Probability bit device based on fullerene Y3N-C80 and preparation method thereof

By embedding fullerene Y3N@C80 molecules between graphene electrodes, the coupling effect of charge transfer and molecular vibration to generate dipole moments is achieved, and the randomness and controllability of nanomaterial-based probabilistic bit devices is solved, and it is suitable for quantum information technology.

CN120302870AActive Publication Date: 2025-07-11NANKAI UNIV

Patent Information

Application Number
CN202510750376.2
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-06-06
Publication Date
2025-07-11
Estimated Expiration
2045-06-06

AI Technical Summary

Technical Problem

The existing nanomaterial-based probability bit devices have shortcomings in terms of randomness and controllability, making it difficult to achieve a stable and adjustable random binary conductivity state, and the state of traditional metal oxide transistors is not random enough.

Method used

Fullerene Y3N@C80 molecules are used as functional molecules, and they are embedded between graphene electrodes through chemical decoupling method to form a single-molecular probability bit device. The dipole moment generated by charge transfer and molecular vibration is used to achieve conductive flip under the transverse source-drain bias voltage, and stability is enhanced through amide covalent bonding.

Benefits of technology

It realizes random high/low conductivity switching at a single molecular scale, and the conductivity ratio is adjustable. The device shows efficient randomness and tunability, enhances chemical stability and integration, and is suitable for high-density integration and miniaturization functional chips.

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Abstract

The invention relates to the technical field of quantum information devices, and particularly discloses a fullerene Y3N-C80-based probability bit device and a preparation method thereof.The probability bit device comprises fullerene Y3N-C80 molecules, graphene point electrodes, a metal electrode and a substrate, the fullerene Y3N-C80 molecules are connected to the two graphene point electrodes, the graphene point electrodes are connected to the metal electrode, and the metal electrode is connected to the substrate. The graphene point electrode and the metal electrode are located on the substrate, and the fullerene Y3NatC80 molecules are connected with the graphene point electrode through amide covalent bonds. According to the invention, the electric dipole moment is driven to overturn under the condition that different transverse source-drain bias voltages are applied to the probability bit device, so that the probability bit device can present different conductive states, the time proportion of the conductive states can be adjusted according to the magnitude of the applied transverse source-drain bias voltages, and the purpose of regulating and controlling the single-molecule probability bit device is achieved.
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Description

Technical Field

[0001] The present invention relates to the technical field of quantum information devices, and particularly to a probability bit device based on fullerene Y3N@C 80 and a preparation method thereof. Background Art

[0002] Exploring the stochastic dynamics in nanomaterials is of great significance in the emerging field of probabilistic computing, which is a new paradigm beyond the traditional von Neumann architecture and aims to solve problems such as combinatorial optimization, reversible logic, and Bayesian inference. The key component of probabilistic computing is the probabilistic bit (p-bit), which is a classical entity that can generate random "0" and "1" with a controllable probability. For example, Chinese Patent Publication No. CN117135995A discloses a spin-orbit torque probabilistic bit and a control method thereof controlled by double pulses. When a first pulse current and a second pulse current are synchronously applied, the first pulse current flows through the spin-orbit coupling layer to induce the magnetization of the magnetic free layer, and the second pulse current sequentially flows through the top electrode layer, the magnetic reference layer, the spacer layer, the magnetic free layer, and the spin-orbit coupling layer to change the energy symmetry of the magnetization of the magnetic free layer, thereby regulating the probability of the magnetic free layer being stabilized in different magnetization states. Another example is Chinese Patent Publication No. CN118102851A, which discloses a logic device including a probabilistic bit based on spin-orbit torque-induced magnetization reversal, a preparation method, and an application thereof. It includes a substrate; a spin current generation layer located on the substrate, which is used to form a spin-orbit coupling effect under the action of a current to generate a spin current and generate heat energy under the action of the current; a functional layer located on the spin current generation layer, which is used to transfer the spin current and heat energy; a magnetic layer located on the functional layer; the spin current injected into the magnetic layer generates a spin-orbit torque in the magnetic layer, so that the magnetic layer undergoes magnetization reversal under the induction of the spin-orbit torque and heat energy. The states of traditional computing units based on traditional metal oxide transistors are often not truly random.

[0003] With the emergence of nanomaterials with intrinsic fluctuating dynamics, ideally, the nanomaterials involved can exhibit binary high and low conductance states that fluctuate over time, and the fluctuation probability can be adjusted by external stimuli.

