Based on fullerene Y3N@C 80 Probability bit device and preparation method thereof

By assembling fullerene Y3N@C80 molecules between graphene electrodes, a single-molecule probabilistic bit device based on charge transfer and molecular vibration was constructed, which solved the problem of insufficient randomness in the state of traditional devices and realized an efficient and adjustable nanoscale probabilistic bit device with good randomness and chemical stability.

CN120302870BActive Publication Date: 2025-09-05NANKAI UNIV
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Patent Information

Application Number
CN202510750376.2
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2025-06-06
Publication Date
2025-09-05
Estimated Expiration
2045-06-06

AI Technical Summary

Technical Problem

In the existing technology, the state of computing units based on traditional metal oxide transistors is not random enough, making it difficult to achieve stable and controllable probabilistic bit devices. Graphene-based single-molecule devices have limitations in the construction of nanoscale probabilistic bit devices.

Method used

Fullerene Y3N@C80 molecules are used as functional molecules and assembled between graphene electrodes through a chemical decoupling method to form a single-molecule probabilistic bit device. The dipole moment generated by charge transfer and molecular vibration is used to drive the device to flip under a lateral source-drain bias, thereby realizing the regulation of the conductivity state.

Benefits of technology

The randomness and adjustability of single-molecule probabilistic bit devices are realized, showing a binary conductance state that fluctuates spontaneously over time. The fluctuation probability can be adjusted by external stimulation, which enhances the chemical stability and integration of the device and supports efficient computing.

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Abstract

The present invention relates to the technical field of quantum information devices, and specifically discloses a quantum information device based on fullerene Y3N@C 80 A probability bit device and a preparation method thereof, wherein the probability bit device comprises: fullerene Y3N@C 80 Molecules, graphene dot electrodes, metal electrodes and substrates, fullerene Y3N@C 80 The molecules are connected to two graphene point electrodes, which are connected to metal electrodes. The graphene point electrodes and metal electrodes are located on the substrate. Fullerene Y3N@C 80 The molecule is connected to the graphene point electrode via an amide covalent bond. The present invention drives the electric dipole moment flipping under different lateral source-drain biases applied to the probabilistic bit device, allowing the device to exhibit different conductance states. The time spent in each conductance state can be adjusted by the applied lateral source-drain bias, achieving the purpose of controlling the single-molecule probabilistic bit device.
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Description

Technical Field

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

[0002] Exploring stochastic dynamics in nanomaterials is of great significance in the emerging field of probabilistic computing, a new paradigm that transcends the traditional von Neumann architecture and aims to address problems such as combinatorial optimization, reversible logic, and Bayesian reasoning. A key component of probabilistic computing is the probability bit (p-bit), a classical entity that can generate random "0" and "1" values ​​with controllable probability. For example, Chinese invention patent application publication number CN117135995A discloses a dual-pulse controlled spin-orbit moment probability bit and control method. Under the simultaneous application of a first pulse current and a second pulse current, the first pulse current flows through the spin-orbit coupling layer to induce the magnetization of the magnetic free layer. The second pulse current flows sequentially through the top electrode layer, magnetic reference layer, spacer layer, magnetic free layer, and 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 stable in different magnetization states. Another example is Chinese invention patent application publication number CN118102851A, which discloses a logic device including a probability bit based on spin-orbit moment-induced magnetization reversal, a preparation method, and its application. The device comprises a substrate; a spin current generating layer, located on the substrate, configured to generate a spin current by generating a spin-orbit coupling effect under the action of an electric current, and to generate heat energy under the action of the electric current; a functional layer, located on the spin current generating layer, configured to transfer the spin current and heat energy; and a magnetic layer, located on the functional layer. The spin current injected into the magnetic layer generates a spin-orbit moment in the magnetic layer, causing the magnetic layer to undergo a magnetization flip under the induction of the spin-orbit moment and the heat energy. The state of conventional computing units based on conventional metal oxide transistors is 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 in time, and the fluctuation probability can be tuned by external stimuli.

