed with water (200 mL) and brine (100 mL), and then filtered through MgSO 4 Dry. Methanol (80 mL) was added to the ether solution, and most of the ether was removed under reduced pressure to give a white precipitate. Almost quantitative precipitation occurred after storage at 7°C for 3 hours. The precipitate was filtered off, washed with cold methanol (2×50 mL) and dried under vacuum to give the product as a white solid (15.5 g, 91%). The following physical, chemical and spectral parameters were obtained. R f (SiO 2 ,CH 2 Cl 2 )=0.81.Melting point (Mp).168.1–170.3℃;1 H NMR (400 MHz, CDCl 3 ): δ8.34(d,J=1.3Hz,2H),8.06–7.97(m,4H),7.97–7.90(m,4H),7.64(ddd,J=8.3,6.9,1.3Hz,2H),7.57(ddd,J=8.3,6.9,1.3Hz,2H)ppm; 13 C NMR (101 MHz, CDCl 3 ): δ196.6,135.4,135.3,132.4,131.9,129.5,128.5,128.4,128.0,126.9,126.0ppm.IR(ATR): 3051(w),1650(m),1618(m),1355(m),1272(m),954(m),918(m),871(m),830(m),776(m)748(s)cm -1 .

[0247] b) Formation of (di(naphthalen-2-yl)methylene)hydrazine

[0248]

[0249] (Di(naphthalene-2-yl)methylene)hydrazine was prepared by modifying the procedure described in the following document: E. Schmitt, G. Landelle, J.-P. Vors, N. Lui, S. Pazenok, FR Leroux, Eur. J. Org. Chem. 2015, 2015, 6052. A mixture of di(naphthalene-2-yl)methanone (4.9 g, 17.3 mmol), hydrazine hydrate (1.18 mL, 24.3 mmol, 1.40 equiv) and EtOH (anhydrous, 6.00 mL, 4.0 M) was heated to 160° C. for 16 hours in a high pressure vessel sealed with a screw cap lined with polytetrafluoroethylene (PTFE). The mixture was cooled to room temperature over 1 hour and stored at 7° C. for another 2 hours. The colorless needles formed were recrystallized from anhydrous EtOH, filtered and dried in vacuo to give the product (4.77 g, 93%). The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,CH 2 Cl 2 / )=0.14;Mp.151.2–152.7℃; 1 H NMR (400 MHz, CDCl 3):δ8.11–8.03(m,2H),8.00–7.87(m,3H),7.86–7.79(m,2H),7.68–7.53(m,4H),7.48–7.35(m,3H),5.58(s,2H)ppm; 13 C NMR(101MHz,CDCl 3 ):δ149.2,136.2,133.7,133.5,133.4,133.3,130.5,129.6,128.6,128.5,128.4,128.1,128.0,127.7,127.1,126.8,126.4,126.3,126.2,123.8ppm;IR(ATR): 3325(m),3189(w),3044(w),1622(w),1580(m),1499(m),1323(w),1270(w),1188(w),1151(w),1113(w),1074(w),927(m),867(m)744(s)cm -1 。

[0250] c) Formation of 2,2'-(diazomethylene)naphthalene

[0251] 2,2'-(diazomethylene) dinaphthalene was prepared by modifying the procedure described in the following document: MI Javed and M. Brewer, Org. Synth. 2008, 85, 189. The workup and isolation of the product was carried out under light protection. Oxalyl chloride (0.22 mL, 0.33 g, 2.61 mmol, 1.05 equiv) in tetrahydrofuran (4 mL) was added to a solution of dimethyl sulfoxide (0.19 mL, 0.21 g, 2.73 mmol, 1.10 equiv) and tetrahydrofuran (anhydrous, 22 mL, 0.13 M) at -55°C over 5 minutes. The solution was kept between -55°C and -50°C for 30 minutes while stirring and then cooled to -78°C. A mixture of (di(naphthalene-2-yl)methylene)hydrazine (0.74 g, 2.48 mmol, 1.00 equiv) and triethylamine (0.72 mL, 0.53 g, 5.22 mmol, 2.10 equiv) in tetrahydrofuran (10 mL) was added to the reaction solution over 5 minutes to provide a dark red solution containing a large amount of white precipitate. The reaction mixture was kept at -78 °C for 30 minutes, then filtered into a round-bottomed flask through a medium porosity sintered glass funnel under cold conditions, and the solid was rinsed with tetrahydrofuran (2 × 50 mL). The filtrate was concentrated at room temperature by rotary evaporation. The red residue was redissolved in n-hexane (200 mL), and filtered quickly through an activated basic alumina plug loaded in a medium porosity sintered glass funnel, and the solid was rinsed with n-hexane (~100 mL) until the filtrate was colorless. The filtrate was concentrated by rotary evaporation (to about 50 mL) at room temperature and stored overnight at 7 °C. The formed precipitate was filtered and dried under vacuum to give the product as a purple crystalline solid (0.63 g, 87%). The following physical, chemical and spectroscopic parameters were obtained. f (Al 2 O 3 Basic, hexane) = 0.52; Mp. 137.3–138.0°C; 1 H NMR (400 MHz, CDCl 3 ): δ7.89(d,J=8.6Hz,1H),7.84(dd,J=7.6,1.8Hz,1H),7.80(d,J=2.0Hz,1H),7.76(dd,J=7.6,1.7Hz,1H),7.54–7.42(m,3H)ppm; 13 C NMR (101 MHz, CDCl 3 ): δ134.1,131.9,129.1,127.9,127.5,127.1,126.8,125.8,123.8,123.5,77.5,77.2,76.8,63.5ppm; IR(ATR): 3053(w),2011(s),1622(m),1590(m),1500(m),1465(m)1385(m),1366(m),1226(m),852(s),806(s),742(s)cm -1 .

[0252] d) Formation of rare-molecule crystals of 2,2'-(diazomethylene)binaphthalene in di(naphthalene-2-yl)methanone

[0253] Di(naphthalene-2-yl)methanone (0.85 g) was dissolved in hot ethyl acetate (HPLC grade, 100 mL, 0.030 M) and the solution was allowed to cool to room temperature. To this solution was added 2,2'-(diazomethylene)dinaphthalene (0.91 mg, 1025 ppm) in the dark. An aliquot (5 milliliters, mL) of the resulting parent solution was added to a 10 mL vial using a syringe equipped with a 0.45 μm pore size syringe filter and the vial was placed in a screw top jar filled with ethanol (HPLC grade). Storage in the dark at room temperature for 7 days formed rare molecular crystals (parallelepiped, approximately 5×4×4 mm). The crystals were isolated in the dark, washed with ethanol (HPLC grade) and dried in vacuo. The rare molecular crystals can be stored in a freezer (T=-22°C) in the dark for several months without detectable degradation.

[0254] To generate di(naphthalene-2-yl)carbene dopant molecules in a di(naphthalene-2-yl)methanone host material, it is only necessary to expose dilute molecular crystals of 2,2'-(diazomethylene)binaphthalene in di(naphthalene-2-yl)methanone to light of the correct wavelength, as described herein.

[0255] Example 4: Synthesis of compounds required for embedding di(phenyl)carbene into di(phenyl)methanone

[0256] The synthetic route for forming the di(phenyl)carbene dopant molecule in the di(phenyl)methanone host material is shown below.

[0257]

[0258] a) Formation of (diphenylmethylene)hydrazine

[0259]

[0260] (Diphenylmethylene)hydrazine was prepared according to the procedure described in E. Schmitt, G. Landelle, J.-P. Vors, N. Lui, S. Pazenok, FR Leroux, Eur. J. Org. Chem. 2015, 2015, 6052.

[0261] b) Formation of (diazomethylene)diphenyl

[0262]

[0263] (Diazomethylene)biphenyl was prepared according to the procedure described in MI Javed and M. Brewer, Org. Synth. 2008, 85, 189.

[0264] c) Formation of dilute molecular crystals of (diazomethylene)diphenyl in di(phenyl)methanone

[0265] Di(phenyl)methanone (0.30 g, purified by sublimation) was dissolved in hot n-hexane (HPLC grade, 4.1 ml, 0.40 M) and the solution was allowed to cool to room temperature. To this solution was added (diazomethylene)diphenyl (0.08 mg, 247 ppm) in the dark. An aliquot (1.0 ml, mL) of this resulting parent solution was added to a 3.0 mL vial, which was sealed with a perforated screw cap. Storage in the dark at room temperature for 6 days formed rare molecular crystals (approximately 6×4×3 mm). The crystals were isolated in the dark, washed with cold n-hexane (HPLC grade) and dried in vacuo. The rare molecular crystals can be stored in a freezer (T=-22° C.) in the dark for several months without detectable degradation.

[0266] To generate di(phenyl)carbene dopant molecules in a di(phenyl)methanone host material, it is only necessary to expose dilute molecular crystals of (diazomethylene)diphenyl in di(phenyl)methanone to light of the correct wavelength, as described herein.

[0267] Example 5: Synthesis of di(naphthalene-2-yl)carbene-d 14 Embedded di(naphthyl)methanone-d 14 The desired compound

[0268] For the formation of di(naphthalene-2-yl)methanone-d 14 Di(naphthalene-2-yl)carbene-d 14 The synthetic route of the dopant molecules is shown below.

