CN112582542B - Monomolecular field effect transistor based on two-dimensional van der Waals heterostructure and preparation method thereof - Google Patents

Monomolecular field effect transistor based on two-dimensional van der Waals heterostructure and preparation method thereof Download PDF

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CN112582542B
CN112582542B CN202011410961.1A CN202011410961A CN112582542B CN 112582542 B CN112582542 B CN 112582542B CN 202011410961 A CN202011410961 A CN 202011410961A CN 112582542 B CN112582542 B CN 112582542B
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CN112582542A (en
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郭雪峰
李佩慧
贾传成
常新月
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Nankai University
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    • H10K10/46Field-effect transistors, e.g. organic thin-film transistors [OTFT]
    • H10K10/462Insulated gate field-effect transistors [IGFETs]
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    • H10K10/46Field-effect transistors, e.g. organic thin-film transistors [OTFT]
    • H10K10/462Insulated gate field-effect transistors [IGFETs]
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Abstract

A monomolecular field effect transistor based on a two-dimensional van der Waals heterostructure and a preparation method thereof belong to the field of new materials and molecular field effect transistors. The graphene-based two-dimensional gate electrode structure is composed of a conductive two-dimensional gate electrode layer, an insulating two-dimensional dielectric layer, a single-molecule heterojunction based on a graphene point electrode and a protective layer, and the preparation method comprises the steps of 1) two-dimensional lamination assembly; 2) the two-dimensional material as each component of the device has atomic-scale controllable flatness and thickness; 3) stability of van der waals heterostructures; 4) combination with graphene-based single molecule heterojunctions. The invention forms the Van der Waals heterostructure by assembling Van der Waals stacking of different two-dimensional materials. The dielectric layer and the grid of the device are enabled to be smooth at atomic level and the atomic layer is controllable, the accurate control preparation of the monomolecular field effect crystal device is realized, hexagonal boron nitride or gallium nitride is used as a protective layer to package the device, the interference of the external environment to the device is greatly reduced, and the stability of the device is improved.

Description

Monomolecular field effect transistor based on two-dimensional van der Waals heterostructure and preparation method thereof
Technical Field
The invention belongs to the field of new materials and molecular field effect transistors, and particularly relates to a van der Waals heterostructure monomolecular field effect transistor which takes a two-dimensional material as a grid electrode, a dielectric layer, a source electrode, a drain electrode and a protective layer.
Background
Transistors are the heart of electronic circuits in the conventional semiconductor industry and are the cornerstone of the contemporary digital revolution. Since the first model of transistors proposed in 1947, researchers have developed many forms of transistors, the basic principle of which is: by applying a suitable voltage to the gate, the carrier concentration at the interface of the insulating layer and the semiconductor layer can be changed due to the capacitance effect of the dielectric layer, so that the current between the source and drain electrodes can be regulated. Thus, on the one hand, the logic function of the switch can be realized; on the other hand, since the output power is higher than the input power, the transistor has a function of an amplifier. With the rapid development of the information age, the requirements for miniaturization and integration of electronic components become increasingly significant, and molecular-atomic-level transistors are urgently needed to solve the problem, so that unimolecular electronics is developed. Different from the traditional field effect transistor, the monomolecular field effect transistor has a molecular size, and the energy level position of molecules can be regulated by applying gate voltage in a monomolecular heterojunction, so that the relative position of the molecular energy level and the Fermi level of a graphene electrode is changed, the conduction characteristic of the molecules can be regulated on one hand, and the vibration mode, the excited state and some information related to vibration of the molecules can be obtained on the other hand.