[0004] Graphene-based single-molecule devices are an important approach for constructing stable single-molecule nanodevices. Graphene-based single-molecule devices utilize graphene's stability and high electron mobility, and by preparing graphene into electrodes, they enable the construction of stable and controllable single-molecule-level electronic devices. Currently, graphene-based single-molecule devices have successfully constructed a variety of molecular electronic devices, including field-effect transistors, switches, rectifiers, memristors, and light-emitting diodes. These devices not only show broad application prospects in terms of chip miniaturization, integration, and multifunctionality, but their unique physical and chemical properties also bring new opportunities to the field of quantum information technology. Based on existing technical backgrounds, selecting chemical molecules with certain characteristics to construct nanoscale molecular electronic devices has made it possible to use nanoscale probabilistic bit devices as 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 fullerene Y3N@C 80 A probability bit device and a preparation method thereof are provided by embedding fullerene Y3N@C 80 The molecules are assembled between nano-gap graphene electrodes by chemical decoupling to form a single-molecule probabilistic bit device. In the single-molecule probabilistic bit device, the fullerene Y3N@C 80 First, the molecules undergo charge transfer to form delocalized charges, and then the delocalized charges and the center point generate a stable electric dipole moment. Combined with the vibration of the fullerene molecule itself, the coupling between the molecular orbital and the dipole is generated, and the electric dipole moment is driven to flip when different lateral source-drain biases are applied to the device, making the fullerene Y3N@C 80 Molecular devices can exhibit different conductance states, and the time proportion of the conductance state can be adjusted by the magnitude of the applied lateral source-drain bias, thereby achieving the purpose of regulating single-molecule probabilistic bit devices.

[0006] The present invention provides a fullerene Y3N@C 80 The probability bit device adopts the following technical solutions: including: fullerene Y3N@C 80 Molecules, graphene dot electrodes, metal electrodes and substrates, fullerene Y3N@C 80 The molecules are connected to two graphene point electrodes, which are connected to metal electrodes. The graphene point electrodes and metal electrodes are located on the substrate. Fullerene Y3N@C 80 The molecules are connected to the graphene dot electrodes via amide covalent bonds.

[0007] Furthermore, two groups of graphene point electrodes and metal electrodes are used as source electrodes and drain electrodes respectively, and a lateral source-drain bias is applied to the source electrodes and the drain electrodes to obtain a current signal with a jumping state.

[0008] Furthermore, different lateral source-drain bias voltages are applied to obtain current signals with different probability bits.

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

[0010] The present invention also provides a fullerene Y3N@C 80 The preparation method of the probability bit device is used to prepare the above-mentioned fullerene Y3N@C 80 The probabilistic bit device adopts the following technical solution: comprising the following steps:

[0011] S1: Fabricate a graphene-PMMA structure, transfer the graphene-PMMA structure to the silicon wafer surface and mark the pattern;

[0012] S2: Preparation of graphene dot electrodes;

[0013] S3: Synthesis of fullerene Y3N@C 80 molecular;

[0014] S4: Fullerene Y3N@C 80 The molecules were condensed with graphene dot electrodes to prepare fullerene-based Y3N@C 80 probability bit device.

[0015] Furthermore, S3 includes the following steps:

[0016] S31: Under a nitrogen atmosphere, place the 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 hours, filter, and wash with dichloromethane; the crude product obtained by rotary evaporation of the filtrate is added to the flask; under a nitrogen atmosphere, add compound 2 and toluene, and heat at 100°C for 6 hours; filter to obtain the crude product, which is purified to obtain compound 3;

[0017] S32: Under a nitrogen atmosphere, compound 3, compound 4, K2CO3, and tetrakis(triphenylphosphine)palladium (Pd(PPh3)4) were added to a two-necked flask; a mixture of toluene and water was added, the mixture was heated to 110°C, and refluxed for 30 h; after cooling to room temperature, the reaction mixture was poured into water and extracted with dichloromethane. The organic layer was dried over anhydrous sodium sulfate, the solvent was removed, and the mixture was purified to obtain compound 5;

[0018] S33: Under nitrogen atmosphere, compound 5 and 50% trifluoroacetic acid (TFA) in dichloromethane were added to a two-necked flask and stirred at room temperature for 2 h. Saturated sodium bicarbonate solution was added, extracted, and washed repeatedly until neutral. The collected organic layer was evaporated to remove the solvent to obtain fullerene Y3N@C 80 molecular;

[0019] .