[0269]

[0270] a) Formation of di(naphthalene-2-yl)methane

[0271]

[0272] Di(naphthalen-2-yl)methane was prepared by adapting the procedure described in TK Wood, WE Piers, BA Keay, M. Parvez, Chem. Eur. J. 2010, 16, 12199. To a solution of di(naphthalen-2-yl)methanol (3.80 g, 13,4 mmol) in AcOH (89.0 mL, 0.15 M) was added HI (7.31 mL, 55% in HO) at room temperature. 2O, 53.5 mmol, 4.00 equiv) and heated the reaction mixture to reflux (130° C.) for 2 h. The reaction mixture was cooled to room temperature and saturated Na 2 SO 3 Aqueous solution (80 mL) was added until no further color change from dark to yellow was observed. The mixture was washed with H 2 O (80 mL) and diluted with Et 2 O (3 x 100 mL). The combined organic phases were cooled to 0°C and aqueous NaOH (50%, 105 mL) was slowly added until a pH of at least 12 was reached. 2 The aqueous phase was extracted with 1% CO (50 mL), and the combined organic phases were washed with brine (80 mL) and purified by Na 2 SO 4 Dry and remove the solvent in vacuo. The residue was recrystallized from hot n-hexane / toluene 5:1 (100 mL) to give white crystals (0.99 g, 87%). The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,30%CH 2 Cl 2 / hexane) = 0.68; Mp. 91.7–93.9°C; 1 H NMR (400 MHz, CDCl 3 ): δ7.85–7.73(m,3H),7.68(d,J=1.7Hz,1H),7.45(tt,J=6.9,5.1Hz,2H),7.36(dd,J=8.4,1.8Hz,1H),4.32(s,1H)ppm; 13 C NMR (101 MHz, CDCl 3 ): δ138.6,133.8,132.3,128.3,127.9,127.8,127.7,127.4,126.2,125.5,42.4ppm; IR(ATR): 3080(w),3051(w),2815(w)1625(w),1596(m),1499(m),1409(w),1361(m),1270(w),954(m),806(s),757(s),730(s)cm -1 .

[0273] b) Formation of di(naphthalene-2-yl)methane-d 14

[0274]

[0275] Di(naphthalen-2-yl)methane-d was prepared by modifying the procedure described in 14 :X. Liang, S. Duttwyler, Asian J. Org. Chem. 2017, 6, 1063. A flame-dried 100 mL glass vial was charged with non-deuterated di(naphthalene-2-yl)methane (2.5 g, 9.32 mmol), C 6 D 6 (99.5% D, 37.3 mL, 0.25 M) and perfluorobutanesulfonic acid (0.15 mL, 0.93 mmol, 10 mol%). The mixture was cooled to 0 °C and sparged with argon for 5 minutes. The vial was sealed with a PTFE-lined screw cap and the reaction mixture was stirred at 70 °C for 2 days. The reaction was cooled to room temperature and D 2 O (4 mL) was added. Saturated NaHCO 3 The organic layer was separated and washed with Et 2 O (3 × 5 mL). The combined organic layers were purified by Na 2 SO 4 The mixture was dried and the solvent was removed under reduced pressure. The same reaction conditions as above were used to subject the obtained crude product (2.38 g, 91%, 93-94% D, determined by internal standard mesitylene) to a second deuteration cycle. The crude product produced by the second cycle was recrystallized from hot n-hexane (20 mL) to give a product (2.15 g, 82%, 98.5% D, determined by internal standard mesitylene) as colorless crystals. The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,10%CH 2 Cl 2 / hexane) = 0.43; Mp. 92.4–93.7°C; 1 H NMR (400 MHz, CDCl 3 ):δ7.87(s, residual H),7.84(s, residual H),7.83(s, residual H),7.75(s, residual H),7.51(s, residual H),7.49(s, residual H),7.42(s, residual H)ppm; 13 C UDEFT NMR (151 MHz, CDCl 3 ):δ138.4(s),133.6(s),132.1(s),128.1(s,residual CH),127.77(t,J 1 C-D =24.3Hz),127.71(s,residual CH),127.4(t,J 1 C-D=24.1Hz),127.3(t,J 1 C-D =24.3Hz),127.2(t,J 1 C-D =25.2Hz),127.0(t,J 1 C-D =23.9Hz),125.9(s,residual CH),125.6(t,J 1 C-D =24.0Hz),125.3(s,residual CH),125.0(t,J 1 C-D =24.3Hz)ppm,42.2ppm (three residual CH signals were not observed due to overlap); IR (ATR): 2901(w),2271(w),1604(w),1555(w),1438(m),1410(m),1251(m)905,m),837(m),738(m),702(m),651(m),584(s)cm -1 .

[0276] c) Formation of di(naphthalene-2-yl)methanone-d 14

[0277]

[0278] Di(naphthyl)methanone-d was prepared by modifying the procedure described in 14 :J. Zhang, Z. Wang, Y. Wang, C. Wan, X. Zheng, Z. Wang, Green Chem. 2009, 11, 1973. 14 (1.33 g, 4.73 mmol), iodine (60.0 mg, 0.24 mmol, 0.05 equiv), pyridine (20.0 μL, 24.0 mmol, 0.05 equiv), tert-butyl hydroperoxide aqueous solution (70% in H 2 O, 3.48mL, 18.9mmol, 4 equivalents) and acetonitrile (23.7mL, 0.2M) were sealed in a 15mL high pressure tube and stirred at 80°C for 16 hours. After cooling to room temperature, water (20mL) and brown precipitate were filtered off and washed with water and a small amount of cold methanol. By flash chromatography (Si 2 O, 20%-80% CH 2 Cl 2 The crude product was purified by evaporation with 4% paraffin (4% paraffin) and 1% paraffin (cyclohexane) to give a colorless microcrystalline solid (1.15 g, 83%). The following physical, chemical and spectral parameters were obtained. f (SiO2 ,CH 2 Cl 2 )=0.82; Mp.167.3-167.5℃; 1 H NMR (400 MHz, CDCl 3 ):δ8.34(s, residual H),8.01(s, residual H),8.00(s, residual H),7.95(s, residual H),7.94(s, residual H),7.64(s, residual H),7.58(s, residual H)ppm; 13 C UDEFT NMR (151 MHz, CDCl 3 ):δ196.9(s),135.3(s),135.1(s),132.3(s),131.9(s,residual CH),131.6(t,J 1 C-D =24.5Hz),129.4(s,residual CH),129.1(t,J 1 C-D =24.3Hz),128.22(s,residual CH),128.16(s,residual CH),128.0(t,J 1 C-D =24.5Hz),127.9(t,J 1 C-D =24.3Hz),127.5(t,J 1 C-D =24.3Hz),126.7(s,residual CH),126.5(t,J 1 C-D =24.3Hz),125.9(s,residual CH),125.6(t,J 1 C-D =24.8Hz)ppm; IR(ATR): 2271(w),1648(s),1597(m),1541(m),1388(m),1213(m),1068(m),1009(m), 919(w),779(s),733(m),705(m),684(m),650(m),637(s),605(m),573(m)cm -1 .

[0279] d) Formation of (di(naphthalen-2-yl)methylene)hydrazine-d 14

[0280]

[0281] (Di(naphthalen-2-yl)methylene)hydrazine-d was prepared by modifying the procedure described in 14 :E. Schmitt, G. Landelle, J.-P. Vors, N. Lui, S. Pazenok, FR Leroux, "European Organic Chemistry (Eur. J. Org. Chem.)" 2015, 2015, 6052. 14 A mixture of (0.30 g, 1.01 mmol), hydrazine hydrate (69.0 μL, 1.41 mmol, 1.40 equiv) and EtOH (anhydrous, 0.94 mL, 1.5 M) was heated to 160 ° C in a high pressure vessel sealed with a PTFE lined screw cap for 12 hours. The mixture was cooled to room temperature over 1 hour and stored at 7 ° C for another 2 hours. The colorless needle formed was filtered off and washed with cold EtOH to give the product (0.21 g, 67%). The following physical, chemical and spectral parameters were obtained. R f (SiO 2 ,CH 2 Cl 2 / hexane) = 0.16; Mp. 151.2–151.5°C; 1 H NMR (600 MHz, CDCl 3 ):δ8.09(s, residual CH),8.09(s, residual CH,0.011H),8.08(s, residual CH,0.011H),8.00(s, residual CH,,0.011H),7.95(s, residual CH,0.011H),7.93(s, residual CH,0.012H),7.86(s, residual CH,0.011H),7.85(s, residual CH,0.011H ), 7.67(s, residual CH, 0.011H), 7.64(s, residual CH, 0.011H), 7.61(s, residual CH, 0.012H), 7.59(s, residual CH, 0.011H), 7.47(s, residual CH, 0.011H), 7.46(s, residual CH, 0.012H), 7.42(s, residual CH, 0.011H), 5.60(s, 2H)ppm. 13 C UDEFT NMR (151 MHz, CDCl 3 ):δ149.2(s),136.1(s),133.5(s),133.4(s),133.3(s),133.1(s),130.3(s),129.4(s, residual CH),129.1(t,J 1 C-D=24.5Hz),128.6–127.0(m),127.0–125.3(m),123.7(s),123.4(t,J 1 C-D =24.0Hz)ppm; IR(ATR): 3324(m),3185(w),2259(w),1621(w),1578(m),1438(w),1402(w),1375(w),1341(w),1306(w),1254(m),1145(m),1090(m),1 062(m),991(m),931(m),868(m),846(m),832(m),809(m),799(m),777(m),758(m),732(s),704(w),665(w),647(m),583(m)cm -1 .

