CN115568261A - Method for opening band gap of double-layer graphene and prepared double-layer graphene device - Google Patents
Method for opening band gap of double-layer graphene and prepared double-layer graphene device Download PDFInfo
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Abstract
The invention discloses a method for opening a band gap of double-layer graphene and a prepared double-layer graphene device. The method provided by the invention is convenient to operate, simple in device structure and wide in application, avoids the micro-nano processing process of the traditional electrical grid voltage regulation and control method, and has important significance for applying the double-layer graphene to the field of semiconductor electronic devices.
Description
Technical Field
The invention relates to the technical field of semiconductor electronics, in particular to a method for opening a band gap of double-layer graphene and a prepared double-layer graphene device.
Background
Graphene, an important two-dimensional material, has attracted much attention because it exhibits excellent properties and novel physical phenomena. Two single-layer graphene AB (or BA) are stacked, i.e., double-layer graphene is formed. The intrinsic double-layer graphene with inversion symmetry is a semiconductor with zero band gap, but the spatial inversion symmetry of the intrinsic double-layer graphene can be broken by applying a vertical electric field to the intrinsic double-layer graphene, so that the band gap of the intrinsic double-layer graphene is opened and can be adjusted within a certain range, and the property endows the intrinsic double-layer graphene with application prospects in semiconductor devices and nanoelectronics.
The currently commonly used method for opening the band gap is mainly an electrical gate voltage method [ nature 459,820 (2009) ], namely, applying voltages on top and bottom electrodes of a material to form an electric displacement field on a middle dielectric layer, and adjusting an electric field in a vertical direction to open the band gap. However, this method requires electrodes on the top and bottom of the material, and the material and the electrodes are separated by insulating materials such as silicon dioxide, aluminum oxide, boron nitride, etc., so it is necessary to introduce micro-nano processing techniques such as photolithography, etching, evaporation coating, etc. during the preparation process, the operation is complicated, and it is very easy to introduce organic residual glue during the process, which causes pollution and affects the material properties. Therefore, how to provide a simple, effective and widely-applied method for opening the band gap of the double-layer graphene has great significance for the development of the graphene in the field of semiconductors.
Disclosure of Invention
Based on the technical problems, the invention provides a method for opening a band gap of double-layer graphene and a prepared double-layer graphene device, so as to solve the problems of complex operation and limited applicability in the method for opening the band gap of the double-layer graphene in the prior art.
The invention firstly provides a method for opening a band gap of double-layer graphene, which is characterized in that the double-layer graphene is arranged between a first molecular layer and a second molecular layer, the first molecular layer carries out electron (N type) doping on the double-layer graphene, and the second molecular layer carries out hole (P type) doping on the double-layer graphene, so that the band gap of the double-layer graphene is opened.
In some embodiments of the invention, the molecule of the first molecular layer is Aminopropyltriethoxysilane (APTES) molecule having a bare-NH 2 A group that electronically (N-type) dopes graphene.
In some embodiments of the invention, the molecule of the second molecular layer is nitric acid (HNO) 3 ) A molecule.
Further, the invention provides a specific method for opening the band gap of the double-layer graphene, which comprises the following steps:
step A: preparing a functional substrate, wherein the substrate sequentially comprises the following components from bottom to top: the silicon substrate, the silicon dioxide layer and the first molecular layer;
and B: forming a double-layer graphene layer on the functional substrate obtained in the step A;
and C: forming a second molecular layer on the double-layer graphene layer obtained in the step B;
step D: and C, preparing an electrode on the second molecular layer obtained in the step C.
In some embodiments of the present invention, the specific method of step a is: irradiating the silicon substrate with the silicon dioxide layer by using ultraviolet light to enable the silicon dioxide layer to generate activity, and then soaking the substrate into a solution of first molecules, wherein the first molecules perform monolayer self-assembly on the active silicon dioxide to form a first molecular layer.
In some embodiments of the present invention, in step B, the bilayer graphene layer is formed directly on the target substrate by a mechanical lift-off process.
In some embodiments of the present invention, the specific method of step C is: and (3) placing the substrate with the double-layer graphene layer with one surface of the double-layer graphene facing downwards at the bottleneck of a beaker filled with a second molecular solution, and volatilizing the second molecules to form a second molecular layer on the surface of the double-layer graphene layer.
In some embodiments of the present invention, in step D, the electrode is at least one of titanium, chromium and gold, and the thickness of the electrode is not less than 30nm.