[0020] Furthermore, S4 includes the following steps:

[0021] S41: Making fullerene Y3N@C 80 The molecule is in a nitrogen atmosphere, anhydrous pyridine is added, and the fullerene Y3N@C 80 The molecule dissolves in anhydrous pyridine;

[0022] S42: Add 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and dissolved fullerene Y3N@C to the graphene dot electrode. 80 The pyridine solution of the molecule was reacted in a nitrogen atmosphere for more than 48 hours to obtain fullerene Y3N@C 80 probability bit device.

[0023] Furthermore, in S41, fullerene Y3N@C 80 The molecule was placed in a two-necked flask, and dichloromethane and trifluoroacetic acid were injected. The reaction was continued for more than 2 hours under a nitrogen atmosphere. The trifluoroacetic acid was removed by extraction with sodium hydroxide, and the remaining solution was transferred to an eggplant-shaped flask. The remaining solution was ventilated in a nitrogen atmosphere, and anhydrous pyridine was injected into the eggplant-shaped flask to dissolve the fullerene Y3N@C 80 molecular.

[0024] Furthermore, in S4, multiple fullerene-based Y3N@C 80 The probability bit device, each based on fullerene Y3N@C 80 The probability bit device is realized by a single fullerene Y3N@C 80 The molecule is prepared by amide condensation with two paired graphene dot electrodes.

[0025] The above one or more technical solutions in the embodiments of the present invention have at least one of the following technical effects:

[0026] 1. The present invention uses fullerene Y3N@C 80 The molecules were used as functional molecules to prepare fullerene-based Y3N@C 80 Single-molecule probabilistic bit device. Fullerene Y3N@C 80 C in the intramolecular fullerene 80 The delocalized charges generated by charge transfer on the cage generate a stable electric dipole moment with the central point. Under different lateral source-drain biases, the embedded fullerene Y3N and C 80The dipoles between the cages flip under the coupling of molecular vibrations, producing two different flipped states. This ensures that the device's conductivity can be adjusted by applying different lateral source-drain biases. Secondly, the coupling between the molecular orbitals and the electric dipole moment generated by the stretching vibrations of the fullerene molecules themselves ensures dynamic switching within a certain time frame, which can be monitored by collecting changes in the current signal: the generation of random high / low conductance state jumps. This probabilistic bit device has a strong randomness or uncertainty characteristic, and the molecular state can be read through conductivity, realizing probabilistic bits at the single-molecule scale.

[0027] 2. The present invention is based on fullerene Y3N@C 80 The probabilistic bit device exhibits binary high (1) and low (0) conductance states that fluctuate spontaneously over time, and the fluctuation probability can be fine-tuned by external stimulation, thereby achieving efficient computation. The proportion of high / low conductance states to the total amount of data under each test condition can be expanded to a probabilistic state, which exhibits continuously tunable characteristics, broadening the research direction for realizing computational nanodevices with adjustable probabilities and high operational stability.

[0028] 3. Fullerene Y3N@C of the present invention 80 The preparation method of the probability bit device forms an amide covalent bond through the amino group –NH2 at the bottom of the molecule and the carboxyl group –COOH at the end of the graphene point electrode, which significantly enhances the chemical stability of the device and ensures the long-term reliability of the single-molecule probability bit device under complex operating conditions.

[0029] 4. Fullerene Y3N@C of the present invention 80 The preparation method of the probability bit device can design the electrode position and hole position by itself through the in-situ drawing of the external electrode and the electron beam exposure etching process. It has strong integrated design at the nanoscale. By designing a row of equidistant dotted lines between an electrode pair, 169 pairs of graphene array electrodes can be obtained, and finally combined with the fullerene Y3N@C 80 By connecting molecules, they fabricated 169 single-molecule probability bit devices, achieving significant miniaturization of the device size and demonstrating extremely high integration. This feature provides new ideas for the miniaturization and high-density integration of functional chips, laying a technological foundation for the future development of micro-nano optoelectronics.