[0282] e) Formation of 2,2'-(diazomethylene)naphthalene-d 1 4

[0283]

[0284] 2,2'-(diazomethylene)binaphthalene-d was prepared by modifying the procedure described in 14 :MI Javed and M. Brewer, "Org. Synth. " 2008,85,189. The product was treated and separated under light-proof conditions. Oxalyl chloride (55.1 μL, 82.0 mg, 0.64 mmol, 1.05 equivalents) in tetrahydrofuran (2.5 mL) was added to a solution of dimethyl sulfoxide (47.8 μL, 53.0 g, 0.67 mmol, 1.10 equivalents) and tetrahydrofuran (anhydrous, 2.5 mL, 0.26 M) at -55 ° C for 5 minutes. The solution was kept between -55 ° C and -50 ° C for 30 minutes while stirring, and then cooled to -78 ° C. Over 5 minutes, (di(naphthalene-2-yl)methylene)hydrazine-d 14A mixture of (190 mg, 0.61 mmol, 1.00 equivalent) and triethylamine (0.18 mL, 0.13 g, 1.29 mmol, 2.10 equivalents) in tetrahydrofuran (2 mL) was added to the reaction solution to provide a dark red solution containing a large amount of white precipitates. The reaction mixture was kept at -78 ° C for 30 minutes, then filtered into a round-bottom flask through a medium porosity sintered glass funnel in a cold state, and the solid was rinsed with tetrahydrofuran (2 × 3 mL). The filtrate was concentrated at room temperature by rotary evaporation. The red residue was redissolved in n-hexane (20 mL), and quickly filtered through an activated basic alumina plug loaded in a medium porosity sintered glass funnel, and the solid was rinsed with n-hexane (~ 30 mL) until the filtrate was colorless. The filtrate was concentrated by rotary evaporation at room temperature (to about 20 mL) and stored overnight at 7 ° C. The precipitate formed was filtered and dried under vacuum to obtain the product (53.0 mg, 28%) as a purple crystalline solid. The following physical, chemical and spectral parameters were obtained. f (Al 2 O 3 basic, hexane) = 0.51; Mp. 134.0–134.2 °C; 1 H NMR (600 MHz, CDCl 3 ):δ7.90(s, residual CH),7.84(s, residual CH),7.81(s, residual CH)7.77(s, residual CH)7.49,(s, residual CH),7.47(s, residual CH),7.46(s, residual CH)ppm; 13 C UDEFT NMR (151 MHz, CDCl 3 ): δ133.9(s),131.7(s),128.9(s),128.6(t,J 1 C-D =24.5Hz),127.7(s),127.4(t,J 1 C-D =24.5Hz)z,126.98(t,J 1 C-D =24.5Hz),126.95(s),126.6(s),126.3(t,J 1 C-D =24.0Hz),125.3(t,J 1 C-D =24.5Hz),123.4(t,J 1 C-D =24.0Hz),123.1(t,J 1 C-D =24.0Hz)ppm; IR(ATR): 2267(w),2013(s),1600(m),1557(m),1442(m),1395(m),1323,(w),1218(m), 1029(w),872(w),853(m),831(m),727(s),644(m),616(m),602(s),579(m)cm -1 .

[0285] f) Formation of di(naphthalene-2-yl)methanone-d 14 2,2'-(diazomethylene)naphthalene-d 14 Diluted molecular crystals

[0286] Di(naphthyl)methanone-d 14 (0.80 g) was dissolved in hot ethyl acetate (HPLC grade, 90 mL, 0.030 M) and the solution was allowed to cool to room temperature. To this solution was added 2,2'-(diazomethylene)bi-naphthyl-d 14 (4.5 mg, 5400 ppm). An aliquot (5 milliliters, mL) of the resulting parent solution was added to a 10 mL vial using a syringe equipped with a 0.45 μm pore size syringe filter, and the vial was placed in a screw-top jar filled with ethanol (HPLC grade). Storage in the dark for 7 days at room temperature formed rare molecular crystals (parallelepiped, approximately 3×3×4 mm). The crystals were separated in the dark, washed with ethanol (HPLC grade) and dried in a vacuum. The rare molecular crystals can be stored in a freezer (T=-22° C.) in the dark for several months without detectable degradation.

[0287] In order to 14 Di(naphthalene-2-yl)carbene-d 14 The dopant molecule is di(naphthalene-2-yl)methanone-d 14 2,2'-(diazomethylene)naphthalene-d 14 The dilute molecular crystals are exposed to light of the correct wavelength, as described herein.

[0288] Example 6: Synthesis of di(phenyl)carbene-d 10 Embedded di(phenyl)ketone-d 10 The desired compound

[0289] For the formation of di(phenyl)methanone-d 10 Di(phenyl)carbene-d 10 The synthetic route of the dopant molecules is shown below.

[0290]

[0291] a) Formation of di(phenyl)methanone-d 10

[0292]

[0293] Di(phenyl)methanone-d was prepared as follows 10 . Bromobenzene-d 5 A solution of (7.86 g, 48.5 mmol, 2.0 equiv., 99.5% D) in diethyl ether (anhydrous, 97 mL, 0.5 M) was cooled to 0 ° C, and n-butyl lithium (2.5 M in hexane, 20.3 mL, 2.1 equiv.) was added via a dropping funnel within 5 minutes. The solution was stirred at room temperature for 1 hour. At 0 ° C, a solution of N-ethoxycarbonylpiperidine (3.81 g, 24.3 mol, 1.00 equiv.) in diethyl ether (anhydrous, 20 mL) was added to the resulting yellow dispersion within 10 minutes. After the addition was complete, the cooling bath was removed, and the reaction mixture was allowed to warm to room temperature within 30 minutes and stirred at room temperature for another 2 hours. The reactants were quenched by adding 10% HCl aqueous solution (150 mL). The organic phase was separated, and the aqueous phase was extracted with diethyl ether (2×70 mL). The combined organic phases were washed with saturated sodium bicarbonate solution (50 mL), water (100 mL) and brine (80 mL), then purified by MgSO 4 The solvent was removed under reduced pressure to give a crude product as an off-white solid. The product was obtained by two recrystallizations from hot n-hexane (2×40 mL) as colorless crystals (3.36 g, 72%, 99.5% D, by internal standard 1 H NMR with mesitylene). The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,40%CH 2 Cl 2 / hexane) = 0.30; Mp. 49.8–50.3°C; 1 H NMR (400 MHz, CDCl 3 ):δ7.82(s, residual H),7.60(s, residual H),7.49(s, residual H)ppm; 13 C UDEFT NMR (151 MHz, CDCl 3 ): δ196.8(s),137.6(s),132.2(t,J 1 C-D =24.3Hz),129.8(t,J 1 C-D =24.7Hz),127.9(t,J 1 C-D =24.7Hz)ppm; IR(ATR): 2291(w),2265(w),1646(s),1558(m),1385(s),1332(m),1216(s),954(m),912(s),821(m),cm -1 .

[0294] b) Formation of (di(phenyl)methylene)hydrazine-d 10

[0295]

[0296] (Di(phenyl)methylene)hydrazine-d was prepared by modifying the procedure described in 10 :E.Schmitt, G.Landelle, J.-P.Vors, N.Lui, S.Pazenok, FR Leroux, "European Organic Chemistry (Eur.J.Org.Chem.)", 2015, 2015, 6052.

[0297] Di(phenyl)methanone-d 10 A mixture of 4-nitropropene (0.50 g, 2.60 mmol), hydrazine hydrate (0.18 mL, 3.64 mmol, 1.40 equiv) and EtOH (0.9 mL, 4.0 M) was heated to reflux for 12 hours. The mixture was cooled to room temperature over 1 hour and stored at 7 ° C for another 3 hours. The formed colorless needles were recrystallized from EtOH (anhydrous, 1.0 mL), filtered and dried in vacuo to give the product (0.43 g, 80%, 99.5% D, by internal standard 1 H NMR with mesitylene). The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,CH 2 Cl 2 )=0.31; Mp.98.5–100.4℃; 1 HNMR (400MHz, CDCl 3 ):δ7.53(m, residual H),7.47(m, residual H),7.29(m, residual H)ppm; 13 CUDEFT NMR (151 MHz, CDCl 3 ): δ149.3(s),138.4(s),132.9(s),129.0(t,J 1 C-D =24.4Hz),128.5(t,J 1 C-D =24.4Hz),127.74(t,J 1 C-D =24.4Hz),127,72(t,J 1 C-D =24.4Hz),126.2(t,J 1 C-D =24.4 Hz) ppm (a set of triplets overlaps at 129.0 ppm); IR (ATR): 3419(m),3266(w),2273(w),1609(m),1578(m),1554(m),1320(m),1290(m),1144(m),1059(m),1024(w),930(m),818(m)cm -1 .

[0298] c) Formation of (diazomethylene)diphenyl-d 10

[0299]

[0300] (Diazomethylene)diphenyl-d 10 :MI Javed and M. Brewer, "Org. Synth. " 2008,85,189. The product was treated and separated under light-proof conditions. Oxalyl chloride (0.17 mL, 0.26 g, 2.04 mmol, 1.05 equiv) in tetrahydrofuran (4 mL) was added to a solution of dimethyl sulfoxide (0.15 mL, 0.17 g, 2.13 mmol, 1.10 equiv) and tetrahydrofuran (anhydrous, 17 mL, 0.13 M) at -55 ° C for 5 minutes. The solution was kept between -55 ° C and -50 ° C for 30 minutes while stirring, and then cooled to -78 ° C. Di(phenyl)methylene)hydrazine-d was added over 5 minutes. 10 A mixture of (0.40 g, 1.94 mmol, 1.00 equiv) and triethylamine (0.56 mL, 0.41 g, 4.07 mmol, 2.10 equiv) in tetrahydrofuran (10 mL) was added to the reaction solution to provide a deep red solution containing a large amount of white precipitate. The reaction mixture was kept at -78 °C for 30 minutes and then filtered into a round-bottom flask through a medium porosity sintered glass funnel in a cold state, and the solid was rinsed with tetrahydrofuran (2×50 mL). The filtrate was concentrated at room temperature by rotary evaporation. The red residue was redissolved in n-pentane (20 mL) and quickly filtered through an activated basic alumina plug loaded in a medium porosity sintered glass funnel, and the solid was rinsed with n-pentane (~50 mL) until the filtrate was colorless. The filtrate was concentrated by rotary evaporation at room temperature to give 1,1'-(diazomethylene)diphenyl-d as an analytically pure purple liquid. 10 (0.25 g, 63%), which solidified to a crystalline solid upon storage at 7°C. The following physical, chemical and spectroscopic parameters were obtained. f (Al 2 O 3 Alkaline, hexane

[0301] alkane)=0.93;Mp.30.3–30.8℃;UVvis(CH2 Cl 2 ):λ max (ε,M -1 cm -1 )290(20800)nm; 1 HNMR (400MHz, CDCl 3 ):7.42(s, residual H),7.34(s, residual H),7.22(m, residual H)ppm; 13 C UDEFTNMR (151MHz, CDCl 3 ):δ129.5(s),128.8(t,J 1 C-D =24.5Hz),125.2(t,J 1 C-D =24.6Hz),124.9(t,J 1 C-D =24.2 Hz) ppm (a set of triplets overlaps at 129.0 ppm); IR (ATR): 2269(w),2028(s),1556(m),1404(m),1376(m),1238(m),1068(w),916(w),823(m),755(m),cm -1 .