At present, the most mature system in the control strategy of the monomolecular field effect transistor is based on the electrostatic field generated by the traditional solid-state grid. The principle is that the energy level of molecules is regulated and controlled through an electric field generated by a solid grid, and then the conductive property of the molecules is changed. However, there are two main problems with this regulation: on the one hand, the control efficiency is low, and the dielectric layer is sensitive to the thickness of the dielectric layer, especially the current dielectric layer is mostly made of silicon dioxide material, and it is very difficult to prepare a solid dielectric layer with the thickness matched with the molecular size in process implementation. On the other hand, most of the materials used by the traditional grid electrode are doped silicon, and the traditional grid electrode is not easy to be made to be extremely small, so that grid voltage cannot be accurately applied to a single molecular heterojunction in the aspect of device integration, and the influence of leakage current on the device is large.
In recent years, the rise of two-dimensional materials has provided new solutions for the optimization of the stability and integration of single-molecule field effect transistors. Two-dimensional materials are very diverse, and there are materials ranging from metallic to insulating. There are hundreds of two-dimensional materials known today, many of which are natural semiconductors, metals, and insulators. Two-dimensional materials are characterized by a layered crystal structure with strong in-plane covalent bonds, with no surface dangling bonds, and thus exhibit excellent electronic and optical properties even at the limits of monoatomic thickness, in sharp contrast to dangling bonds and trapped states present on the surface and interface of typical bulk semiconductors. Meanwhile, van der waals heterostructures formed by coupling together two-dimensional material layers through weak van der waals forces (vdW) can maintain flatness at an atomic level and close contact between layers. Assembling different two-dimensional materials can form van der Waals heterostructures with abundant types. Plays an important role in improving the stability of the device. Hexagonal boron nitride (h-BN), gallium nitride (Ga) 2 N 3 ) Etc. are as twoThe insulator in the fiber material has large band gap, physical inertia and chemical inertia, and is difficult to react with other substances, so the fiber material is also a good protective material.
Disclosure of Invention
The invention aims to provide a monomolecular field effect transistor based on a two-dimensional van der Waals heterostructure and a preparation method thereof, wherein a stable two-dimensional material is introduced into a device for lamination to form the van der Waals heterostructure, so that the problems of poor stability, low gate regulation efficiency and the like of the existing scheme are solved, and meanwhile, a two-dimensional material gate can be prepared into a small strip matched with the molecular scale due to the inherent characteristics of the two-dimensional material gate, the width of the small strip is 5-100 nm, and the small strip is positioned under a molecule, so that the precise regulation and control of the gate on the molecule are realized, the contact area of the gate electrode and the device is reduced, and the generation of leakage current is reduced. Furthermore, the planar processability of the two-dimensional material itself is also of great significance in terms of device integration. In addition, insulating two-dimensional materials of hexagonal boron nitride (h-BN) or gallium nitride (Ga) are adopted 2 N 3 ) The device is packaged, a single-molecule heterojunction functional unit and a graphene electrode can be protected, and the stability and integration possibility of the device are further improved.
In order to achieve the purpose, the monomolecular field effect transistor is composed of a conductive two-dimensional material gate electrode layer, an insulating two-dimensional material dielectric layer, a graphene point electrode, a monomolecular heterojunction and a two-dimensional material protective layer;
the two-dimensional grid material is graphene, silicon alkene and 1T-phase titanium disulfide (1T-TiS) 2 ) 1T phase molybdenum disulfide (1T-MoS) 2 ) 1T phase vanadium selenide (1T-VSe) 2 ) 1T phase tungsten antimonide (1T-WTE) 2 ) Or the thickness of the conductive rest metal type two-dimensional material is different from a single layer to multiple layers; the layered two-dimensional material can be obtained by mechanical stripping or CVD growth, and can be stacked and assembled by a dry transfer or wet transfer mode;
the conductive two-dimensional material gate electrode layer can realize accurate imaging, namely: the gate electrode layer is in a strip shape, has the width of 5-100 nm and is positioned right below the molecules; and is positioned between the insulating two-dimensional material dielectric layer and the substrate;