[0030] Additional aspects and advantages of the present invention will be set forth in part in the description which follows and, in part, will be obvious from the description which follows, or may be learned by practice of the present invention. BRIEF DESCRIPTION OF THE DRAWINGS

[0031] In order to more clearly illustrate the technical solutions in the present invention or the prior art, the following briefly introduces the drawings required for use in the embodiments or the description of the prior art. Obviously, the drawings described below are some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without paying any creative work.

[0032] Figure 1 It is a schematic structural block diagram of the probabilistic bit device provided by the present invention.

[0033] Figure 2 This is a schematic diagram of the random flipping of molecules in the probabilistic bit device provided by the present invention when driven by an electric field.

[0034] Figure 3 It is a graph of the It characteristic of the probabilistic bit device provided by the present invention when different lateral source-drain bias voltages are applied.

[0035] Figure 4 It is a fitting diagram of the lateral source-drain bias and the probability bit of the probability bit device provided by the present invention.

[0036] Description of reference numerals:

[0037] 1. Graphene dot electrode; 2. Metal electrode; 3. Substrate; 4. Fullerene Y3N@C 80 molecular. DETAILED DESCRIPTION

[0038] To make the purpose, technical solutions and advantages of the present invention clearer, the technical solutions of the present invention will be clearly and completely described below in conjunction with the accompanying drawings of the present invention. Obviously, the embodiments described are part of the embodiments of the present invention, rather than all the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative work are within the scope of protection of the present invention. The following embodiments are used to illustrate the present invention, but are not used to limit the scope of the present invention.

[0039] In the description of this specification, the description with reference to the terms "one embodiment", "some embodiments", "example", "specific example", or "some examples" means that the specific features, structures or characteristics described in conjunction with the embodiment or example are included in at least one embodiment or example of the embodiment of the present invention. In this specification, the schematic representation of the above terms does 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, those skilled in the art can combine and combine different embodiments or examples described in this specification and features of different embodiments or examples without contradiction.

[0040] The following combination Figures 1 to 4 The present invention is further described in detail, and a method based on fullerene Y3N@C 80 Probability bit device and preparation method thereof:

[0041] In this embodiment, Figure 1 As shown, a fullerene-based Y3N@C 80 Probabilistic bit devices, including: fullerene Y3N@C 80 Molecule 4, graphene dot electrode 1, metal electrode 2, and substrate 3. Fullerene Y3N@C 80 The molecules are connected to two graphene point electrodes, which are connected to metal electrodes. The graphene point electrodes and metal electrodes are located on the substrate. Fullerene Y3N@C 80 The molecules are connected to the graphene dot electrodes via amide covalent bonds. In this embodiment, the metal electrodes are gold electrodes and the substrate is a silicon substrate.

[0042] Fullerene Y3N@C 80 The graphene dot electrodes and metal electrodes on both sides of the molecule constitute the source electrode and the drain electrode respectively. That is, the two groups of graphene dot electrodes and metal electrodes serve as the source electrode and the drain electrode respectively.

[0043] Based on fullerene Y3N@C 80 The probability bit device has the following characteristics:

[0044] (1) In the embedded fullerene Y3N@C 80 There are extra electrons on the embedded Y3N molecules in the molecule, which serve as the charge source for forming delocalized charges. 80 When the excess electrons between cages are transferred, the charge is transferred from the embedded part to the carbon cage and becomes a delocalized charge that conducts electricity.

[0045] (2) C embedded in fullerene 80 The delocalized charge on the cage and the center point generate a stable electric dipole moment, and the stretching vibration of the fullerene molecule itself generates a coupling effect between the molecular orbital and the electric dipole moment. Under different lateral source-drain biases, the embedded fullerene Y3N and C 80 The dipoles between the cages generate the driven flip.

[0046] (3) By applying a lateral source-drain bias to the source and drain electrodes of the probabilistic bit device, a current signal with a hopping state is obtained, from which an It characteristic curve with a hopping state can be plotted. By changing the magnitude of the source-drain bias, It characteristic curves with different hopping states can be obtained. The proportion of high / low conductance states in each It characteristic curve shows a characteristic that varies with the source-drain bias.