[0302] d) Formation of di(phenyl)methanone-d 10 (diazomethylene)diphenyl-d 10 Diluted molecular crystals

[0303] Di(phenyl)methanone-d 10 (0.30 g, purified by sublimation) was dissolved in hot n-pentane (HPLC grade, 7.8 mL, 0.20 M) and the solution was allowed to cool to room temperature. To this solution was added (diazomethylene)diphenyl-d 10 (0.08 mg, 247 ppm). An aliquot (1.0 milliliter, mL) of the resulting parent solution was added to a 3.0 mL vial and sealed with a perforated screw cap. Stored in the dark at 7°C for 12 days, rare molecular crystals (approximately 3×5×4 mm) were formed. The crystals were separated in the dark, washed with cold n-pentane (HPLC grade) and dried in a vacuum. The rare molecular crystals can be stored in a freezer (T=-22°C) in the dark for several months without detectable degradation.

[0304] In order to 10 Di(phenyl)carbene-d is generated in the main material 10 The dopant molecule is di(phenyl) ketone-d 10 1,1'-(diazomethylene)diphenyl-d 10 The dilute molecular crystals are exposed to light of the correct wavelength, as described herein.

[0305] Example 7: Synthesis of di(naphthalene-2-yl)carbene- 13 Cd 14 Embedded di(naphthalene-2-yl)methanone- 13 Cd 14 The required Compound

[0306] For the formation of di(naphthalene-2-yl)methanone- 13 Cd 14 Di(naphthalene-2-yl)carbene in the host material 13 Cd 14 The synthetic route of the dopant molecules is shown below.

[0307]

[0308] a) Formation of 2-bromonaphthalene-d 7

[0309]

[0310] 2-Bronaphthalene-d was prepared by modifying the procedure described in 7 :X. Liang, S. Duttwyler, Asian J. Org. Chem. 2017, 6, 1063. A flame-dried 350 mL high pressure reaction vessel was charged with 2-bromonaphthalene (5.0 g, 24.1 mmol), C 6 D 6 (99.5% D, 80.5 mL, 0.3 M) and perfluorobutanesulfonic acid (0.40 mL, 2.41 mmol, 10 mol%) and a stirring bar. The mixture was cooled to 0 ° C and sparged with argon for 5 minutes. The vial was sealed with a PTFE-lined screw cap and the reaction mixture was stirred at 130 ° C for 2 days. The reaction was cooled to room temperature and D 2 O (4 mL) was added. Saturated NaHCO 3 The organic layer was separated and washed with Et 2 O (3 × 30 mL). The combined organic layers were 2 SO 4 The crude product (4.85 g, 94% yield, 95.0% D, as determined by internal standard mesitylene) was subjected to a second deuteration cycle using the same reaction conditions as above. -2 The crude product from the second cycle was purified at 400 mbar, 60°C to give a colorless microcrystalline solid (4.71 g, 91% yield, 98.8% D as determined by internal standard mesitylene). The following physical, chemical and spectroscopic parameters were obtained. f (SiO 2 , hexane) = 0.68; Mp. 56.9–57.0°C; 1HNMR (400MHz, CDCl 3 ):δ8.02(s, residual H),7.82(s, residual H),7.76(s, residual H),7.72(s, residual H),7.55(s, residual H),7.51(s, residual H),7.50(s, residual H)ppm; 13 CUDEFT NMR (151 MHz, CDCl 3 ):δ134.5(s),131.9(s),130.0(s,residual CH),129.7(t,J 1 C-D =24.8Hz),129.6(s,residual CH),129.28(s,residual CH),129.26(t,J 1 C-D =24.5Hz),129.0(t,J 1 C-D =25.5Hz),127.9(s,residual CH),127.5(t,J 1 C-D =24.4Hz),127.0(s,residual CH),126.7(t,J 1 C-D =24.3Hz),126.5(t,J 1 C-D =24.2Hz),126.2(s,residual CH),125.9(t,J 1 C-D =24.5Hz),119.7(s)ppm. IR(ATR): 2272(w),1626(m),1553(m),1448(m),1380(w),1247(m),1098(w),1004(s),886(s),784(s),710(s),653(m),591(s)cm -1 .

[0311] b) Formation of 2-naphthoic acid- 13 Cd 7

[0312]

[0313] 2-Naphthoic acid was formed according to the following procedure 13 Cd 7 2-Bronaphthalene-d was prepared by heating the mixture to 2-bromonaphthalene-d at -78 °C. 7 To a solution of 2-nitro-naphthalene-d 2-nitro-naphthalene (2.9 g, 13.5 mmol, 1.00 equiv) in THF (54.1 mL, 0.25 M) was slowly added n-butyl lithium (2.5 M / hexane, 5.42 mL, 13.5 mmol, 1.00 equiv) to prepare 2-nitro-naphthalene-d7 The solution was stirred at -78°C for 30 hours. A gaseous 13 CO 2 (99.0% 13 C, except for 5% ethanol, until no blue formation was observed. The solution was allowed to warm to room temperature for 2 hours and then quenched by the addition of 1 M aqueous NaOH (20 mL) at room temperature. 2 O (2×40 mL). 3M HCl aqueous solution was added to the aqueous layer until pH <3, and Et 2 O (2 × 40 mL). The combined organic phases were purified by 2 SO 4 Trituration with hexanes gave a white solid which was filtered off, washed with hexanes (30 mL), and dried under vacuum for 4 hours to give 2-naphthoic acid- 13 Cd 7 (1.90 g, 10.5 mmol, 78% yield). The following physical, chemical and spectroscopic parameters were obtained. f (SiO 2 ,10%MeOH / CH 2 Cl 2 )=0.75; Mp.184.6–184.7℃; 1 H NMR (600 MHz, DMSO-d 6 ):δ13.05(s,br,1H),8.61(d,J C-H =4.7Hz, residual H),8.12(s, residual H),8.01(s, residual H),8.00(s, residual H),7.98(d, J C-H =3.4 Hz, residual H), 7.65 (s, residual H), 7.60 (s, residual H) ppm; 13 C UDEFTNMR (151MHz, DMSO-d 6 ):δ167.4,134.7,132.0(d,J C-C =4.9Hz),130.1(t,J 1 C-D =24.7Hz),128.8(t,J 1 C-D =24.5Hz),127.79(t,J 1 C-D =23.8Hz),127.78(d,J C-C =71.3Hz),127.5(s,residual CH),127.1(t,J 1C-D =24.3Hz),126.5(s,residual CH),126.3(t,J 1 C-D =24.0Hz),125.0(s,residual CH),124.7(t,J 1 C-D =24.7Hz)ppm; IR(ATR): 2893(br),2557(w),1642(s),1552(m),1415(m),1327(m),1262(s),1247(m) ,1122(m),932(s),867(m),840(m),741(s),690(s)650(m),576(s),533(s)cm -1 .

[0314] c) Formation N- Methoxy- N- Methyl-2-naphthylamide 13 Cd 7

[0315]

[0316] N-methoxy-N-methyl-2-naphthylamide was formed according to the following procedure: 13 Cd 7 . 2-Naphthoic acid- 13 Cd 7 (1.85 g, 10.3 mmol, 1.00 equiv) was dissolved in CH 2 Cl 2 (anhydrous, 37.6 mL, 0.3 M) and one drop of DMF was added under Ar atmosphere. Oxalyl chloride (0.97 mL, 1.10 equiv) was then quickly added and after stirring for 2 hours, the solvent was evaporated under reduced pressure to give a crude acid chloride as an off-white solid. N,O-dimethylhydroxylamine (1.16 g, 1.00 equiv) was dissolved in CH under Ar atmosphere. 2 Cl 2 (anhydrous, 37.6 mL, 0.3 M) and cooled to 0°C. Triethylamine (3.31 mL, 2.0 equiv) was added dropwise and stirred at 0°C for 5 minutes. The acid chloride was redissolved in CH 2 Cl 2 (anhydrous, about 10.0 mL) and added dropwise to the amine solution. The solution was warmed to room temperature and stirred for 2 hours. The reactant was then quenched with HCl aqueous solution (10 mL, 1.0 M) and transferred to a separatory funnel. The organic layer was separated and washed with CH 2 Cl 2 The combined organic phases were washed with saturated NaHCO 3The mixture was washed with aqueous solution (30 mL) and then with brine (2 mL). 2 SO 4 After drying the organic phase, all volatiles were removed under reduced pressure. 2 The residue was purified by HPLC (20-50% ethyl acetate / hexanes) to give the product as a yellow oil (2.01 g, 88%). The following physical, chemical and spectral parameters were obtained. f (SiO 2 , 50% EtOAc / hexane) = 0.56; 1 HNMR (600MHz, CDCl 3 ):δ8.23(d,J C-H =4.4Hz, residual H), 7.91(s, residual H), 7.86(s, residual H), 7.76(d, J C-H =3.3Hz, residual H), 7.55(s, residual H), 7.52(s, residual H), 3.57(s, 3H), 3.42(d, J C-H =2.1 Hz, 3H) ppm; 13 CUDEFT NMR (151 MHz, CDCl 3 ):δ170.1(s),134.2(s,residual CH),132.5(d,J=4.6Hz),131.4(d,J=67.5Hz),128.8(s,residual CH),128.5(t,J 1 C-D =24.9 Hz), 127.8–126.7 (m, multi-CD and residual CH), 126.4 (s, residual CH), 126.1 (t, J 1 C-D =24.4Hz),125.1(s,residual CH),124.8(t,J 1 C-D =25.1Hz),61.3(s),34.0(s)ppm; IR(ATR): 2968(w),2993(w),2275(w),1593(s),(w),1410(m),1376(m),1352(m),1438(m),1182(m) ),1074(m),988(m),940(m),855(m),792(m),683(m),649(m),604(m),556(m),516(m)cm -1 .