the single-molecule heterojunction and the graphene point electrode are connected through an amido bond;
the monomolecular heterojunction is obtained by self-assembly of one of terphenyl, hexabiphenyl or pyrrolopyrrole-Dione (DPP) molecules with amino modification at the tail ends of two sides;
van der Waals contact is formed between the insulating two-dimensional material dielectric layer and the conductive two-dimensional material gate electrode layer;
the insulating two-dimensional material dielectric layer is in van der Waals contact with the graphene point electrode;
the two-dimensional material protective layer is hexagonal boron nitride (h-BN) or gallium nitride (Ga) 2 N 3 ) The thickness of the graphene point electrode is 0.7-20nm, the graphene point electrode and the top of the single-molecule heterojunction are covered, on one hand, the stability of molecules is improved through Van der Waals contact, on the other hand, the air effect is isolated, and the device is protected;
the dielectric layer of the insulating two-dimensional material has material selection diversity and can be selected from h-BN and Bi 2 SeO 5 ,Ga 2 N 3 Or SrTiO 3 As a dielectric layer; the thickness of the material atomic layer is controllable, the h-BN thickness is 0.7-20nm, and the range of the corresponding applicable gate voltage is 0.1-10V; bi 2 SeO 5 The thickness is 1-20nm, and the corresponding applicable grid voltage range is 0.1-10V; ga 2 N 3 The thickness is 0.5-20nm, and the corresponding applicable grid voltage range is 0.1-10V; SrTiO 3 The thickness is 0.5-20nm, and the corresponding applicable grid voltage range is 0.1-10V;
the thickness of the gate electrode layer of the conductive two-dimensional material is 1-100 nm;
the method for preparing the monomolecular field effect transistor comprises the following steps:
1) preparing a conductive two-dimensional material gate electrode layer on a substrate; 2) preparing an insulating two-dimensional material dielectric layer on the upper surface of the conductive two-dimensional material gate electrode layer; 3) preparing a graphene electrode layer on the insulating two-dimensional material dielectric layer; 4) constructing a graphene nano gap point electrode;
wherein the method further comprises:
5) contacting at least one of terphenyl, hexa-biphenyl or pyrrolopyrrole-Dione (DPP) molecules with amino-modified tail ends on two sides with the system obtained in the step 4) for self-assembly, namely connecting the graphene point electrodes through amido bonds to obtain a molecular heterojunction;
6) covering hexagonal boron nitride (h-BN) or gallium nitride (Ga) with a certain thickness on the top of the graphene point electrode and the monomolecular heterojunction 2 N 3 ) So as to play a role in protection and obtain the monomolecular field effect transistor;
said step 5) of the above method of self-assembly further comprises adding a dehydration activator or 1-ethyl-3- (3-dimethylaminopropyl) carbodiimide hydrochloride (EDCI) to the system; the molar ratio of any one of terphenyl, hexabiphenyl or pyrrolopyrroledione (DPP) molecules with amino modification at both side ends to the dehydration activating agent is 1:20-40 or 1: 30;
the self-assembly is carried out in a solvent, and the solvent can be pyridine;
the concentration of the dehydration activator in the solvent is 2X 10 -3 -4×10 -3 mol/L, specifically 3X 10 -3 mol/L;
The graphene electrode can be prepared by various conventional methods in the steps 3) and 4) of the method, such as Electron Beam Lithography (EBL), Reactive Ion Etching (RIE) and other processes;
the conductive two-dimensional material gate electrode layer in the step 1) and the insulating two-dimensional material dielectric layer in the step 2) can be prepared by conventional methods such as mechanical stripping-dry transfer, CVD synthesis-wet transfer and the like;
the invention claims graphene, silylene, 1T phase titanium disulfide (1T-TiS) 2 ) 1T phase molybdenum disulfide (1T-MoS) 2 ) 1T phase vanadium selenide (1T-VSe) 2 ) 1T phase tungsten antimonide (1T-WTE) 2 ) To the use of at least one of the above in the preparation of said monomolecular field effect device;
the invention claims h-BN, Bi 2 SeO 5 ,Ga 2 N 3 Or SrTiO 3 Preparation of the monomolecular field effect device by using at least one of insulating two-dimensional materialsThe dielectric layer of the insulating two-dimensional material;
the invention discloses a monomolecular field effect transistor based on different two-dimensional materials and using terphenyl, hexabiphenyl or pyrrolopyrrole-Dione (DPP) molecules with amino modification at the tail ends of two sides as functional units and a preparation method thereof. The novel two-dimensional material is adopted to replace the grid electrode and dielectric layer material in the traditional field effect transistor. The dielectric layer and the grid of the device are enabled to be smooth at an atomic level, the thickness of the atomic layer is controllable, the accurate control of the monomolecular heterojunction is realized, and the stability and the integration of the device are greatly improved.