[0047] (4) The proportion of high / low conductance states to the total amount of data under each test condition can be expanded into a probabilistic state, which exhibits a continuously tunable characteristic. The amount of data in the low conductance state divided by the total amount of all collected data is defined as a probability bit. Applying different lateral source-drain bias voltages, current signals with different probability bits are obtained. Through experiments, applying lateral source-drain bias voltages of 0.11 to 0.27 V, the probability bits of the current signals obtained are 21.70% to 91.46%.

[0048] In this embodiment, a fullerene-based Y3N@C 80 The preparation method of the probability bit device is used to prepare the above-mentioned fullerene Y3N@C 80 The probabilistic bit device adopts the following technical solution: comprising the following steps:

[0049] S1: Prepare a graphene-PMMA structure, transfer the graphene-PMMA structure to the silicon wafer surface and mark the pattern. The specific steps are as follows:

[0050] S11: Soak and clean the silicon wafer (silicon substrate) in a 110°C piranha solution for 3 hours, then ultrasonically clean it with acetone, anhydrous ethanol, and ultrapure water, and blow it dry with nitrogen for later use. Specifically, prepare a mixed piranha solution of concentrated sulfuric acid and hydrogen peroxide in a volume ratio of 3:7 in a beaker. Place the cut silicon wafer of size 1cm×1cm in the beaker, then transfer it to a heating table and heat it at 110°C for 3 hours. After taking it out, wash it with acetone, anhydrous ethanol, and ultrapure water in sequence, and blow it dry with a nitrogen gun for later use;

[0051] S12: Produce a single layer of graphene on copper foil using chemical vapor deposition. Specifically, take a section of copper foil and soak it in 36% acetic acid for 10-15 minutes to remove surface copper oxide. Rinse it with ethanol and ultrapure water, and dry it. Grow graphene on the copper foil surface using chemical vapor deposition.

[0052] S13: Spin-coat PMMA on the monolayer graphene, and remove excess graphene and glue on the back of the copper foil by oxygen plasma etching to obtain a copper foil-graphene-PMMA structure. Specifically, the back of the copper foil is cleaned by plasma etching and then transferred to a ferric chloride solution. Let it stand for 1 to 2 hours, and the monolayer graphene is attached to a clean quartz wafer with transparent tape. Methyl methacrylate (950 PMMA) is spin-coated on the monolayer graphene. The coating is performed at 4000 rpm for 40 seconds using a glue spreader, and the glue is baked on a heating plate at 180°C for 2 minutes. Excess PMMA and graphene on the back of the copper foil are etched by oxygen plasma to obtain a copper foil-graphene-PMMA structure.

[0053] S14: Patterning the copper foil-graphene-PMMA structure by ultraviolet exposure. Specifically, a UV lithography machine is used to pattern the structure by ultraviolet exposure, and then a thermal resistance evaporation coating apparatus is used to evaporate 8 nm of chromium and 50 nm of gold, respectively, and the pattern is formed after removing the adhesive.

[0054] S2: Prepare graphene dot electrodes. The specific steps are as follows:

[0055] S21: Etching a dotted line with a length of 150 nm and a width of 5 nm according to the pattern by electron beam exposure to obtain a graphene dot electrode. Specifically, PMMA A5 950 photoresist is spin-coated on a silicon wafer according to the dotted line of the pattern, and the silicon wafer with the PMMA A5 950 photoresist is subjected to electron beam exposure. The graphene is exposed in the pattern-exposed area, 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 electrode pairs;

[0056] S22: The graphene point electrode pairs are subjected to oxygen plasma etching and electrical burnout to obtain a graphene nanogap point electrode array. Specifically, a plasma etcher is used to etch the silicon wafer along the dashed lines between the electrode pairs to produce the graphene electrodes. During the etching process, the electrode pair preparation is assessed by monitoring the magnitude and shape of the current between the electrode pairs. Typically, under a 1V bias, a microampere current and a linear volt-ampere characteristic curve indicate that the graphene is intact. When the current magnitude gradually decreases with etching time, it indicates that the pores in the graphene are gradually expanding, causing the graphene conductive channel between the electrode pairs to gradually narrow, and an electrode gap is about to form. When the current magnitude reaches a few nanoamperes and the volt-ampere characteristic curve exhibits nonlinearity, specifically exhibiting a certain turn-on voltage, it indicates that a graphene gap has formed. The gap size can be assessed by the tunneling current. Ultimately, triangular electrode pairs with a gap size of approximately 5nm are obtained, resulting in a graphene nanogap point electrode array. The graphene nanogap point electrode array comprises multiple pairs of graphene point electrodes. In the subsequent steps, each pair of graphene dot electrodes is connected to a fullerene Y3N@C 80 A probabilistic bit device was fabricated by molecular amide condensation.