[0317] d) Formation of di(naphthalene-2-yl)methanone- 13 Cd 14

[0318]

[0319] Di(naphthalen-2-yl)methanone was prepared according to the following procedure: 13 Cd 14 2-Bronaphthalene-d 7 A solution of (1.73 g, 8.08 mmol, 1.00 equiv) in THF (anhydrous, 32.3 mL, 0.25 M) was cooled to -78°C. Then, n-butyl lithium (2.5 M / hexane, 3.56 mL, 1.10 equiv) was added dropwise over 5 minutes so that the temperature did not exceed -70°C, and the solution was stirred at -78°C for another 20 minutes. The corresponding Weinreb amide N-methoxy-N-methyl-2-naphthamide- 13 Cd 7 (1.80 g, 8.08 mmol, 1.00 equiv) was dissolved in THF (anhydrous, 10 mL) and slowly added to the lithium salt solution. The mixture was stirred at -78 °C for 10 minutes and then allowed to warm to room temperature over 2 hours. The reaction was quenched by adding aqueous HCl (10 mL, 1.0 M). Et 2 O (4 × 20 mL) and washed with saturated NaHCO 3 The combined organic layers were washed with 4% paraformaldehyde (30 mL), water (20 mL), and brine (20 mL). The solution was dried (MgSO 4 ), filtered, and the volatiles were removed under reduced pressure. The crude product was dissolved in a minimum amount of CH 2 Cl 2 The solid formed was filtered off and washed with methanol (30 mL) to give the product as a colorless microcrystalline solid (2.24 g, 93%). -1 mbar) within 6 hours to obtain the analytically pure product as colorless crystals. The following physical, chemical and spectral parameters were obtained. f (SiO 2 ,CH 2 Cl 2 )=0.81; Mp.167.6-167.9℃; 1 H NMR (400 MHz, CDCl 3 ):δ8.35(d,J C-H =4.4Hz, residual H), 8.02(d, J C-H =3.2Hz, residual H), 7.99(s, residual H), 7.94(d, J C-H =7.4 Hz, residual H), 7.63 (s, residual H), 7.57 (s, residual H) ppm; 13CUDEFT NMR (151 MHz, CDCl 3 ):δ135.3,135.2(d,J 1 C-C =55.2Hz),132.3(d,J C-C =4.4 Hz), 131.9 (s, residual CH), 131.6 (t, J 1 C-D =24.3Hz),129.4(s,residual CH),129.1(t,J 1 C-D =24.4Hz),128.3(d,J C-C =3.9Hz),128.2(t,J 1 C-D =24.4Hz),128.0(td,J 1 C-D =24.4,J C-C =3.1Hz),128.0(t,J 1 C-D =24.2Hz),127.5(t,J 1 C-D =24.4Hz),126.8(s,residual CH),126.5(t,J 1 C-D =24.5Hz),125.9(s,residual CH),125.6(t,J 1 C-D =24.6Hz)ppm; IR(ATR): 2271(w),1619(s),1591(s),1540(m),1388(m),1315(m),1243(w),792(s),733(m),679(m),637(m),584(s)cm -1 .

[0320] e) forming (di(naphthalene-2-yl)methylene- 13 C) Hydrazine-d 14

[0321]

[0322] (Di(naphthalen-2-yl)methylene- 13 C) Hydrazine-d 14 :E. Schmitt, G. Landelle, J.-P. Vors, N. Lui, S. Pazenok, FR Leroux, "European Organic Chemistry (Eur. J. Org. Chem.)" 2015, 2015, 6052. 13Cd 14 A mixture of (1.00 g, 3.36 mmol), hydrazine hydrate (0.23 mL, 4.71 mmol, 1.40 equiv) and EtOH (anhydrous, 4.71 mL, 1.0 M) was heated to 160 ° C in a high pressure vessel sealed with a PTFE lined screw cap for 12 hours. The mixture was cooled to room temperature over 1 hour and stored at 7 ° C for another 2 hours. The colorless needle formed was filtered off and washed with cold EtOH to give the product (0.21 g, 67%). The following physical, chemical and spectral parameters were obtained. R f (SiO 2 ,CH 2 Cl 2 / hexane) = 0.15; Mp. 151.4–151.7°C; 1 HNMR (600MHz, CDCl 3 ):δ8.06(s, residual H),8.05(d,J C-H =3.2Hz, residual H), 7.97(s, residual H), 7.92(s, residual H), 7.89(d, J C-H =3.8Hz, residual H), 7.82(s, residual H), 7.81(s, residual H), 7.64(s, residual H), 7.61(s, residual H), 7.58(s, residual H), 7.55(d, J C-H =5.3Hz, residual H),7.44(d,J C-H =2.9Hz, residual H), 7.43(s, residual H), 7.39(s, residual H), 5.57(d, J C-H =6.9 Hz, 2H) ppm; 13 C UDEFT NMR (151 MHz, CDCl 3 ):δ149.3(s),136.1(d,J C-C =66.0Hz),133.6(d,J C-C =4.0Hz),133.4(s),133.3(s),133.2(d,J C-C =5.3Hz),130.3(d,J C-C =52.5Hz),129.5(s,residual CH),129.1(t,J C-D =24.4Hz), 128.5–125.4 (m, multi-CD and residual CH signals), 123.7 (s, residual CH), 123.46 (t, J C-D =24.7Hz)ppm; IR(ATR): 3324(m),3182(w),2258(w),1620(w),1550(m),1438(w),1392(w),1335(w),1304(w),1252(m),1144(m),1088(m),1058( m),997(m),930(m),862(m),847(m),832(m),809(m),799(m),777(m),758(m),731(s),704(w),672(w),646(m),583(m)cm -1 .

[0323] f) Formation of 2,2'-(diazomethylene- 13 C) Dinaphthyl-d 14

[0324]

[0325] 2,2'-(diazomethylene- 13 C) Dinaphthyl-d 14 :MI Javed and M. Brewer, "Org. Synth. " 2008,85,189. The product was treated and isolated under light-proof conditions. Oxalyl chloride (0.12 mL, 0.17 g, 1.35 mmol, 1.05 equiv) in tetrahydrofuran (5.0 mL) was added to a solution of dimethyl sulfoxide (0.10 mL, 0.11 g, 1.41 mmol, 1.10 equiv) and tetrahydrofuran (anhydrous, 11.3 mL, 0.13 M) at -55 ° C for 5 minutes. The solution was kept between -55 ° C and -50 ° C for 30 minutes while stirring, and then cooled to -78 ° C. Over 5 minutes, (di(naphthalene-2-yl)methylene- 13 C) Hydrazine-d 14 A mixture of (0.40g, 1.28mmol, 1.00 equivalent) and triethylamine (0.37mL, 2.70mmol, 2.10 equivalent) in tetrahydrofuran (3.0mL) was added to the reaction solution to provide a dark red solution containing a large amount of white precipitates. The reaction mixture was kept at -78°C for 30 minutes, then filtered into a round-bottom flask through a medium porosity sintered glass funnel in a cold state, and the solid was rinsed with tetrahydrofuran (2×5mL). The filtrate was concentrated at room temperature by rotary evaporation. The red residue was redissolved in n-hexane (20mL), and quickly filtered through an activated basic alumina plug loaded in a medium porosity sintered glass funnel, and the solid was rinsed with n-hexane (~50mL) until the filtrate was colorless. The filtrate was concentrated by rotary evaporation at room temperature (to about 20mL) and stored overnight at 7°C. The precipitate formed was filtered and dried under vacuum to obtain the product (53.0mg, 28%) as a purple crystalline solid. The following physical, chemical and spectral parameters were obtained.f (Al 2 O 3 Basicity, hexane) = 0.49; Mp. 134.3 °C; 1 H NMR (600 MHz, C 6 D 6 ):δ7.66(d,J C-H =5.4Hz, residual H), 7.60(s, residual H), 7.58(s, residual H), 7.46(s, residual H), 7.28(d, J C-H =4.3 Hz, residual H) 7.23 (s, residual H), 7.22 (s, residual H) ppm; 13 C UDEFT NMR (151MHz, C 6 D 6 ): δ134.4(d,J=5.2Hz),132.2(s),129.2(d,J C-C =4.8Hz),128.9(t,J 1 C-D =24.2Hz),127.7(t,J 1 C-D =24.2Hz),127.3(t,J 1 C-D =24.4Hz),127.2(d,J C-C =68.1Hz),126.6,126.3(t,J 1 C-D =24.3Hz),125.6,125.4(t,J 1 C-D =24.5Hz),123.8,123.6(t,J 1 C-D =24.2Hz),123.5(t,J 1 C-D =24.2Hz),63.5(s)ppm; IR(ATR): 2267(w),2012(s),1600(m),1557(m),1439(m),1393(m),1322,(w),1201(m),912 (w),872(w),852(m),795(m),782(m),726(s),645(m),616(m),601(s),579(m)cm -1 .

[0326] g) Formation of di(naphthalene-2-yl)methanone- 13 Cd 14 (diazomethylene) dinaphthalene - 13 Cd 14 Diluted molecular crystals

[0327] Di(naphthyl)methanone- 13 Cd14 (0.80 g) was dissolved in hot ethyl acetate (HPLC grade, 90 mL, 0.030 M) and the solution was allowed to cool to room temperature. To this solution was added 2,2'-(diazomethylene) dinaphthyl- 13 Cd 14 (4.5 mg, 5400 ppm). An aliquot (5 milliliters, mL) of the resulting parent solution was added to a 10 mL vial using a syringe equipped with a 0.45 μm pore size syringe filter, and the vial was placed in a screw-top jar filled with ethanol (HPLC grade). Storage in the dark for 7 days at room temperature formed rare molecular crystals (parallelepiped, approximately 3×3×4 mm). The crystals were separated in the dark, washed with ethanol (HPLC grade) and dried in a vacuum. The rare molecular crystals can be stored in a freezer (T=-22° C.) in the dark for several months without detectable degradation.

[0328] In order to di(naphthalene-2-yl)methanone- 13 Cd 14 Di(naphthalene-2-yl)carbene- 13 Cd 14 Dopant molecules, only need to di (naphthalene-2-yl) ketone- 13 Cd 14 (diazomethylene) dinaphthalene 13 Cd 14 The dilute molecular crystals are exposed to light of the correct wavelength, as described herein.