Drawings
FIG. 1 is a schematic diagram of the three-dimensional structure of a unimolecular field effect transistor based on a two-dimensional van der Waals heterostructure (taking a graphene gate electrode layer and an h-BN dielectric layer/protective layer as an example);
in the figure: 1 is a graphene electrode (source electrode), 2 is a single-molecule heterojunction, 3 is an h-BN dielectric layer, 4 is an h-BN protective layer, 5 is a graphene electrode (drain electrode), and 6 is a graphene gate electrode layer;
FIG. 2 is a side view schematic of a two-dimensional van der Waals heterostructure based single molecule field effect transistor (taking a graphene gate electrode layer and an h-BN dielectric layer/protective layer as an example);
fig. 3 is a graph of current-bias characteristics of a single molecule field effect transistor based on a terphenyl molecule at a gate voltage of 0V;
FIG. 4 is a characteristic diagram of a current with a gate voltage of a single molecule field effect transistor based on a terphenyl molecule at a bias voltage of 0.1V;
Detailed Description
The present invention will be further illustrated with reference to the following specific examples, but the present invention is not limited to the following examples. The method is a conventional method unless otherwise specified. The starting materials are commercially available from the open literature unless otherwise specified.
The electrical test involved in the present invention is carried out under vacuum conditions (<1×10 -4 Pa) was used. The main related test instruments include Agilent 4155C semiconductor tester, ST-500-probe station (Janis Research Company), and comprehensive physical property test system (PPMS). Wherein, the testing temperature is accurately regulated and controlled by the combination of liquid nitrogen, liquid helium and a heating platform.
Example 1: graphene and h-BN based on CVD growth to construct monomolecular field effect transistor
1) Growing a large-area single-layer graphene film on the copper foil by using a Chemical Vapor Deposition (CVD) method;
2) then, spin-coating PMMA glue on the graphene to form a PMMA-graphene-copper foil sandwich structure, placing the structure into an ammonium persulfate solution with the concentration of 3% for etching, and transferring a sample into clean deionized water to remove residual ammonium persulfate in the graphene after the copper foil is dissolved;
3) then transferring the graphene-PMMA structure to a monocrystalline silicon substrate, and removing PMMA glue by soaking in an acetone solution to obtain a graphene bottom grid;
4) then, growing a single layer of h-BN (Nature,2020,579,219) on the Cu (111) foil obtained through the annealing process by using CVD, and repeating the step to obtain a plurality of single layer of (h-BN) -copper foils;
5) then, spin-coating PMMA glue on h-BN to form a PMMA- (h-BN) -copper foil sandwich structure;
6) then, the structure is placed into an ammonium persulfate solution with the concentration of 3% for etching, after the copper foil is dissolved, a sample is transferred into clean deionized water to remove residual ammonium persulfate, and a PMMA- (h-BN) structure is obtained;
7) stacking the PMMA- (h-BN) structure with the (h-BN) -copper foil structure obtained in the step 4) to obtain PMMA- (h-BN) 2 -copper foil construction, repeating step 6) to remove the copper foil and obtain PMMA- (h-BN) 2 Structure (c);
8) repeating the step 7) for a plurality of times according to the thickness requirement to obtain the required PMMA- (h-BN) n (subscript n represents the number of h-BN layers) structure;
9) transferring the structure onto the graphene bottom grid obtained in the step 3), and removing PMMA glue by soaking in an acetone solution. And then the structure is annealed at 400 ℃ so that the two-dimensional materials are laminated more tightly.