[0057] S3: Synthesis of fullerene Y3N@C 80 The specific steps are as follows:

[0058] S31: Under a nitrogen atmosphere, place the flask at 0°C in an ice bath. Add 10 mmol of compound 1 and 30 mL of DCM, stir, and then slowly add 60 mmol of MnO2. Remove the ice bath and allow the mixture to react at room temperature for 24 h. The mixture is then filtered and washed with DCM. The filtrate is rotary evaporated to obtain a crude product, which is then added directly to the 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, filter to obtain the crude product, which is further purified 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;

[0059] S32: Under a nitrogen atmosphere, 5 mmol of compound 3, 10 mmol of compound 4, 10 mmol of K2CO3 and 0.2 mmol of Pd(PPh3)4 were added to a two-necked flask; 110 ml of a mixture of toluene and water in a volume ratio of 5:1 was added to the two-necked flask via a syringe, the mixture was heated to 110°C and refluxed for 30 h; after cooling to room temperature, the reaction mixture was poured into water and extracted three times with 50 ml of dichloromethane, the organic layer was dried over anhydrous sodium sulfate, and the solvent was removed; the crude product was purified by silica gel column chromatography to obtain compound 5. 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), 5.21(t, J = 4.9 Hz, 2H), 3.18 (td, J = 5.7, 4.9 Hz, 4H), 2.66 (tt, J = 7.7, 1.0 Hz,4H), 1.80 (tt,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;

[0060] S33: Under nitrogen atmosphere, 5 mmol of compound 5 and 20 mL of 50% TFA in DCM solution were added to a two-necked flask and stirred at room temperature for 2 h. After the reaction was complete, saturated sodium bicarbonate solution was added, extracted, and washed repeatedly until neutral. The collected organic layer was evaporated to remove the solvent to obtain fullerene Y3N@C 80 molecular. 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 CNMR (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 30N3Y31672.19.

[0061] Fullerene Y3N@C 80 The synthesis process of the molecule is:

[0062] .

[0063] S4: Fullerene Y3N@C 80 The molecules were condensed with graphene dot electrodes to prepare fullerene-based Y3N@C 80 The specific steps are as follows:

[0064] S41: Take fullerene Y3N@C 80 The molecule was placed in a two-necked flask, and 5-6 ml of dichloromethane and 0.5-0.7 ml of trifluoroacetic acid were injected into the two-necked flask. The reaction was continued for more than 2 hours under a nitrogen atmosphere. The trifluoroacetic acid was removed by extraction with sodium hydroxide, and the remaining solution was transferred to an eggplant-shaped flask. The remaining solution was ventilated under a nitrogen atmosphere, and 10 ml of anhydrous pyridine was drawn with a syringe and injected into the eggplant-shaped flask to dissolve the fullerene Y3N@C 80 In this example, 5 ml of dichloromethane and 0.5 ml of trifluoroacetic acid were used;

[0065] S42: Place the graphene point electrode in a two-necked flask, add sufficient 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and dissolved fullerene Y3N@C into the two-necked flask. 80 The pyridine solution of the molecule was reacted in a nitrogen atmosphere for more than 48 hours to obtain fullerene Y3N@C 80 probability bit device.

[0066] In this example, 169 fullerene-based Y3N@C 80 The probability bit device, each based on fullerene Y3N@C 80 The probability bit device is realized by a single fullerene Y3N@C 80 The molecule is prepared by amide condensation with two paired graphene dot electrodes.