[0004] In nanomaterials, graphene-based single-molecule devices are an important method for constructing stable single-molecule nanodevices. Based on graphene single-molecule devices, taking advantage of the stability and high electron mobility of graphene, by preparing graphene into electrodes, it becomes possible to construct stable and controllable single-molecule-level electronic devices. Currently, various molecular electronic devices including field-effect transistors, switches, rectifiers, memristors, and light-emitting diodes have been successfully constructed with graphene-based single-molecule devices. These devices not only show broad application prospects in chip miniaturization, integration, and multifunctionality, but also their unique physical and chemical properties bring new opportunities to the field of quantum information technology. Selecting chemical molecules with certain characteristics along the existing technical background to construct nanoscale molecular electronic devices makes it possible for nanoscale probabilistic bit devices to become new computing units. Summary of the Invention

[0005] The present invention aims to solve the above problems. To this end, the present invention provides a probabilistic bit device based on fullerene Y3N@C 80 and its preparation method. By assembling the encapsulated fullerene Y3N@C 80 molecules between graphene electrodes with a nanogap through a chemical decoupling method to form a single-molecule probabilistic bit device. In the single-molecule probabilistic bit device, the fullerene Y3N@C 80 molecules first undergo charge transfer to form delocalized charges, and then the delocalized charges generate a stable electric dipole moment with the central point; combined with the coupling effect between the molecular orbit and the dipole generated by the vibration of the fullerene molecule itself, when different transverse source-drain biases are applied to the device, the electric dipole moment is driven to flip, enabling the fullerene Y3N@C 80 molecular device to exhibit different conductance states, and the time ratio of the conductance states can be adjusted by the magnitude of the applied transverse source-drain bias, achieving the purpose of regulating the single-molecule probabilistic bit device.

[0006] The present invention provides a probabilistic bit device based on fullerene Y3N@C 80 adopting the following technical solutions: including: fullerene Y3N@C 80 molecules, graphene dot electrodes, metal electrodes, and a substrate. The fullerene Y3N@C 80 molecules are connected to two graphene dot electrodes, the graphene dot electrodes are connected to the metal electrodes, the graphene dot electrodes and the metal electrodes are located on the substrate, and the fullerene Y3N@C 80 molecules are connected to the graphene dot electrodes through amide covalent bonds.

[0007] Further, two groups of graphene dot electrodes and metal electrodes are respectively used as the source electrode and the drain electrode, and a transverse source-drain bias is applied to the source electrode and the drain electrode to obtain a current signal with a hopping state.

[0008] Further, by applying lateral source-drain bias voltages of different magnitudes, current signals with different probability bits are obtained.

[0009] Further, by applying a lateral source-drain bias voltage of 0.11~0.27 V, the probability bits of the obtained current signals are 21.70%~91.46%.

[0010] The present invention also provides a preparation method for a probability bit device based on fullerene Y3N@C 80 to prepare the above-mentioned probability bit device based on fullerene Y3N@C 80 The technical solution adopted is as follows: It includes the following steps: S1: Fabricate a graphene-PMMA structure, transfer the graphene-PMMA structure to the surface of a silicon wafer and mark the pattern; S2: Prepare graphene dot electrodes; S3: Synthesize fullerene Y3N@C 80 molecules; S4: Condense the fullerene Y3N@C 80 molecules with the graphene dot electrodes by amide condensation to obtain a probability bit device based on fullerene Y3N@C 80 .

[0011] Further, S3 includes the following steps: S31: Under a nitrogen atmosphere, keep the three-necked flask at 0 °C in an ice bath, add Compound 1 and dichloromethane (DCM), stir, and then slowly add MnO2; remove the ice bath, react at room temperature for 24 h, filter and wash with dichloromethane, add the crude product obtained by rotary evaporation of the filtrate to the three-necked flask; under a nitrogen atmosphere, add Compound 2 and toluene, heat at 100 °C for 6 h; filter to obtain the crude product, and purify the crude product to obtain Compound 3; S32: Under a nitrogen atmosphere, add Compound 3, Compound 4, K2CO3 and tetrakis(triphenylphosphine)palladium (Pd(PPh3)4) to a two-necked flask; add a mixture of toluene and water, heat to 110 °C, and reflux for 30 h; after cooling to room temperature, pour the reaction mixture into water, extract with dichloromethane, dry the organic layer with anhydrous sodium sulfate, remove the solvent, and purify to obtain Compound 5; S33: Under a nitrogen atmosphere, add Compound 5 and a dichloromethane solution of 50% trifluoroacetic acid (TFA) to the two-necked flask, stir at room temperature for 2 h; add saturated sodium bicarbonate solution, extract, and wash repeatedly until it is neutral, and rotary evaporate the collected organic layer to remove the solvent to obtain fullerene Y3N@C 80 molecules; .