Growing a layer of graphene on the surface of the h-BN dielectric layer by utilizing plasma enhanced chemical vapor deposition (PE-CVD) growth, and forming a gap of 1-4nm through electron beam Exposure (EBL) and Reactive Ion Etching (RIE) to obtain a graphene nano gap point electrode;
the chemical assembly of the molecular heterojunction is specifically as follows:
first, a selected single molecule compound: the dehydrating agent, namely the activating agent 1-ethyl-3- (3-dimethylaminopropyl) carbodiimide hydrochloride (EDCI), of terphenyl and carbodiimide with amino modification at the tail ends of two sides is dissolved in pyridine, and the concentration is respectively 10 - 4 mol/L and 3X 10 -3 mol/L;
Then, a graphene nanogap electrode device (including a graphene gate electrode and an h-BN dielectric layer) is added into the solution. And reacting for 48 hours in an argon atmosphere under dark conditions. Thereafter, the device was taken out of the solution, washed three times with acetone and ultrapure water, respectively, and dried with a nitrogen stream.
And finally covering an h-BN protective layer with the thickness of 10nm on the top of the device, wherein the obtaining mode is the same as that of an h-BN dielectric layer, and the monomolecular field effect transistor based on the CVD grown graphene and h-BN provided by the invention is obtained.
The monomolecular field effect transistor is composed of a graphene gate electrode layer 6, an h-BN dielectric layer 3, a graphene point electrode, a hexabiphenyl monomolecular heterojunction 2 with amino modification at the tail ends of two sides and an h-BN protective layer 4; the molecular heterojunction and the graphene point electrode are connected through an amido bond (see, specifically, Angew. chem. int.Ed.,2013,52, 8666); van der Waals contact is formed between the two-dimensional materials; at any temperature in a temperature range of 2K-300K, fixing the voltage applied to the graphene gate electrode to be 0V, applying source-drain voltage (range: minus 1V-1V), and measuring the I-V characteristic curve (shown in figure 3) of the monomolecular field effect transistor along with the change of bias voltage at an interval of 5 mV; the fixed bias voltage is 0.1V, and the voltage applied to the graphene gate electrode is changed in the range: and (2) 2V to 2V at an interval of 10mV, and measuring an I-V characteristic curve (shown in figure 4) of the monomolecular field effect transistor regulated by the gate voltage, wherein the characteristic shows the conductance characteristic changing along with the gate voltage. The monomolecular field effect transistor obtained by the embodiment has strong regulation and control capability on molecular conductance characteristics, and can be exposed in the air for a long time.
Example 2: graphene and h-BN based on mechanical stripping to construct monomolecular field effect transistor
Firstly, obtaining one or a few layers of graphene by a mechanical stripping mode, namely repeatedly tearing the graphene by using an adhesive tape;
then, transferring graphene onto a silicon substrate by using Polydimethylsiloxane (PDMS) as a transfer medium to serve as a bottom gate electrode; specifically, contacting graphene on the tape with Polydimethylsiloxane (PDMS) on top of the slide, a thin layer of graphene will remain on the PDMS upon separation. And adjusting the alignment of the graphene and the silicon substrate through a three-dimensional translation stage in a microscope system. At the moment, slightly applying force to the glass slide to enable the graphene to be adhered to the silicon substrate, then slowly separating PDMS, and successfully transferring the graphene to the silicon substrate;