[0067] Figure 2 The present invention provides a fullerene Y3N@C 80 Schematic diagram of the random flipping of the functional molecules of the probabilistic bit device under the driving of the electric field. This figure explains the random flipping of the functional molecules of the probabilistic bit device under the driving of the electric field. 80 The reason for the high / low conduction state of the probability bit device is that when a lateral source-drain bias is applied to the probability bit device, the embedded fullerene Y3N and C 80The excess electrons first transfer between the cages, and the charge becomes a conductive delocalized charge. The delocalized charges on the carbon cage embedded with fullerenes generate a stable electric dipole moment with the center point. The vibration of the fullerene molecule itself will couple with the dipoles. Under different lateral source-drain biases, the embedded fullerene Y3N and C 80 The dipoles between the cages produce a driven flip, and the two flipped states exhibit different conductances.

[0068] Figure 3 The present invention provides a fullerene Y3N@C 80 The It characteristic curve of the probability bit device under different lateral source-drain bias voltages is shown in FIG. 80 The probability bit device is placed in a comprehensive physical property measurement system (PPMS). The system is first cooled to 97K, and then the fullerene-based Y3N@C 80 The probability bit device is sequentially applied with lateral source-drain bias voltages of 0.11V, 0.13V, 0.15V, 0.17V, 0.19V, 0.21V, 0.23V, 0.25V, and 0.27V, and the change of the current signal over time at each voltage is recorded to obtain the It characteristic curve. Figure 3 From the It characteristic curve, it can be first observed that within a time range of 120s, the probabilistic bit device clearly exhibits high and low conductance states, and the proportion of conductance states varies significantly with changes in the lateral source-drain bias, with the high conductance state defined as "1" and the low conductance state defined as "0". The probabilistic bit device exhibits binary high (1) and low (0) conductance states that fluctuate over time, and the fluctuation probability can be adjusted by external stimulation (lateral source-drain bias).

[0069] Figure 4 The present invention provides a fullerene Y3N@C 80 The lateral source-drain bias and probability bit fitting diagram of the probability bit device, Figure 4 Depend on Figure 3 The data in the further processing results are as follows, specifically, Figure 4This is a plot of the full-scale probability (0 to 1) as a function of input voltage measured at 97K and fitted with a fundamental sigmoid function. The data collected at each lateral source-drain bias during the test were sorted and categorized. The probability bit, p, was defined as the amount of low-conductance data divided by the total amount of data collected. The calculated values ​​for a lateral source-drain bias of 0.11V were 21.70%, 0.13V, 0.15V, 29.65%, 0.17V, 38.86%, 0.19V, 50.60%, 0.21V, 59.73%, 0.23V, 82.02%, 0.25V, 85.05%, and 0.27V, respectively. The resulting probability bit was plotted as a function of input voltage and fitted with the fundamental sigmoid function for random neurons used in probability calculations. The probabilistic bit device shows that when the input lateral source-drain bias increases from 0.11V to 0.27V, the probability of the low-conductance state "0" appearing can be tuned approximately from 0 to 1.

[0070] The present invention utilizes fullerene Y3N@C 80 The charge transfer of embedded Y3N molecules, electric field driven dipole moment flipping and the coupling between molecular orbitals and electric dipole moments realize adjustable probability characteristics and construct nanoscale probability bit devices. 80 The amino group at the bottom of the molecule forms an amide covalent bond with 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 fluctuate spontaneously over time, and the fluctuation probability can be nonlinearly adjusted by external stimulation, achieving efficient computing. This invention provides new research directions and ideas for the application of electrical control technology and molecular devices in the field of quantum information.

[0071] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, rather than to limit it. Although the present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art should understand that they can still modify the technical solutions described in the aforementioned embodiments, or make equivalent replacements for some of the technical features therein. However, these modifications or replacements do not deviate the essence of the corresponding technical solutions from the spirit and scope of the technical solutions of the various embodiments of the present invention.

Claims

1. A fullerene-based Y3N@C 80 A probabilistic bit device, characterized in that include: Fullerene Y3N@C 80 Molecules, graphene dot electrodes, metal electrodes and substrates, fullerene Y3N@C 80 The molecules are connected to two graphene point electrodes, which are connected to metal electrodes. The graphene point electrodes and metal electrodes are located on the substrate. Fullerene Y3N@C 80 The molecules are connected to the graphene dot electrodes via amide covalent bonds; Fullerene Y3N@C 80 The specific structure of the molecule is: 。 2. A fullerene-based Y3N@C as claimed in claim 1 80 A probabilistic bit device, characterized in that Two groups of graphene point electrodes and metal electrodes are used as source electrodes and drain electrodes respectively. A lateral source-drain bias is applied to the source electrodes and the drain electrodes to obtain a current signal with a jumping state.