[0012] Further, S4 includes the following steps: S41: Make the fullerene Y3N@C80 The molecule is in a nitrogen atmosphere, and anhydrous pyridine is added. Fullerene Y3N@C 80 The molecule is dissolved in anhydrous pyridine; S42: Add 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and the pyridine solution dissolving fullerene Y3N@C 80 to the graphene dot electrode, and react for more than 48 h in a nitrogen atmosphere to obtain a probabilistic bit device based on fullerene Y3N@C 80

[0013] Furthermore, in S41, take fullerene Y3N@C 80 molecules and place them in a two-necked flask. Inject dichloromethane and trifluoroacetic acid, and react for more than 2 h in a nitrogen atmosphere. Remove trifluoroacetic acid by extraction with sodium hydroxide, and transfer the remaining solution to a pear-shaped flask; Place the remaining solution in a nitrogen atmosphere by air replacement, inject anhydrous pyridine into the pear-shaped flask, and dissolve fullerene Y3N@C 80 molecules.

[0014] Furthermore, in S4, prepare multiple probabilistic bit devices based on fullerene Y3N@C 80 at one time. Each probabilistic bit device based on fullerene Y3N@C 80 is prepared by amide condensation of a single fullerene Y3N@C 80 molecule with a pair of two graphene dot electrodes.

[0015] One or more of the above technical solutions in the embodiments of the present invention have at least one of the following technical effects: 1. The present invention uses fullerene Y3N@C 80 molecules as functional molecules to prepare a single-molecule probabilistic bit device based on fullerene Y3N@C 80 . The delocalized charges generated by charge transfer on the C 80 cage of the endohedral fullerene in the fullerene Y3N@C 80 molecule generate a stable electric dipole moment with the central point. Under the drive of different lateral source-drain bias voltages, the dipoles between the endohedral fullerene Y3N and the C 80 cage flip under the coupling action of molecular vibration to generate two different flip states, which ensures that different lateral source-drain bias voltages can be applied to adjust the conductive state of the device. Secondly, combined with the coupling action between the stretching vibration of the fullerene molecule itself to generate molecular orbitals and the electric dipole moment, it ensures the dynamic switching that can be monitored by collecting the change of the current signal within a certain time range: the generation of random high / low conductance state jumps. This probabilistic bit device has good randomness or uncertainty characteristics, and the state of the molecule can be read through conductance, realizing a probabilistic bit at the single-molecule scale.

[0016] ​2. The probability bit device based on fullerene Y3N@C of the present invention 80 exhibits binary high (1) and low (0) conductance states that spontaneously fluctuate over time, and the fluctuation probability can be finely tuned by external stimuli, thus enabling efficient computing. The proportion of the high / low conductance states in the total amount of data under each test condition can be extended to probabilistic states, which exhibit continuously tunable characteristics, broadening the research direction for realizing tunable probabilistic computational nanodevices with high operating stability.

[0017] 3. The preparation method of the probability bit device based on fullerene Y3N@C of the present invention 80 forms an amide covalent bond connection through the amino group –NH2 at the bottom of the molecule and the carboxyl group –COOH at the end of the graphene dot electrode, significantly enhancing the chemical stability of the device and ensuring the long-term reliability of the single-molecule probability bit device under complex operating conditions.

[0018] 4. The preparation method of the probability bit device based on fullerene Y3N@C of the present invention 80 Through in-situ drawing of the external lead electrode and electron beam lithography etching process, the electrode position and hole position can be designed independently, with strong designability at the nanoscale. A row of equally spaced dotted lines can be designed between a pair of electrodes, and finally 169 pairs of graphene array electrodes can be obtained, and finally connected to the fullerene Y3N@C 80 molecule to fabricate 169 single-molecule probability bit devices, achieving significant miniaturization of the device size and showing extremely high integration. This characteristic provides new ideas for the miniaturization and high-density integration of functional chips, laying a technical foundation for the future development of micro-nano optoelectronics.

[0019] The additional aspects and advantages of the present invention will be partly given in the following description, partly become apparent from the following description, or be understood through the practice of the present invention. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] In order to more clearly illustrate the technical solutions in the present invention or the prior art, the following will briefly introduce the drawings required for use in the description of the embodiments or the prior art. Obviously, the following drawings are some embodiments of the present invention. For those of ordinary skill in the art, without creative efforts, other drawings can also be obtained based on these drawings.

[0021] Figure 1 is a schematic structural diagram of the probability bit device provided by the present invention.

[0022] Figure 2 is a schematic diagram of the random flipping of the molecule of the probability bit device provided by the present invention under the drive of an electric field.

[0023] Figure 3It is the I-t characteristic curve diagram of the probabilistic bit device provided by the present invention under different lateral source-drain bias voltages.

[0024] Figure 4 It is the fitting diagram of the lateral source-drain bias voltage of the probabilistic bit device provided by the present invention and the probabilistic bit.