[0329] Example 8: X-ray crystal structure of (diazomethylene) dinaphthalene embedded in di(naphthalene-2-yl)methanone

[0330] Diluted single crystals of 2,2'-(diazomethylene)binaphthalene embedded in di(naphthalene-2-yl)methanone were grown by slow vapor diffusion of ethanol into a solution of 2,2'-(diazomethylene)binaphthalene (340 ppm) and dilute solutions of ethyl acetate of di(naphthalene-2-yl)methanone (0.035 M) at room temperature over seven days in the dark. Appropriate crystals were selected and the Cu-K α radiation The Atlas diffractometer was mounted on a SuperNova, Dual, Cu. During data collection, the crystal was kept at 150.00 (14) Kelvin. The structure was solved using Olex2, the XT structure solver using the intrinsic phase method, and refined using the XL refinement package using the least squares method. All non-H atoms were refined with anisotropic thermal parameters. The H atoms in all structures were refined in the rigid group model at calculated positions. Table 1 shows the resulting crystal data. Due to the nature of the diffraction measurements, only periodically assembled molecules (i.e., the bulk material) appear in the crystal structure, and no carbene precursors are observed.

[0331] Table 1: Crystallographic data and structural refinement of rare-molecule crystals of 340 ppm 2,2'(diazomethylene) dinaphthalene in di(naphthalene-2-yl)methanone

[0332]

[0333] (a)GooF=[∑[w(F 2 0 -F 2 c ) 2 / (np)] 1 / 2 , where n is the number of reflections and p is the total number of refined parameters.

[0334] (b)R 1 =∑||F 0 |-|F c | / ∑|F 0 |;wR 2 =[∑[w(F 2 0 -F 2 c ) 2 ] / ∑[w(F 2 0 ) 2 ]] 1 / 2

[0335] Example 9: General synthetic route for forming nitrene dopant molecules

[0336] The general synthetic route for forming nitrene dopant molecules in organic host materials is shown below.

[0337]

[0338] Nitren materials are prepared following principles similar to those outlined above for the preparation of carbenes. That is, a photoactive nitrene precursor is embedded in an inert matrix (i.e., a host material) by substitutional doping, and after photolysis using an appropriate light source, the activated nitrene 10 is obtained. Nitenes can be attached directly to aryl groups or via sulfonyl (SO 2 -) linker connection. Substituents at the nitrene aryl unit can be used to fine-tune thermodynamic / kinetic stability and electronic properties. Here, again, one or more substituents R can be attached, such as one or more nitrile, carbonyl, carboxylic acid, ester, alkyl, aryl, heteroaryl, imine, amine, nitro, phosphine, alcohol, ether, thiol, thioether, or halogen groups. As in the case of carbenes, such groups can be selected (e.g., using computational molecular modeling, high-throughput synthesis and screening, etc.) to fine-tune electronic properties, such as ZFS, zero phonon lines, spectral stability, and / or thermodynamic / kinetic stability.

[0339] The precursors of nitrene (10) are aryl azides (–N 3 , 11), aryl isocyanate (-NCO, 12), or iminoiodoalkane (13). Each of these groups can be photolyzed with UV / visible light (λ = 200 to 500 nm) to afford nitrene and dinitrogen, respectively. 2 , carbon monoxide CO or an aryl iodide molecule.

[0340]

[0341] An exemplary approach for embedding an aryl azide precursor (15) into a structurally related matrix (16) is shown below.

[0342]

[0343] Example 10: Formation of rare molecular crystals of 4-azidobenzoic acid in 4-iodobenzoic acid

[0344] 4-Iodobenzoic acid (1.00 g) was dissolved in methanol (HPLC grade, 50 mL, 0.080 M) and the solution was cooled to room temperature. In the dark, 4-azidobenzoic acid (0.2 M in tert-butyl methyl ether, ≥95.0%, 130 μL, 6600 ppm) was added to this solution. An aliquot (8 milliliters, mL) of the resulting parent solution was added to a 10 mL vial using a syringe equipped with a 0.20 μm pore size syringe filter and the vial was stored in the dark for 4 days at room temperature. Dilute molecular crystals (thin rectangular plates, about 5×10×0.01 mm) were isolated in the dark, washed with a small amount of cold methanol (HPLC grade) and dried in a vacuum.

[0345] To generate 4-azidobenzoic acid dopant molecules in a 4-iodobenzoic acid host material, it is only necessary to expose a crystal of a dilute 4-azidobenzoic acid molecule in 4-iodobenzoic acid to light of the correct wavelength, as described herein.

[0346] Example 11: Optical crystal alignment for characterizing dopant molecules in host materials

[0347] The chemical system formed by embedding dopant molecules (or their precursors) into a host material may also be referred to herein as a "rare molecule crystal". Rare molecule crystals exhibit intrinsic birefringence, i.e., optical anisotropy. This property can be used to identify a set of axes of the material (i.e., an orthogonal axis system of optical refractive index ellipse axes n1, n2, and n3) for later comparison in an experimental setup. A microscope in transmission mode with two crossed linear polarizers (denoted as polarizer and analyzer) can be used to identify such axes.

[0348] Here, examples are given of typical configurations when the crystal is rotated in the field of view. Whenever the crossed polarizer axes are parallel to the vectors n1 and n2 (or more generally, to their projections in a plane perpendicular to the viewing direction), the crystal appears dark, whereas in the case of the crystal positioned in all other orientations, some light will pass through the analyzer and the crystal displays varying degrees of visible brightness. The maximum brightness of the birefringent material is observed when the polarizer and analyzer axes are at an angle of 45° relative to n1 and n2. This method can also be used to inspect the crystal for the presence of microscopic defects, such as strain-induced elongation effects (e.g., edge or screw dislocations).

[0349] Example 12: Preparation, photoactivation and annealing of carbene in host materials

[0350] After the crystal index ellipsoid has been macroscopically determined by the above-mentioned optical alignment method, a crystal of appropriate size is prepared from the original crystal by micromechanical methods (e.g., blade cutting, diamond wire saw, etc.), and if necessary, the surface is cut or polished with a suitable organic solvent (e.g., hexane, pentane, ethanol, methanol). The prepared crystal is transferred to a suitable sample holder (e.g., electron paramagnetic resonance (EPR) tube, glass sample holder, etc.) and placed in an apparatus of interest (e.g., EPR, optical instrument) together with an integrated cryostat. The sample is cooled to a temperature at which the generated carbene or nitrene is stable (depending on the carbene or nitrene itself and the matrix). Using an integrated optical access such as an optical fiber or window, the sample is irradiated with light (e.g., UV LED with a wavelength range between 300 and 400nm) in a macroscopic manner for a certain amount of time (depending on the light source output power, from a few seconds to a few hours) to activate the entire sample. This process involves converting the carbene or nitrene precursor molecule embedded in a suitable matrix into its corresponding carbene and a dinitrogen molecule (for nitrene, carbon monoxide and aryl iodide are also possible). Alternatively, a focused laser beam that can be adjusted in the lateral dimensions (x and y axis) can be used to activate regions of carbene or nitrene with a size > 200 nm.

[0351] Fig. 6A Shown is an exemplary continuous wave (cw) EPR signal associated with the stepwise photoactivation of di(naphth-2-yl)carbene (500 ppm) in di(naphth-2-yl)methanone using a green laser (λ=532 nm) at a temperature of 25 K. The appearance of the ground state triplet carbene can be seen. Figure 6B shows the change of applied light energy Fig. 6AThe double integral of the cw EPR signal of , and depicts the activation process for obtaining activated carbenes in dilute molecular crystals. Such a graph can be used as a calibration curve for activating dopant molecules (e.g., carbenes dopant molecules) in dilute molecular crystals. By using such a calibration curve (i.e., the amount of carbenes activated per irradiation), a well-defined carbenes density can be generated within the doped molecular crystal. The qubit pattern can be written into the sample (e.g., gradients, connecting regions, lattices) using photolithographic methods.

[0352] For very low temperatures (<140K in some cases, below 260K for other samples), carbene and dinitrogen molecules are dynamically trapped within the matrix, preventing them from adopting the molecular geometry typical of carbene. An annealing procedure involves controllably raising the temperature of the sample to a sample-dependent temperature (here 140K, for other samples >50K) for a sufficient amount of time (several minutes to several hours), which triggers a reorientation of the activated carbene and its immediate molecular environment within the dilute molecular crystal. The process can be monitored by cw EPR.

[0353] Fig. 7A Shown is an exemplary cw EPR signal associated with the conversion of di(naphthalen-2-yl)carbene (340 ppm) in freshly photoactivated di(naphthalen-2-yl)methanone to the annealed form at a temperature of 140 K. The annealing process is observed as the disappearance of the cw EPR signal at 6925 G and the appearance of a new signal at 7065 G. Figure 7B The annealing time is shown Fig. 7A The double integration of the cw EPR signal is usually accompanied by line sharpening and can therefore be used to further control the inhomogeneous broadening within the sample, which is required for efficient single-molecule manipulation by optical control. Figure 7B The appearance and disappearance of the annealing signal and the non-annealing signal at a specific time are shown, respectively.

[0354] Example 13: Di(naphthalene-2-yl)methanone-d 14 Di(naphth-2-yl)carbene-d 14 The spin-lattice (T 1 ) and spin- Spin (T 2 ) Relaxation time

[0355] The sample di(naphthalene-2-yl)methanone-d was measured at 466.6 mT. 14 Di(naphth-2-yl)carbene-d 14 (5400ppm) spin-lattice (T 1 ) relaxation time, where the magnetic field is roughly parallel to the zero-field splitting tensor B 0 ||D X A principal axis. 1The measurements were made using an inversion recovery sequence with Hahn echo based detection (π-T-π / 2-τ-π-τ-echo). The measurements were made using rectangular 10 ns π / 2 pulses and 20 ns π pulses with 16-step phase cycling. The data were fitted using a stretched exponential function to extract T 1 The average and maximum values ​​of T 1 Deviations from the monoexponential behavior of the curve can be associated with inhomogeneities in the microscopic spin environment in the sample, for example, through an inhomogeneous distribution of carbene spins. It can be rewritten as a continuous distribution of a single exponential function, where the distribution can be expressed according to T 1,char and exponent β to evaluate its mean value (T 1,av ) and the most likely value (T 1,max ). Fig. 8A An exemplary decay curve is shown as well as a temperature for extracting T at 3.5 K. 1 Stretched exponential fit curves of the time average and maximum values. Figure 8B Shown in the temperature range of 3.5K to 25K T 1 Exemplary graphs of the temperature dependence of the time average and most probable values.