In some embodiments of the present invention, the specific method of step D is: and placing a hard mask plate with electrode patterns above the second molecular layer, observing and operating through an optical microscope to align the electrode patterns to the double-layer graphene and fixing the electrode patterns, and then performing electron beam evaporation coating to obtain the electrode patterns.
Furthermore, the invention also provides a double-layer graphene device prepared by the method, which sequentially comprises the following components from bottom to top: a silicon substrate; a silicon dioxide layer; a first molecular layer formed over the silicon dioxide layer; a bilayer graphene layer formed over the first molecular layer; the second molecular layer is formed above the double-layer graphene layer; and an electrode formed over the second molecular layer and in contact with the double-layer graphene (the second molecular layer does not affect the contact of the electrode with the graphene).
According to the technical scheme, the method for opening the band gap of the double-layer graphene and the prepared double-layer graphene device have the following beneficial effects:
(1) The method for opening the band gap of the double-layer graphene is simple and convenient to operate, complex micro-nano processing steps are not needed, and the condition that the material properties are influenced due to the pollution of organic residual glue is avoided.
(2) The double-layer graphene device provided by the invention has a simple structure, is not covered by an insulating layer and a top gate electrode above the double-layer graphene, has wide application compared with a device obtained by a traditional electric gate voltage method, and not only can be applied to transport test, but also can be applied to characterization research in the aspects of optical property research and scanning probe microscopy.
Drawings
Fig. 1 to 4 are schematic diagrams of steps of a method for opening a band gap of a double-layer graphene provided by the present invention, wherein fig. 4 is a schematic diagram of a structure of a finally obtained double-layer graphene device.
Fig. 5 is a raman spectrum characterization of double-layer graphene obtained by using a mechanical exfoliation method in example 1 of the present invention.
Fig. 6 is an optical microscope image of a double-layered graphene device prepared in example 1 of the present invention.
Fig. 7 is a graph showing the result of the regulation and control of resistance with gate voltage in the room temperature environment of the double-layer graphene device prepared in embodiment 1 of the present invention.
Reference numbers in the figures: 10-a functional substrate; 11-a silicon substrate; 12-a silicon dioxide layer; 13-a first molecular layer; 20-bilayer graphene layers; 30-a second molecular layer; 40-electrodes.
Detailed Description
The method for opening the band gap of the double-layer graphene and the prepared double-layer graphene device have the advantages of simple structure, convenience in operation and wide application, and have great significance for the development of graphene in the field of semiconductors.
To make the objects, technical solutions and advantages of the present invention more apparent, the present disclosure will be described in further detail with reference to the following embodiments and the accompanying drawings.
As shown in fig. 1 to 4, the method for opening the band gap of the double-layer graphene provided by the invention comprises the following steps:
step A: preparing a functional substrate 10 comprising, in order from bottom to top: a silicon substrate 11, a silicon dioxide layer 12, a first molecular layer 13;
and B: forming a double-layer graphene layer 20 on the functional substrate 10 obtained in the step a;
and C: forming a second molecular layer 30 on the bilayer graphene layer 20 obtained in the step B;
step D: an electrode 40 is prepared on the second molecular layer 30 obtained in step C.
The method for opening the band gap of the double-layer graphene is simple and convenient to operate, wide in application and strong in controllability.
Specifically, the molecules in the first molecular layer 13 in the functional substrate 10 are Aminopropyltriethoxysilane (APTES) molecules. APTES molecules having naked-NH 2 A group that electronically (N-type) dopes graphene.
Specifically, the method of forming the bilayer graphene layer 20 on the functional substrate 10 includes: is formed directly on the functional substrate 10 using a mechanical lift-off process.
In particular toThe second molecular layer 30 is nitric acid (HNO) 3 ) The molecules, hole (P-type) doping the bilayer graphene layer 20.
Specifically, the material of the electrode 40 is at least one of titanium, chromium and gold, and the thickness of the electrode 40 is not less than 30nm.
Specifically, the electrode 40 is prepared by using a hard mask in combination with an electron beam evaporation coating to obtain an electrode pattern. The electrode is prepared by adopting a hard mask method, so that the pollution of organic residual glue to the double-layer graphene layer in the micro-nano processing process can be avoided.