[0025] Explanation of reference numerals: 1. Graphene dot electrode; 2. Metal electrode; 3. Substrate; 4. Fullerene Y3N@C 80 molecule. Detailed implementation manners

[0026] To make the objectives, technical solutions and advantages of the present invention clearer, the technical solutions in the present invention will be clearly and completely described below with reference to the accompanying drawings in the present invention. Obviously, the described embodiments are some but not all of the embodiments of the present invention. All other embodiments obtained by those of ordinary skill in the art without making creative efforts based on the embodiments in the present invention belong to the scope protected by the present invention. The following embodiments are used to illustrate the present invention, but cannot be used to limit the scope of the present invention.

[0027] In the description of this specification, the descriptions referring to terms such as "one embodiment", "some embodiments", "example", "specific example", or "some examples" etc. mean that the specific features, structures or characteristics described in connection with the embodiment or example are included in at least one embodiment or example of the embodiments of the present invention. In this specification, the schematic representations of the above terms do not necessarily refer to the same embodiment or example. Moreover, the specific features, structures or characteristics described can be combined in any one or more embodiments or examples in a suitable manner. In addition, without conflict, those skilled in the art can combine the different embodiments or examples described in this specification and the features of different embodiments or examples.

[0028] The following is a further detailed description of the present invention in conjunction with Figures 1 to 4 to describe a probabilistic bit device based on fullerene Y3N@C 80 of the present invention and its preparation method: In this embodiment, as Figure 1 shown, a probabilistic bit device based on fullerene Y3N@C 80 is provided, including: fullerene Y3N@C 80 molecule 4, graphene dot electrode 1, metal electrode 2 and substrate 3. The fullerene Y3N@C 80 molecule is connected to two graphene dot electrodes, the graphene dot electrodes are connected to the metal electrodes, the graphene dot electrodes and the metal electrodes are located on the substrate, and the fullerene Y3N@C 80The molecule is covalently bonded to the graphene dot electrodes through amide bonds. In this embodiment, the metal electrode is a gold electrode and the substrate is a silicon substrate.

[0029] Fullerene Y3N@C 80 The graphene dot electrodes and the metal electrodes on both sides of the molecule respectively form the source electrode and the drain electrode. That is, two groups of graphene dot electrodes and metal electrodes are used as the source electrode and the drain electrode respectively.

[0030] Based on fullerene Y3N@C 80 The probabilistic bit device has the following characteristics: (1) There are extra electrons on the encapsulated Y3N molecule in the encapsulated fullerene Y3N@C 80 These electrons serve as the charge source for forming delocalized charges. When charge transfer occurs between the encapsulated fullerene Y3N and the C 80 cage for the extra electrons, the charge transfers from the encapsulated part to the carbon cage and becomes conductive delocalized charges.

[0031] (2) The delocalized charges on the C 80 cage of the encapsulated fullerene generate a stable electric dipole moment with the center point, and the stretching vibration of the fullerene molecule itself generates a coupling effect between the molecular orbit and the electric dipole moment. Under different applied transverse source-drain biases, the dipole between the encapsulated fullerene Y3N and the C 80 cage generates a driving flip.

[0032] (3) Apply a transverse source-drain bias to the source electrode and the drain electrode of the probabilistic bit device to obtain a current signal with a jump state, and thus an I-t characteristic curve with a jump state can be plotted. By changing the magnitude of the source-drain bias, I-t characteristic curves with different jump states can be obtained. The ratio of the high / low conductance states of each I-t characteristic curve shows a characteristic that varies with the change of the source-drain bias.

[0033] (4) The ratio of the high / low conductance states to the total amount of data under each test condition can be extended to a probabilistic state, which shows a continuously tunable characteristic. Divide the amount of data in the low conductance state by the total amount of all collected data and define it as the probabilistic bit. Apply different magnitudes of transverse source-drain biases to obtain current signals with different probabilistic bits. Through experiments, when applying a transverse source-drain bias of 0.11~0.27V, the probabilistic bits of the obtained current signals are 21.70%~91.46%.