and then transferring the h-BN thin layer onto the graphene gate electrode layer by using Polycarbonate (PC) glue as a transfer medium and adopting a dry transfer method. Specifically, the method comprises the following steps: the appropriate h-BN was first prepared on the PC surface on top of the slide 1 by mechanical lift-off. And taking a glass slide 2 with PMDS on the top, taking the PC- (h-BN) from the glass slide 1 by using a transparent adhesive tape, and placing the PC- (h-BN) on the PDMS with the h-BN upward to form a PDMS-PC- (h-BN) structure. The h-BN is almost contacted with the graphene on the silicon substrate through the operation of an optical microscope, meanwhile, the temperature is heated to 60-90 ℃, the PC glue can be heated and stretched, the contact area of the PC and the silicon can be enlarged, the h-BN and the graphene can be completely contacted in the process of gradually moving, then, the heating is stopped, the PC glue can be gradually cooled, the PC glue shrinks from the substrate and is separated from the silicon, and the h-BN is combined on the graphene. Finally, slowly separating the PC glue from the h-BN to obtain an h-BN-graphene van der Waals heterostructure;
growing a layer of graphene on the surface of the h-BN dielectric layer by utilizing PE-CVD growth, and forming a gap of 1-4nm through electron beam Exposure (EBL) and Reactive Ion Etching (RIE) to obtain a graphene nano gap point electrode;
the chemical assembly of the molecular heterojunction is specifically as follows:
first, a selected single molecule compound: with ammonia at both endsThe group-modified terphenyl and carbodiimide dehydrating agent-activating agent 1-ethyl-3- (3-dimethylaminopropyl) carbodiimide hydrochloride (EDCI) is dissolved in pyridine with the concentration of 10 respectively - 4 mol/L and 3X 10 -3 mol/L;
Then, a graphene nanogap electrode device (including a graphene gate electrode and an h-BN dielectric layer) is added into the solution. And reacting for 48 hours in an argon atmosphere under dark conditions. Thereafter, the device was taken out of the solution, washed three times with acetone and ultrapure water, respectively, and dried with a nitrogen stream.
And finally covering an h-BN protective layer with the thickness of 10nm on the top of the device to obtain the monomolecular field effect transistor based on the mechanically stripped graphene and the h-BN.
Referring to the attached drawings 1 and 2, the monomolecular field effect transistor is composed of a graphene gate electrode layer 6, an h-BN dielectric layer 3, a graphene point electrode, a hexabiphenyl monomolecular heterojunction with amino modification at the tail ends of two sides and an h-BN protective layer 4; the molecular heterojunction and the graphene point electrode are connected through an amido bond (see, specifically, Angew. chem. int.Ed.,2013,52, 8666); van der Waals contact is formed between the two-dimensional materials; at any temperature in the temperature range of 2K-300K, fixing the voltage applied to the graphene gate electrode to be 0V, applying source-drain voltage (the range is-1V), and measuring the I-V characteristic curve of the monomolecular field effect transistor along with the change of bias voltage at the interval of 5 mV; the fixed bias voltage is 0.1V, and the voltage applied to the graphene gate electrode is changed in the range: and (2) 2V to 2V at an interval of 10mV, and measuring an I-V characteristic curve of the monomolecular field effect transistor regulated by the gate voltage to show the conductance characteristic changing along with the gate voltage. The monomolecular field effect transistor obtained in the embodiment has strong regulation and control capability on molecular conductance characteristics, and can stably exist in an air environment for a long time.
Example 3: 1T-MoS based on CVD growth 2 Preparation of monomolecular field effect transistor of grid electrode, h-BN medium/protective layer
Following the procedure of example 1, only graphene in the gate electrode layer of the conductive two-dimensional material was replaced with 1T-MoS grown by CVD 2 Obtaining the 1T-MoS based on CVD growth provided by the invention 2 A gate electrode formed on the substrate and having a first electrode,a monomolecular field effect transistor of h-BN dielectric/protective layer.
Example 4: 1T-MoS based on mechanical stripping 2 Preparation of monomolecular field effect transistor of grid electrode, h-BN medium/protective layer
Following the procedure of example 2, only graphene in the gate electrode layer of the conductive two-dimensional material was replaced with mechanically exfoliated 1T-MoS 2 Obtaining the 1T-MoS based on mechanical stripping provided by the invention 2 A gate, a single molecule field effect transistor of h-BN dielectric/protective layer.