[0356] The spin-spin (T) was measured using a Hahn-echo pulse sequence (π / 2-τ-π-τ-echo). 2 ) relaxation times and fitted to a stretched exponential decay similar to the procedure described above. The measurements used rectangular 10 nsπ / 2 pulses and 20 nsπ pulses with four-step phase cycling. Fig. 9 The decay curves of protonated and deuterated dilute molecular crystals are shown, and the T of the dilute molecular crystal after full deuteration is highlighted. 2 For example, for the protonated sample (di(naphthalene-2-yl)carbene in di(naphthalene-2-yl)methanone (5400 ppm)), a most likely value T of 4.78 μs was observed. 2,max and an average T of 2.67μs 2,av , while the fully deuterated sample di(naphthalene-2-yl)methanone-d 14 Di(naphth-2-yl)carbene-d 14 (5400ppm) gives the most likely value T of 53.6μs 2,max and an average value T of 16.0μs 2,av We note that the line shapes of these spectra may be distorted due to inhomogeneous broadening and electron spin echo envelope modulation (ESEEM) effects caused by the coupling of electron spins to nearby hydrogen and deuterium nuclei, respectively.

[0357] Example 14: Di(naphthalene-2-yl)methanone-d 14 Di(naphth-2-yl)carbene-d 14 The intermolecular coupling strength

[0358] Double electron-electron resonance (DEER) experiments were performed to probe the intermolecular coupling between randomly distributed carbenes in dilute molecular crystals. While sweeping the magnetic field, echo-detected field sweep spectra were collected using a Hahn-echo pulse sequence with a fixed τ value. In the DEER experiment, due to the 13 Ultrafine coupling (HFC) of C carbenes, using a crystal orientation B 0 ||D Y A large coupling of 214.6 MHz is observed to selectively address the probe and pump pulses. The π-pump pulse optimized by adiabatic inversion chirped pulses flips the coupled complexes and thus the probe spins experience additional decoherence due to static 2-pole coupling with the pump spins during the entire evolution time of the sequence. For example, Fig.10 The curve decays for the experiment with the pump pulse turned off and on are shown, along with the time elapsed for each decay that the initial signal has fallen to 1 / e. The two groups refer to different photoactivation steps (partial activation and full activation), which further highlights the tunability of the intermolecular coupling.

[0359] Example 15: Preparation, photoactivation and annealing of nitrene in host material

[0360] Fig.11A Shown is an exemplary continuous wave (cw) EPR signal associated with the stepwise photoactivation of 4-azenebenzoic acid in 4-iodobenzoic acid using light of wavelength λ = 370 nm at a temperature of 25 K. The appearance of the ground state triazine can be seen. Fig. 11B The activation time is shown Fig.11A The double integral of the cw EPR signal of , and depicts the activation process for obtaining activated nitrenes in dilute molecular crystals. Such a graph can be used as a calibration curve for activating dopant molecules (e.g., nitrene dopant molecules) in dilute molecular crystals. By using such a calibration curve (i.e., the amount of nitrenes activated per irradiation), a well-defined nitrene density can be generated within a doped molecular crystal. The qubit pattern can be written into the sample (e.g., gradient, connecting region, lattice) using photolithographic methods.

[0361] Fig.12 Shown is an exemplary cw EPR signal associated with the conversion of 4-nitrenebenzoic acid in freshly photoactivated 4-iodobenzoic acid to the annealed form at room temperature.

[0362] The foregoing description is presented for illustrative purposes. It is not exhaustive and is not limited to the precise form or embodiment disclosed. By considering the specification and the practice of the disclosed embodiments, modifications and adaptations of the embodiments will be apparent. For example, the described embodiments include hardware, but systems and methods consistent with the present disclosure can be implemented with hardware and software. In addition, although certain components have been described as being coupled to each other, such components can be integrated with each other or distributed in any suitable manner.

[0363] In addition, although illustrative embodiments have been described herein, the scope includes any and all embodiments having equivalent elements, modifications, omissions, combinations (e.g., combinations of aspects of the various embodiments), adaptations, or variations based on the present disclosure. The elements in the claims are to be interpreted broadly based on the language employed in the claims, and are not limited to the examples described in this specification or during the practice of the application, which examples are to be understood as non-exclusive. Further, the steps of the disclosed methods may be modified in any manner, including reordering steps or inserting or deleting steps.

[0364] According to the detailed description, the features and advantages of the present disclosure are obvious, and therefore the appended claims are intended to cover all systems and methods that fall within the true spirit and scope of the present disclosure. As used herein, the indefinite articles "a" and "an" mean "one or more". Similarly, unless the use of plural terms is clear in a given context, it does not necessarily represent a plural number. In addition, since various modifications and changes will be easily made by studying the present disclosure, it is not desired to limit the present disclosure to the exact construction and operation shown and described, and therefore all suitable modifications and equivalents can be attributed to and fall within the scope of the present disclosure.

[0365] As used herein, unless otherwise specifically stated, the term "or" encompasses all possible combinations unless not feasible. For example, if it is stated that a component may include A or B, then unless otherwise specifically stated or not feasible, the component may include A, or B, or A and B. As a second example, if it is stated that a component may include A, B, or C, then unless otherwise specifically stated or not feasible, the component may include A, or B, or C, or A and B, or A and C, or B and C, or A and B and C.

[0366] Other embodiments will be apparent from consideration of the specification and practice of the embodiments disclosed herein. It is intended that the specification and examples be considered as examples only, with a true scope and spirit of the disclosed embodiments being indicated by the following claims.

Claims

1. A method for generating a non-classical computer, comprising: preparing at least one host material; embedding at least one precursor of at least one dopant molecule into the at least one host material, the at least one precursor comprising at least one cleavable moiety; and cutting the at least one cleavable portion to generate the at least one dopant molecule and the at least one cleaving molecule in the at least one host material, wherein: The at least one dopant molecule includes a qubit having at least a first qubit state and a second qubit state; The at least one dopant molecule is associated with an electronic energy level structure comprising a triplet electron manifold; The triplet electron manifold includes a first triplet state, a second triplet state, and a third triplet state; the first qubit state comprises a first linear combination of the first triplet state, the second triplet state, and the third triplet state; the second qubit state comprises a second linear combination of the first triplet state, the second triplet state, and the third triplet state; and The first qubit state is different from the second qubit state.

2. The method of claim 1, wherein the at least one cleavable portion comprises at least one photocleavable portion.

3. The method of claim 1, wherein the at least one photocleavable moiety comprises at least one diazo moiety, an azide moiety, an isocyanate moiety, or an iminoiodinane moiety.

4. The method of claim 3, wherein the at least one cleavage molecule comprises at least one dinitrogen molecule, a carbon monoxide molecule, or an aryl iodide molecule.

5. The method of any one of claims 1 to 4, wherein cleaving the at least one cleavable moiety comprises exposing the at least one precursor to light.

6. The method of claim 5, wherein the light has a central wavelength between about 200 nanometers (nm) and about 500 nm.

7. The method of any one of claims 1 to 6, wherein the at least one dopant molecule comprises a plurality of dopant molecules.

8. The method of any one of claims 1 to 7, wherein the host material comprises at least one organic molecule.

9. The method of any one of claims 1 to 8, wherein the host material comprises a crystalline host material, a single crystal host material, a polycrystalline host material, a liquid crystal host material, a powder host material, an amorphous host material, or a frozen solution host material.

10. The method according to any one of claims 1 to 9, wherein the host material comprises C4-C20 straight or branched alkanes; aromatic hydrocarbons; polyaromatic hydrocarbons optionally substituted by methylene, nitrile, carbonyl, carboxylate, alkyl, deuterated alkyl, aryl, deuterated aryl, heteroaryl, deuterated heteroaryl, borane, imine, amine, nitro, phosphine, thioether, ether, fluorine, chlorine, bromine, iodine or thiocarbonyl; diaryl ketones; naphthalene; anthracene; p-terphenyl; benzoic acid; fluorene; biphenyl; benzene; n-hexane; biphenylene; o-terphenylene; m-terphenylene; p-terphenylene; phenanthrene; di(naphthalene-2-yl)ketone; di(phenyl)ketone; or any partially or fully isotopically labeled derivatives thereof.

11. The method of any one of claims 1 to 10, wherein the host material comprises a thin film having a thickness of at most 100 nanometers (nm).

12. The method of any one of claims 1 to 11, wherein the at least one dopant molecule comprises an organic molecule.

13. The method of any one of claims 1 to 12, wherein the at least one precursor comprises a derivative of a carbene molecule; a derivative of a nitrene molecule; a diazo derivative of a carbene molecule; an azide derivative of a nitrene molecule; an isocyanate derivative of a nitrene molecule; an imidoiodinane derivative of a nitrene; (diazomethylene) dinaphthalene; (diazomethylene) diphenyl; 4-azidobenzoic acid; or any partially or fully isotopically labeled derivative thereof.

14. The method of any one of claims 1 to 13, wherein the at least one dopant molecule comprises a carbene molecule; a nitrene molecule; a di(naphthalene-2-yl)carbene molecule; a di(phenyl)carbene molecule; or any partially or fully isotopically labeled derivative thereof.

15. The method according to any one of claims 1 to 14, wherein the plurality of dopant molecules are arranged in a pseudo two-dimensional (pseudo-2D) layer.

16. The method of claim 15, wherein the pseudo-2D layer comprises a self-assembled monolayer (SAM).

17. A method according to any one of claims 1 to 16, wherein the average distance between dopant molecules is at most 20 nm.

18. The method according to any one of claims 1 to 17, wherein the at least one dopant molecule is present in an amount of at least 10 6 Dopant molecules / cubic micrometer (μm 3 ) is contained in the at least one host material.