[0034] In this embodiment, a preparation method for a probabilistic bit device based on fullerene Y3N@C 80 is also provided to prepare the above-mentioned probabilistic bit device based on fullerene Y3N@C 80 The technical solution adopted is as follows: It includes the following steps: S1: Fabricate a graphene-PMMA structure, transfer the graphene-PMMA structure to the surface of a silicon wafer and mark the pattern. The specific steps are as follows: S11: Immerse and clean the silicon wafer (silicon substrate) in a piranha solution at 110 °C for 3 h, then ultrasonically clean it with acetone, absolute ethanol, and ultrapure water, and dry it with nitrogen for standby. Specifically, prepare a mixed piranha solution with a volume ratio of concentrated sulfuric acid to hydrogen peroxide of 3:7 in a beaker. Place the cut silicon wafer with a size of 1 cm × 1 cm in the beaker, then transfer it to a heating stage and heat it at 110 °C for 3 h, take it out, clean it successively with acetone, absolute ethanol, and ultrapure water, and dry it with a nitrogen gun for standby; S12: Obtain single-layer graphene on a copper foil by chemical vapor deposition. Specifically, take a section of copper foil and soak it in 36% acetic acid for 10 - 15 min to remove the copper oxide on the surface, rinse it with ethanol and ultrapure water, and dry it for standby. Grow graphene on the surface of the copper foil by chemical vapor deposition; S13: Spin-coat PMMA on the single-layer graphene, and remove the excess graphene and glue on the back of the copper foil by oxygen plasma etching to obtain a copper foil-graphene-PMMA structure. Specifically, after cleaning the back of the copper foil by plasma etching, transfer it to a ferric chloride solution and let it stand for 1 - 2 h. Paste the single-layer graphene onto a clean quartz wafer with transparent tape. Spin-coat methyl methacrylate (950 PMMA) on the single-layer graphene, spin-coat it at 4000 revolutions per minute for 40 s with a spin coater, and bake the glue at 180 °C on a heating stage for 2 min. Remove the excess PMMA and graphene on the back of the copper foil by oxygen plasma etching to obtain a copper foil-graphene-PMMA structure; S14: Fabricate a pattern on the copper foil-graphene-PMMA structure by ultraviolet exposure. Specifically, use an ultraviolet lithography machine to fabricate a pattern by ultraviolet exposure, and then use a thermal resistance evaporation coater to evaporate 8 nm of chromium and 50 nm of gold respectively, and form a pattern after removing the glue.

[0035] S2: Prepare graphene dot electrodes. The specific steps are as follows: S21: According to the pattern, etch a dotted line with a length of 150 nm and a width of 5 nm by electron beam exposure to obtain graphene dot electrodes. Specifically, spin-coat PMMA A5 950 photoresist on the silicon wafer according to the dotted line of the pattern. Perform electron beam exposure on the silicon wafer spin-coated with PMMA A5 950 photoresist. The graphene is exposed at the exposed part of the pattern, and the other parts are covered and protected by the photoresist. After development, a dotted line with a length of 150 nm and a width of 5 nm is formed between the graphene dot electrodes; S22: Obtain a graphene nano-gap point electrode array by subjecting the graphene dot electrode pair to oxygen plasma etching and electro-burning. Specifically, according to the dotted line between the electrode pairs, use a plasma etching machine to etch the silicon wafer to fabricate a graphene electrode. During the etching process, evaluate the preparation of the electrode pair by monitoring the magnitude and curve shape of the current between the electrode pairs. Generally, at a bias voltage of 1V, a microampere-level current and a linear volt-ampere characteristic curve indicate that the graphene is not disconnected. When the current magnitude gradually decreases with the increase of the etching time, it means that the holes on the graphene gradually expand, making the graphene conduction channel between the electrode pairs gradually narrow, and the electrode gap is about to form. When the current magnitude reaches a few nanoampere levels and the volt-ampere characteristic curve shows non-linearity, specifically manifested as having a certain turn-on voltage, it represents the formation of a graphene gap. The gap size can be evaluated by the magnitude of the tunneling current, and finally a triangular electrode pair with a gap size of about 5nm is obtained, obtaining a graphene nano-gap point electrode array. The graphene nano-gap point electrode array includes multiple pairs of paired graphene dot electrodes. In the subsequent steps, each pair of paired graphene dot electrodes is condensed with a fullerene Y3N@C 80 molecule amide to obtain a probabilistic bit device.