Example 5: graphene gate based on CVD growth, Ga 2 N 3 Preparation of monomolecular field effect transistor of dielectric layer
The procedure of example 1 was followed to replace h-BN in the dielectric layer of an insulating two-dimensional material by CVD-grown Ga 2 N 3 The material is obtained into the graphene grid based on CVD growth, Ga 2 N 3 A monomolecular field effect transistor of the dielectric layer.
Example 6: graphene gate, Ga, based on mechanical exfoliation 2 N 3 Preparation of monomolecular field effect transistor of dielectric layer
The procedure of example 2 was followed to replace h-BN in the dielectric layer of an insulating two-dimensional material with mechanically exfoliated Ga 2 N 3 The material is obtained from the graphene grid based on mechanical stripping, Ga 2 N 3 A monomolecular field effect transistor of the dielectric layer.
Example 7: CVD-grown graphene grid, SrTiO 3 Preparation of monomolecular field effect transistor of dielectric layer
The procedure of example 1 was followed to replace h-BN in the dielectric layer of insulating two-dimensional material with CVD grown SrTiO 3 The material can be the graphene grid based on CVD growth, SrTiO 3 A monomolecular field effect transistor of the dielectric layer.
Example 8: graphene grid based on mechanical exfoliation, SrTiO 3 Preparation of monomolecular field effect transistor of dielectric layer
Following the procedure of example 1, the insulation was two-dimensionallyh-BN in the material dielectric layer is replaced by mechanically stripped SrTiO 3 The material obtained is the graphene grid based on mechanical stripping, SrTiO 3 A monomolecular field effect transistor of the dielectric layer.

Claims (9)

1. A monomolecular field effect transistor based on a two-dimensional Van der Waals heterostructure is characterized in that: the graphene dot electrode structure is composed of a conductive two-dimensional material gate electrode layer (6), an insulating two-dimensional material dielectric layer (3), a single-molecule heterojunction (2) based on a graphene dot electrode and a protective layer (4);
the single-molecule heterojunction and the graphene point electrode are connected through an amido bond;
van der waals contact is formed between the two-dimensional materials.
2. The two-dimensional van der waals heterostructure based single molecule field effect transistor of claim 1, wherein: graphene, silicon alkene and 1T-TiS for conductive two-dimensional material gate electrode layer (6) 2 、1T-MoS 2 、1T-VSe 2 Or 1T-WTE 2 As a bottom gate electrode;
h-BN and Bi for insulating two-dimensional material dielectric layer (3) 2 SeO 5 、Ga 2 N 3 Or SrTiO 3 As a dielectric layer;
h-BN or Ga for the protective layer (4) 2 N 3 As a protective layer.
3. The two-dimensional van der waals heterostructure based single molecule field effect transistor of claim 1, wherein: the thickness of the gate electrode layer of the conductive two-dimensional material is 1-100 nm;
in the dielectric layer of the insulating two-dimensional material, the thickness of h-BN is 0.7-20nm, Bi 2 SeO 5 Ga with a thickness of 1-20nm 2 N 3 0.5-20nm thick and SrTiO 3 The thickness is 0.5-20 nm;
the thickness of the protective layer is 0.7-20 nm.
4. The two-dimensional van der waals heterostructure based single molecule field effect transistor of claim 1, wherein: the single-molecule heterojunction adopts terphenyl, hexabiphenyl or pyrrolopyrrole Diketone (DPP) molecules with amino modification at the tail ends of two sides.
5. The two-dimensional van der waals heterostructure based single molecule field effect transistor of claim 1, wherein: the single-molecule heterojunction adopts a self-assembly mode.
6. The method for preparing a two-dimensional van der waals heterostructure-based single molecule field effect transistor as claimed in any of claims 1 to 5, wherein: the van der waals assembling process is adopted, wherein the materials are contacted in a van der waals acting force mode, and the van der waals assembling process comprises the following steps: 1) assembling two-dimensional lamination; 2) the two-dimensional material as each component of the device has atomic-scale controllable flatness and thickness; 3) stability of van der waals heterostructures; 4) combination with graphene-based single-molecule heterojunctions;
the monomolecular heterojunction and the graphene point electrode are connected through an amido bond.