3. A fullerene-based Y3N@C as claimed in claim 2 80 A probabilistic bit device, characterized in that By applying lateral source-drain bias voltages of different magnitudes, current signals with different probability bits are obtained.

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

5. A fullerene-based Y3N@C 80 The method for preparing a probability bit device is characterized in that: For preparing the fullerene-based Y3N@C according to any one of claims 1 to 4 80 The probability bit device comprises the following steps: S1: Fabricate a graphene-PMMA structure, transfer the graphene-PMMA structure to the silicon wafer surface and mark the pattern; S2: Preparation of graphene dot electrodes; S3: Synthesis of fullerene Y3N@C 80 molecular; S4: Fullerene Y3N@C 80 The molecules were condensed with graphene dot electrodes to prepare fullerene-based Y3N@C 80 probability bit device.

6. A fullerene-based Y3N@C as claimed in claim 5 80 The method for preparing a probability bit device is characterized in that: S3 includes the following steps: S31: Under a nitrogen atmosphere, place the flask at 0°C in an ice bath, add compound 1 and dichloromethane, stir, and then slowly add MnO2; remove the ice bath, react at room temperature for 24 hours, filter and wash with dichloromethane, and add the crude product obtained by rotary evaporation of the filtrate to the flask; under a nitrogen atmosphere, add compound 2 and toluene, and heat at 100°C for 6 hours; filter to obtain the crude product, which is purified to obtain compound 3; S32: Under a nitrogen atmosphere, compound 3, compound 4, K2CO3, and tetrakis(triphenylphosphine)palladium were added to a two-necked flask; a mixture of toluene and water was added, and the mixture was heated to 110°C and refluxed for 30 h; after cooling to room temperature, the reaction mixture was poured into water and extracted with dichloromethane. The organic layer was dried over anhydrous sodium sulfate, the solvent was removed, and the mixture was purified to obtain compound 5; S33: Under nitrogen atmosphere, compound 5 and 50% trifluoroacetic acid in dichloromethane were added to a two-necked flask and stirred at room temperature for 2 h. Saturated sodium bicarbonate solution was added, extracted, and washed repeatedly until neutral. The collected organic layer was evaporated to remove the solvent to obtain fullerene Y3N@C 80 molecular; 。 7. A fullerene-based Y3N@C as claimed in claim 5 80 The method for preparing a probability bit device is characterized in that: S4 includes the following steps: S41: Making fullerene Y3N@C 80 The molecule is in a nitrogen atmosphere, anhydrous pyridine is added, and fullerene Y3N@C 80 The molecule dissolves in anhydrous pyridine; S42: Add 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and dissolved fullerene Y3N@C to the graphene dot electrode. 80 The pyridine solution of the molecule was reacted in a nitrogen atmosphere to obtain fullerene Y3N@C 80 probability bit device.

8. A fullerene-based Y3N@C as claimed in claim 7 80 The method for preparing a probability bit device is characterized in that: In S41, take fullerene Y3N@C 80 The molecule was placed in a two-necked flask, and dichloromethane and trifluoroacetic acid were injected. The reaction was continued for more than 2 hours under a nitrogen atmosphere. The trifluoroacetic acid was extracted and removed, and the remaining solution was transferred to an eggplant-shaped flask. The remaining solution was ventilated in a nitrogen atmosphere, and anhydrous pyridine was injected into the eggplant-shaped flask to dissolve the fullerene Y3N@C 80 molecular.

9. A fullerene-based Y3N@C as claimed in claim 5 80 The method for preparing a probability bit device is characterized in that: In S4, multiple fullerene-based Y3N@C 80 The probability bit device, each based on fullerene Y3N@C 80 The probability bit device is realized by a single fullerene Y3N@C 80 The molecule is prepared by amide condensation with two paired graphene dot electrodes.

Citation Information

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