[0036] S3: Synthesize the fullerene Y3N@C 80 molecule. The specific steps are as follows: S31: Under a nitrogen atmosphere, use an ice bath to keep the three-necked flask at 0°C. Add 10 mmol of compound 1 and 30 mL of DCM, stir the system, and then slowly add 60 mmol of MnO2. Remove the ice bath and react at room temperature for 24 h. Then filter and wash with DCM. The crude product obtained by rotary evaporation of the filtrate is directly added to the three-necked flask. Under a nitrogen atmosphere, add 11 mmol of compound 2 and 20 mL of toluene, and heat at 100°C for 6 h. After the reaction is completed, filter to obtain the crude product, and further purify the obtained crude product by silica gel column chromatography to obtain compound 3. 1 H NMR (500 MHz, CDCl3) δ 8.11 (s, 2H), 8.10 (d, J = 10.8 Hz, 2H), 7.63(dd, J = 8.6, 2.2 Hz, 2H). 13 C NMR (125 MHz, CDCl3) δ 148.83, 143.53, 138.99,133.19, 128.84, 123.93, 123.00,81.87, 74.03, 48.08. (TOF-ESI+) (m / z)C 93 H6Br2NY31563.60; S32: Under a nitrogen atmosphere, add 5 mmol of compound 3, 10 mmol of compound 4, 10 mmol of K2CO3, and 0.2 mmol of Pd(PPh3)4 to a two-necked flask; add a 110 ml mixture of toluene and water with a volume ratio of 5:1 to the two-necked flask through a syringe, heat to 110 °C, and reflux for 30 h; after cooling to room temperature, pour the reaction mixture into water, and extract three times with 50 ml of dichloromethane. Dry the organic layer with anhydrous sodium sulfate and remove the solvent; purify the obtained crude product by silica gel column chromatography to obtain compound 5. 1 H NMR (500 MHz, CDCl3) δ 8.26 (d, J J = 8.3 Hz, 2H), 8.08 (d, J J = 2.0 Hz, 2H),7.68 (dd, J J = 8.3, 2.0 Hz, 2H), 7.60 – 7.53 (m, 4H), 7.26 – 7.20 (m, 4H), 5.21(t, J J = 4.9 Hz, 2H), 3.18 (td, J J = 5.7, 4.9 Hz, 4H), 2.66 (tt, J J = 7.7, 1.0 Hz,4H), 1.80 (tt, J J = 7.9, 5.6 Hz, 4H). 13 C NMR (125 MHz, CDCl3) δ 156.50, 151.39,143.84, 142.44, 141.91, 138.21, 137.67, 129.52, 129.42, 127.79, 127.73,124.01, 81.87, 79.55, 74.03, 48.08, 40.22, 33.59, 29.66, 28.30. (TOF-ESI+)(m / z) C 121 H 46 N3O4Y31872.43; S33: Under a nitrogen atmosphere, add 5 mmol of compound 5 and 20 mL of a 50% TFA DCM solution to a two-necked flask, stir at room temperature for 2 h; after the reaction is complete, add saturated sodium bicarbonate solution, extract, and wash repeatedly until neutral. Rotate the collected organic layer to remove the solvent to obtain fullerene Y3N@C 80 molecule. 1 H NMR (500 MHz, CDCl3) δ 8.26 (d, J= 8.3 Hz, 2H), 8.08 (d, J = 2.0 Hz, 2H), 7.68 (dd, J = 8.3, 2.0 Hz, 2H), 7.60 – 7.53 (m, 4H), 7.26 – 7.20 (m, 4H), 2.77 (tt, J = 6.3, 5.4 Hz, 4H), 2.65 (tt, J = 7.6, 1.0 Hz, 4H), 1.76 (tt, J = 7.5, 5.3 Hz, 4H), 1.59 (d, J = 12.6 Hz, 2H). 13 13C NMR (125 MHz, CDCl3) δ 151.39, 143.84, 141.94, 141.91, 138.21, 137.67, 129.52, 129.38, 127.79, 127.73, 124.01, 81.87, 74.03, 48.08, 41.70, 33.92, 33.06. (TOF-ESI+) (m / z) C 111 H 30 N3Y31672.19。

[0037] Fullerene Y3N@C 80 The synthesis process of the molecule is as follows: 。

[0038] S4: Fullerene Y3N@C 80 The molecule reacts with the graphene dot electrode by amide condensation to prepare a probabilistic bit device based on Fullerene Y3N@C 80 The specific steps are as follows: S41: Place the Fullerene Y3N@C 80 molecule in a two-necked flask, inject 5 - 6 ml of dichloromethane and 0.5 - 0.7 ml of trifluoroacetic acid into the two-necked flask, react for more than 2 h under a nitrogen atmosphere, remove trifluoroacetic acid by extraction with sodium hydroxide, and transfer the remaining solution to a pear-shaped flask. Place the remaining solution under a nitrogen atmosphere through a gas exchange operation, and use a syringe to draw 10 ml of anhydrous pyridine and inject it into the pear-shaped flask to dissolve the Fullerene Y3N@C 80 molecule. In this example, 5 ml of dichloromethane and 0.5 ml of trifluoroacetic acid were used; S42: Place the graphene dot electrode in a two-necked flask, add a sufficient amount of 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and dissolve the Fullerene Y3N@C80 A pyridine solution of the molecule is reacted for more than 48 h in a nitrogen atmosphere to obtain a probability bit device based on fullerene Y3N@C 80 .

[0039] In this embodiment, 169 probability bit devices based on fullerene Y3N@C 80 are prepared at one time. Each probability bit device based on fullerene Y3N@C 80 is prepared by amide condensation of a single fullerene Y3N@C 80 molecule with two paired graphene dot electrodes.