7. The method of claim 6, wherein the two-dimensional van der waals heterostructure-based single-molecule field effect transistor is formed by: in the step 1), the two-dimensional laminated assembly adopts an atomically flat silicon wafer, mica or sapphire as a substrate.
8. The method for preparing a two-dimensional van der waals heterostructure-based single molecule field effect transistor as claimed in claim 6 or 7, wherein: preparing a laminated device by adopting a dry transfer process and a mechanical stripping mode, firstly tearing off a small piece of two-dimensional material crystal A by using an adhesive tape, and then continuously tearing the small piece of two-dimensional material crystal A by using a new adhesive tape to obtain a single-layer or few-layer two-dimensional material A; directly sticking the adhesive tape adhered with the two-dimensional material A on a substrate of mica, monocrystalline silicon or sapphire, and tearing the adhesive tape to obtain a gate electrode layer on the substrate; obtaining a single-layer or few-layer two-dimensional material B by using an adhesive tape by using the same mechanical stripping method, then contacting the two-dimensional material B on the adhesive tape with Polydimethylsiloxane (PDMS) on the top of the glass slide, and when the two-dimensional material B is separated again, keeping a thin layer of the two-dimensional material B on the PDMS; then searching an ultrathin two-dimensional material B on PDMS under a microscope, distinguishing the spatial positions of the two-dimensional materials through the microscope, and adjusting the spatial positions of A and B to be completely consistent through a three-dimensional translation stage so as to overlap and contact; and at the moment, a force is slightly applied to the glass slide on which the B is arranged, the A and the B adhere together, then the PDMS and the A-B heterojunction are slowly separated, so that the PDMS is separated from the B, and only the A-B heterojunction is left on the substrate, thereby realizing the further assembly of the two-dimensional material layer.
9. A method for preparing a two-dimensional van der waals heterostructure-based single molecule field effect transistor as claimed in claim 6 or 7, wherein: the preparation of the laminated device adopts a wet transfer process, (1) a large-area graphene film is grown on a copper foil by using a Chemical Vapor Deposition (CVD) method; (2) the method comprises the steps of spin-coating polymethyl methacrylate (PMMA) glue on graphene to form a PMMA-graphene-copper foil sandwich structure, placing the structure into an ammonium persulfate solution with the concentration of 3% for etching, and transferring a sample into clean deionized water to remove ammonium persulfate remained in the graphene after the copper foil is dissolved; (3) then transferring the graphene-PMMA structure onto a silicon substrate, and removing PMMA glue by soaking in an acetone solution to obtain a graphene grid; (4) growing single-layer h-BN on the Cu (111) foil obtained through annealing process treatment by using CVD, and repeating the step (4) to obtain a plurality of single-layer h-BN-copper foils; (5) spin-coating PMMA glue on the h-BN to form a PMMA- (h-BN) -copper foil sandwich structure; (6) the structure is put into ammonium persulfate solution with the concentration of 3% for etching, and after the copper foil is dissolved, a sample is transferred into clean deionized water to remove residual ammonium persulfate so as to obtain a PMMA- (h-BN) structure; (7) stacking the PMMA- (h-BN) structure with the (h-BN) -copper foil structure obtained in (4) to obtain PMMA- (h-BN) 2 -copper foil construction, repeating step (6) and removing the copper foil to obtain PMMA- (h-BN) 2 Structure; (8) repeating the step (7) for a plurality of times according to the thickness requirement to obtain the required PMMA- (h-BN) n Structure, wherein n represents the number of h-BN layers; (9) transferring the structure to the graphene thin layer obtained in the step (3)Soaking in acetone solution to remove PMMA glue; then, the structure is annealed at 200-500 ℃ to ensure that the two-dimensional materials are laminated more tightly.
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