As shown in fig. 4, the present invention further provides a double-layer graphene device prepared by the above method, which sequentially includes, from bottom to top: a silicon substrate 11; a silicon dioxide layer 12; a first molecular layer 13 (i.e., a layer of APTES molecules) formed over the silicon dioxide layer; a bilayer graphene layer 20 formed over the first molecular layer 13; a second molecular layer 30 (i.e., nitric acid molecules) formed over the bilayer graphene layer 20; and an electrode 40 formed over the second molecular layer 30 and in contact with the double-layer graphene 20. Among them, the silicon substrate 11, the silicon dioxide layer 12, and the first molecular layer 13 constitute the functional substrate 10.
From the above description, those skilled in the art should clearly understand the method for opening the band gap of the bi-layer graphene and the prepared bi-layer graphene device provided by the present invention.
The method for opening the band gap of the double-layer graphene and the effectiveness of the prepared double-layer graphene device provided by the invention are verified by using a specific embodiment.
Example 1
The method for opening the band gap of the double-layer graphene and the prepared double-layer graphene device provided by the embodiment specifically include:
a, step a: with SiO grown on a silicon knife 2 Si substrate of the layer (hereinafter expressed as SiO) 2 Si substrate) cut into squares of about 1cm side, using SiO 2 SiO in Si substrate 2 The thickness is 285-300nm, and the 365nm ultraviolet light is used for irradiating SiO 2 Si substrate for 15 minutes. Ozone is generated in the air after the ultraviolet light is irradiated, and the ozone can enable the silicon dioxide layer to generate activity. Will be purplePlacing the substrate irradiated by external light into prepared aminopropyltriethoxysilane solution, wherein the concentration of aminopropyltriethoxysilane in the solution is one percent, and the solvent is toluene, at this time, aminopropyltriethoxysilane (APTES) molecules will be in SiO with activity 2 Performing monolayer self-assembly. And soaking the substrate for 3 hours, taking out the substrate, putting the substrate into a toluene solution, carrying out ultrasonic treatment for 15 minutes, cleaning the redundant aminopropyltriethoxysilane molecules on the surface of the substrate, and only leaving a layer of self-assembled molecules on the substrate. And then, placing the substrate cleaned by the toluene in an acetone solution for 5 minutes to remove the residual toluene solution, then carrying out ultrasonic treatment for 5 minutes by using ethanol, taking out the substrate, and drying the substrate by using a nitrogen gun to obtain the functional substrate, wherein the functional substrate is shown in figure 1.
Step b: placing graphene on a functional substrate by a mechanical stripping method, observing and finding double-layer graphene under an optical microscope, and determining the obtained graphene to be the double-layer graphene by auxiliary judgment of Raman spectrum testing, as shown in fig. 2 and 5.
Step c: and d, sticking the functional substrate with the double-layer graphene layers obtained in the step b on a glass sheet by using solid Polydimethylsiloxane (PDMS), pouring the glass sheet on the opening of a 100mL beaker with the side with the double-layer graphene facing downwards, pouring about 20mL of concentrated nitric acid (analytically pure AR, the content of 65.0% -68.0%) into the beaker, wherein the distance between the concentrated nitric acid liquid and the double-layer graphene is 4-6cm, and placing the beaker in a sealed box or a fume hood for a period of time, wherein the general time is not more than 12 hours, and the longer the time is, the larger the doping degree of the nitric acid molecules to the cavities (P type) of the double-layer graphene is, as shown in fig. 3.
Step d: placing a hard mask on the double-layer graphene, observing and operating through an optical microscope to align an electrode pattern on the double-layer graphene and fixing the electrode pattern, and sequentially and physically depositing 5nm of titanium and 30nm of gold by using an electron beam evaporation coating technology to obtain an electrode pattern, as shown in fig. 4 and 6.
Through the above preparation steps, the double-layer graphene device shown in fig. 4 is obtained in this embodiment, and includes, from bottom to top: a silicon substrate 11; a silicon dioxide layer 12; a first molecular layer 13 (i.e., a layer of APTES molecules) formed over the silicon dioxide layer 12; a bilayer graphene layer 20 formed over the first molecular layer 13; a second molecular layer 30 (i.e., nitric acid molecules) formed over the bilayer graphene layer 20; and an electrode 40 formed over the second molecular layer 30 and in contact with the double-layer graphene 20. Among them, the silicon substrate 11, the silicon dioxide layer 12, and the first molecular layer 13 constitute the functional substrate 10.