[0040] Figure 2 is a schematic diagram of the random flipping generated by the functional molecule of the probability bit device based on fullerene Y3N@C 80 provided by the present invention under the drive of an electric field. This figure explains the reason for the generation of the high / low conductance states of the probability bit device based on fullerene Y3N@C 80 under the application of a transverse source-drain bias voltage, that is, under the application of a transverse source-drain bias voltage to the probability bit device, charge transfer of excess electrons first occurs between the encapsulated fullerene Y3N and the C 80 cage, and the charge becomes conductive delocalized charge. The delocalized charge on the carbon cage of these encapsulated fullerenes generates a stable electric dipole moment with the central point. The vibration inherent in the fullerene molecule will couple with the dipole. Under the application of different transverse source-drain bias voltages, the dipoles between the encapsulated fullerene Y3N and the C 80 cage will generate driving flips, and the two flip states exhibit different conductances.

[0041] Figure 3 is the I-t characteristic curve of the probability bit device based on fullerene Y3N@C 80 provided by the present invention under the application of different transverse source-drain bias voltages. Specifically, the probability bit device based on fullerene Y3N@C 80 is placed in a physical property measurement system (PPMS). First, the system is cooled to 97 K, and then transverse source-drain bias voltages of 0.11 V, 0.13 V, 0.15 V, 0.17 V, 0.19 V, 0.21 V, 0.23 V, 0.25 V, and 0.27 V are sequentially applied to the probability bit device based on fullerene Y3N@C 80 . The change of the current signal with time at each voltage is recorded, that is, the I-t characteristic curve is obtained. By Figure 3, it can be first observed from the I-t characteristic curve that within a time range of 120 s, the high / low conductance states of the probabilistic bit device clearly appear, and with the change of the lateral source-drain bias voltage, the proportion of the conductance states is significantly different. The high conductance state is defined as "1" and the low conductance state is defined as "0". The probabilistic bit device exhibits binary high (1) and low (0) conductance states that fluctuate with time, and the fluctuation probability can be adjusted by external stimuli (lateral source-drain bias voltage).

[0042] Figure 4 For the probabilistic bit device based on fullerene Y3N@C provided by the present invention 80 fitting graph of the lateral source-drain bias voltage of the probabilistic bit device and the probabilistic bit, Figure 4 derived from further processing of the data in Figure 3 , specifically, Figure 4 is an image obtained by fitting the full-scale probability (0 to 1) as a function of the input voltage measured at 97 K with the basic sigmoid function. The data collected at each lateral source-drain bias voltage during the test are screened and classified. The amount of data in the low conductance state is divided by the total amount of all the collected data to define the probabilistic bit p. It is calculated that when the lateral source-drain bias voltage is 0.11 V, p = 21.70%; when it is 0.13 V, p = 27.88%; when it is 0.15 V, p = 29.65%; when it is 0.17 V, p = 38.86%; when it is 0.19 V, p = 50.60%; when it is 0.21 V, p = 59.73%; when it is 0.23 V, p = 82.02%; when it is 0.25 V, p = 85.05%; when it is 0.27 V, p = 91.46%. The obtained probabilistic bits are plotted as a function curve of the input voltage and fitted with the basic sigmoid function of the random neuron in probability calculation. The probabilistic bit device shows that when the input lateral source-drain bias voltage increases from 0.11 V to 0.27 V, the probability of the low conductance state "0" appearing can be approximately tuned from 0 to 1.

[0043] The present invention utilizes the charge transfer of the Y3N molecule embedded in the fullerene Y3N@C 80 molecule, the electric field-driven dipole moment flipping, and the coupling effect between the molecular orbit and the electric dipole moment to achieve adjustable probabilistic characteristics and construct a nanoscale probabilistic bit device. The probabilistic bit device forms an amide covalent bond connection through the amino group at the bottom of the fullerene Y3N@C 80 molecule and the carboxyl group at the end of the graphene dot electrode, enhancing the chemical stability and long-term reliability of the device. The probabilistic bit device exhibits binary high (1) and low (0) conductance states that spontaneously fluctuate with time, and the fluctuation probability can be non-linearly adjusted by external stimuli to achieve efficient calculation. The present invention provides a new research direction and idea for the application of electro-control technology and molecular devices in the field of quantum information.