19. The method according to any one of claims 1 to 18, wherein: The at least one dopant molecule comprises a plurality of dopant molecules; A first dopant molecule of the plurality of dopant molecules is configured to absorb first electromagnetic energy having a first center wavelength or a first center frequency; A second dopant molecule of the plurality of dopant molecules is configured to absorb second electromagnetic energy having a second center wavelength or a second center frequency; and The first center wavelength or the first center frequency is different from the second center wavelength or the second center frequency.

20. The method of claim 19, wherein: The first center wavelength or the first center frequency is associated with a first wavelength range or a first frequency range having a first full width at half maximum (FWHM) bandwidth; The second center wavelength or the second center frequency is associated with a second wavelength range or a second frequency range having a second FWHM bandwidth; and The first wavelength range or the first frequency range within the first FWHM bandwidth and the second wavelength range or the second frequency range within the second FWHM bandwidth do not overlap.

21. The method of claim 20, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 megahertz (MHz).

22. The method of any one of claims 19 to 21, wherein the first central wavelength or the second central wavelength is between 200 nm and 1,000 nm.

23. The method of claim 21, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 gigahertz (GHz).

24. The method of claim 23, wherein the first center frequency or the second center frequency is between 1 MHz and 100 GHz.

25. The method of any one of claims 1 to 24, wherein the triplet electron manifold comprises a ground state triplet (GST) electron manifold.

26. A system for performing non-classical computing, comprising: at least one host material; at least one dopant molecule, the at least one dopant molecule contained in the at least one host material; as well as at least one cleaving molecule, the at least one cleaving molecule being contained in the at least one host material, wherein: The at least one dopant molecule includes a qubit having at least a first qubit state and a second qubit state; The at least one dopant molecule is associated with an electronic energy level structure comprising a triplet electron manifold; The triplet electron manifold includes a first triplet state, a second triplet state, and a third triplet state; the first qubit state comprises a first linear combination of the first triplet state, the second triplet state, and the third triplet state; the second qubit state comprises a second linear combination of the first triplet state, the second triplet state, and the third triplet state; and The first qubit state is different from the second qubit state.

27. The system of claim 26, wherein the at least one dopant molecule and the at least one cleaving molecule are generated by cleaving at least one precursor of the at least one dopant molecule, the at least one precursor comprising at least one cleavable portion.

28. The system of claim 27, wherein the at least one cuttable portion comprises at least one photocuttable portion.

29. The system of claim 28, wherein the at least one photocleavable moiety comprises at least one diazo moiety, an azide moiety, an isocyanate moiety, or an imidoiodoalkane moiety.

30. The system of claim 29, wherein the cleavage molecule comprises at least one of a dinitrogen molecule, a carbon monoxide molecule, or an aryl iodide molecule.

31. The system of any one of claims 27 to 30, wherein cutting the at least one precursor comprises exposing the at least one precursor to light.

32. The system of claim 31, wherein the light has a central wavelength between approximately 200 nanometers (nm) and approximately 500 nm.

33. The system of any one of claims 26 to 32, wherein the at least one dopant molecule comprises a plurality of dopant molecules.

34. The system of any one of claims 26 to 33, wherein the host material comprises at least one organic molecule.

35. The system of any one of claims 26 to 34, wherein the host material comprises a crystalline host material, a single crystal host material, a polycrystalline host material, a liquid crystal host material, a powder host material, an amorphous host material, or a frozen solution host material.

36. A system according to any one of claims 26 to 35, wherein the host material comprises C4-C20 straight or branched chain alkanes; aromatic hydrocarbons; polyaromatic hydrocarbons optionally substituted with methylene, nitrile, carbonyl, carboxylate, alkyl, deuterated alkyl, aryl, deuterated aryl, heteroaryl, deuterated heteroaryl, borane, imine, amine, nitro, phosphine, thioether, ether, fluorine, chlorine, bromine, iodine or thiocarbonyl; diaryl ketones; naphthalene; anthracene; p-terphenyl; benzoic acid; fluorene; biphenyl; benzene; n-hexane; diphenylene; o-terphenylene; m-terphenylene; p-terphenylene; phenanthrene; di(naphthalen-2-yl)methanone; di(phenyl)methanone; or any partially or fully isotopically labeled derivatives thereof.

37. The system of any one of claims 26 to 36, wherein the host material comprises a thin film having a thickness of at most 100 nanometers (nm).

38. The system of any one of claims 26 to 37, wherein the at least one dopant molecule comprises an organic molecule.

39. The system of any one of claims 26 to 38, wherein the at least one precursor comprises a derivative of a carbene molecule; a derivative of a nitrene molecule; a diazo derivative of a carbene molecule; an azido derivative of a nitrene molecule; an isocyanate derivative of a nitrene molecule; an imidoiodoalkane derivative of a nitrene molecule; (diazomethylene) dinaphthalene; (diazomethylene) diphenyl; 4-azidobenzoic acid; or any partially or fully isotopically labeled derivative thereof.

40. The system of any one of claims 26 to 39, wherein the at least one dopant molecule comprises a carbene molecule; a nitrene molecule; a di(naphthalene-2-yl)carbene molecule; a di(phenyl)carbene molecule; or any partially or fully isotopically labeled derivative thereof.

41. The system of any one of claims 26 to 40, wherein the plurality of dopant molecules are arranged in a pseudo two-dimensional (pseudo-2D) layer.

42. The system of claim 41, wherein the pseudo-2D layer comprises a self-assembled monolayer (SAM).

43. The system of any one of claims 26 to 42, wherein the average distance between dopant molecules is at most 20 nm.

44. The system of any one of claims 26 to 43, wherein the at least one dopant molecule is present in an amount of at least 10 6 Dopant molecules / cubic micrometer (μm 3 ) is contained in the at least one host material.

45. A system according to any one of claims 26 to 44, wherein: The at least one dopant molecule comprises a plurality of dopant molecules; A first dopant molecule of the plurality of dopant molecules is configured to absorb first electromagnetic energy having a first center wavelength or a first center frequency; A second dopant molecule of the plurality of dopant molecules is configured to absorb second electromagnetic energy having a second center wavelength or a second center frequency; and The first center wavelength or the first center frequency is different from the second center wavelength or the second center frequency.

46. ​​The system of claim 45, wherein: The first center wavelength or the first center frequency is associated with a first wavelength range or a first frequency range having a first full width at half maximum (FWHM) bandwidth; The second center wavelength or the second center frequency is associated with a second wavelength range or a second frequency range having a second FWHM bandwidth; and The first wavelength range or the first frequency range within the first FWHM bandwidth and the second wavelength range or the second frequency range within the second FWHM bandwidth do not overlap.

47. The system of claim 46, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 megahertz (MHz).

48. The system of any one of claims 45 to 47, wherein the first central wavelength or the second central wavelength is between 200 nm and 1,000 nm.

49. The system of claim 48, wherein the first FWHM bandwidth or the second FWHM bandwidth is at most 100 gigahertz (GHz).

50. The system of claim 49, wherein the first center frequency or the second center frequency is between 1 MHz and 100 GHz.

51. The system of any one of claims 26 to 50, wherein the triplet electron manifold comprises a ground state triplet (GST) electron manifold.

52. The system according to any one of claims 26 to 51 further comprises at least one initialization unit, wherein the at least one initialization unit is configured to direct a third electromagnetic energy to the at least one dopant molecule, thereby initializing the quantum state of the at least one dopant molecule to the first qubit state or the second qubit state.

53. The system of claim 52, wherein the third electromagnetic energy comprises at least one wavelength between 200 nm and 1,000 nm.

54. The system according to any one of claims 26 to 53, further comprising at least one non-classical operation unit, wherein the at least one non-classical operation unit is configured to apply fourth electromagnetic energy to the at least one dopant molecule, thereby performing at least one non-classical operation on the at least one dopant molecule.

55. The system of claim 54, wherein the at least one non-classical operation comprises at least one quantum operation, at least one quantum computing operation, at least one quantum gate operation, at least one quantum simulation operation, or at least one quantum annealing operation.

56. The system of claim 54 or 55, wherein the fourth electromagnetic energy comprises at least one frequency between 1 MHz and 100 GHz.

57. The system of any one of claims 54 to 56, wherein after performing the at least one non-classical operation, a result of the at least one non-classical operation is related to an electronic state of the at least one dopant molecule.

58. The system of claim 57, further comprising at least one storage unit configured to apply fifth electromagnetic energy and sixth electromagnetic energy to the at least one dopant molecule, wherein the fifth electromagnetic energy and the sixth electromagnetic energy are collectively configured to transfer information from the electronic state to the nuclear spin state of the at least one dopant molecule.

59. The system of claim 58, wherein the fifth electromagnetic energy and the sixth electromagnetic energy are configured to jointly apply a swap gate to the at least one dopant molecule, thereby transferring the information from the electronic state to the nuclear spin state of the at least one dopant molecule.

60. The system of claim 58 or 59, wherein the fifth electromagnetic energy comprises at least one frequency between 1 kHz and 100 MHz, and wherein the sixth electromagnetic energy comprises at least one frequency between 1 MHz and 100 GHz.

61. The system according to any one of claims 26 to 60 further comprises at least one detection unit, wherein the at least one detection unit is configured to detect the electronic state of the at least one dopant molecule or the nuclear spin state of the at least one dopant molecule, thereby obtaining the result of the at least one non-classical operation.

62. The system of claim 61, wherein the at least one detection unit is configured to apply a seventh electromagnetic energy to the at least one dopant molecule to obtain the result of the at least one non-classical operation.

63. A system according to claim 61 or 62, wherein the at least one detection unit comprises at least one optical detector, and the at least one optical detector is configured to detect light emitted by the at least one dopant molecule in response to the seventh electromagnetic energy.

64. The system of claim 63, wherein the light emitted by the at least one dopant molecule has a first optical property associated with the first qubit state and a second optical property associated with the second qubit state, and wherein the first optical property is different from the second optical property.

65. The system of claim 64, wherein the first optical property or the second optical property comprises an intensity, polarization, wavelength, or frequency of the light.

66. The system of any one of claims 26 to 65, further comprising a cryogenic unit configured to contain the at least one bulk material and to cool the at least one bulk material to a temperature of at most 20K.

67. The system of claim 66, wherein the cryogenic unit comprises a helium cryocooler or a closed cycle helium cryocooler.

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