[0044] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not intended to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those of ordinary skill in the art should understand that they can still modify the technical solutions described in the foregoing embodiments, or perform equivalent replacements for some of the technical features; and these modifications or replacements do not cause the essence of the corresponding technical solutions to deviate from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A probability bit device based on fullerene Y3N@C 80 , characterized in that Including: Fullerene Y3N@C 80 A molecule, graphene dot electrodes, metal electrodes, and a substrate, Fullerene Y3N@C 80 The molecule is connected to two graphene dot electrodes, the graphene dot electrodes are connected to the metal electrodes, and the graphene dot electrodes and the metal electrodes are located on the substrate, Fullerene Y3N@C 80 The molecule is covalently bonded to the graphene dot electrodes through amide bonds.

2. The probability bit device according to claim 1, based on fullerene Y3N@C 80 , characterized in that Two sets of graphene dot electrodes and metal electrodes serve as the source electrode and the drain electrode respectively. A lateral source-drain bias voltage is applied between the source electrode and the drain electrode to obtain a current signal with hopping states.

3. The probability bit device according to claim 2, based on fullerene Y3N@C 80 , characterized in that By applying different magnitudes of the lateral source-drain bias voltage, current signals with different probability bits are obtained.

4. The probability bit device according to claim 3, based on fullerene Y3N@C 80 , characterized in that When a lateral source-drain bias voltage of 0.11 - 0.27 V is applied, the probability bits of the obtained current signal are 21.70% - 91.46%.

5. A preparation method of a probability bit device based on fullerene Y3N@C 80 , characterized in that For preparing a probability bit device based on fullerene Y3N@C as described in any one of claims 1 to 4 80 , comprising the following steps: S1: Fabricate a graphene-PMMA structure, transfer the graphene-PMMA structure onto the surface of a silicon wafer and mark the pattern; S2: Prepare graphene dot electrodes; S3: Synthesize fullerene Y3N@C 80 molecule; S4: Fullerene Y3N@C 80 The molecule undergoes amide condensation with the graphene dot electrode to fabricate a probability bit device based on fullerene Y3N@C 80 ​ 6. The preparation method of a probability bit device based on fullerene Y3N@C 80 , characterized in that S3 includes the following steps: S31: Under a nitrogen atmosphere, keep the three-necked flask at 0 °C in an ice bath, add Compound 1 and dichloromethane, stir, and then slowly add MnO₂; remove the ice bath and react at room temperature for 24 h, filter and wash with dichloromethane, add the crude product obtained by rotary evaporation of the filtrate to the three-necked flask; under a nitrogen atmosphere, add Compound 2 and toluene, heat at 100 °C for 6 h; filter to obtain the crude product, and purify the crude product to obtain Compound 3; S32: Under a nitrogen atmosphere, add Compound 3, Compound 4, K₂CO₃ and tetrakis(triphenylphosphine)palladium to a two-necked flask; add a mixture of toluene and water, heat to 110 °C and reflux for 30 h; after cooling to room temperature, pour the reaction mixture into water, extract with dichloromethane, dry the organic layer with anhydrous sodium sulfate, remove the solvent, and purify to obtain Compound 5; S33: Under a nitrogen atmosphere, add a dichloromethane solution of compound 5 and 50% trifluoroacetic acid to a two-necked flask, stir at room temperature for 2 h; add saturated sodium bicarbonate solution, extract, and wash repeatedly until neutral. Rotate the collected organic layer to remove the solvent to obtain fullerene Y3N@C 80 molecule; 。 7. The preparation method of a probability bit device based on fullerene Y3N@C 80 as described in claim 5, characterized in that S4 includes the following steps: S41: Place fullerene Y3N@C 80 molecules in a nitrogen atmosphere, add anhydrous pyridine, and fullerene Y3N@C 80 molecules dissolve in anhydrous pyridine; S42: Add 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and a pyridine solution dissolving fullerene Y3N@C molecules to the graphene dot electrode, and react in a nitrogen atmosphere to obtain a probabilistic bit device based on fullerene Y3N@C. 80 80 ​ 8. The preparation method of a probability bit device based on fullerene Y3N@C as claimed in claim 7, characterized in that, 80 In S41, Fullerene Y3N@C 80 molecules are placed in a two-necked flask, dichloromethane and trifluoroacetic acid are injected, and the reaction is carried out for more than 2 h under a nitrogen atmosphere. The trifluoroacetic acid is removed by extraction, and the remaining solution is transferred to a round-bottomed flask. The remaining solution is placed under a nitrogen atmosphere by changing the gas, and anhydrous pyridine is injected into the round-bottomed flask to dissolve the Fullerene Y3N@C 80 molecules. ​ 9. The preparation method of a probability bit device based on fullerene Y3N@C as described in claim 5, characterized in that, 80 In S4, multiple probability bit devices based on fullerene Y3N@C are prepared at one time. 80 Each probability bit device based on fullerene Y3N@C 80 is prepared by amide condensation of a single fullerene Y3N@C 80 molecule with a pair of two graphene dot electrodes.

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