The device obtained in this example was placed in a room temperature environment to perform a gate voltage variation test, and a comparison was performed with a double-layer graphene device without the first molecular layer and the second molecular layer, and the result is shown in fig. 7. It can be seen that the resistance of the neutral point (CNP) in the variation curve of the resistance with the gate voltage obtained in this embodiment is increased by about 9 times compared with the comparative sample, the bandgap of the double-layer graphene is effectively opened, and the fermi energy and the bandgap can be changed by adjusting the gate voltage or changing the doping time of the nitric acid molecule on the double-layer graphene.
In conclusion, the method for opening the band gap of the double-layer graphene and the prepared double-layer graphene device can realize the opening of the band gap of the double-layer graphene and the continuous regulation and control of the fermi surface, and the device has the advantages of simple structure, convenience in operation, strong controllability and wide application. Compared with the traditional method for regulating and controlling the electric grid voltage, the method avoids the pollution of organic residual glue in the micro-nano processing process, and meanwhile, the obtained double-layer graphene device with the opened band gap is not covered by an insulating layer or a top grid electrode, so that the method can be applied to transport test, optical property research and characterization research in scanning probe microscopy, and has important significance for applying the double-layer graphene to the field of semiconductor electronic devices.
It should also be noted that directional terms, such as "upper", "lower", "front", "rear", "left", "right", and the like, used in the embodiments are only directions referring to the drawings, and are not intended to limit the scope of the present disclosure. Throughout the drawings, like elements are represented by like or similar reference numerals. Conventional structures or constructions will be omitted when they may obscure the understanding of the present disclosure. And the shapes and sizes of the respective components in the drawings do not reflect actual sizes and proportions, but merely illustrate the contents of the embodiments of the present invention.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention, and it should be understood that the above-mentioned embodiments are only exemplary embodiments of the present invention, and are not intended to limit the present invention, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention shall be included in the protection scope of the present invention.
Claims (10)
1. A method for opening a band gap of double-layer graphene is characterized in that: the double-layer graphene is arranged between a first molecular layer and a second molecular layer, the first molecular layer carries out electron doping on the double-layer graphene, and the second molecular layer carries out hole doping on the double-layer graphene, so that the band gap of the double-layer graphene is opened.
2. The method of opening the bandgap of bilayer graphene according to claim 1, wherein: the molecules of the first molecular layer are aminopropyltriethoxysilane molecules.
3. The method of opening the bandgap of bilayer graphene according to claim 1, wherein: the molecules of the second molecular layer are nitric acid molecules.
4. A method of opening the bandgap of bi-layer graphene according to claim 1, 2 or 3, including the steps of:
step A: preparing a functional substrate, wherein the substrate sequentially comprises the following components from bottom to top: the silicon substrate, the silicon dioxide layer and the first molecular layer;
and B: forming a double-layer graphene layer on the functional substrate obtained in the step A;
and C: forming a second molecular layer on the double-layer graphene layer obtained in the step B;
step D: and C, preparing an electrode on the second molecular layer obtained in the step C.
5. The method for opening the band gap of the bilayer graphene according to claim 4, wherein the specific method of the step A is as follows: irradiating the silicon substrate with the silicon dioxide layer by using ultraviolet light to enable the silicon dioxide layer to generate activity, and then soaking the substrate into a solution of first molecules, wherein the first molecules perform monolayer self-assembly on the active silicon dioxide to form a first molecular layer.
6. The method of opening the bandgap of bi-layer graphene of claim 4, wherein: in the step B, the double-layer graphene layer is directly formed on the target substrate by a mechanical stripping method.
7. The method of opening the bandgap of bilayer graphene according to claim 4, wherein: the specific method of the step C comprises the following steps: and (3) placing the substrate with the double-layer graphene layer with one surface of the double-layer graphene facing downwards at the bottleneck of a beaker filled with a second molecular solution, and volatilizing the second molecules to form a second molecular layer on the surface of the double-layer graphene layer.
8. The method of opening the bandgap of bi-layer graphene of claim 4, wherein: in step D, the electrode is at least one of titanium, chromium and gold, and the thickness of the electrode is not less than 30nm.
9. The method of opening the bandgap of bilayer graphene according to claim 4, wherein: the specific method of the step D is as follows: and placing a hard mask plate with electrode patterns above the second molecular layer, aligning the electrode patterns to the double-layer graphene through observation and operation of an optical microscope, fixing the electrode patterns, and then performing electron beam evaporation coating to obtain the electrode patterns.
10. A double-layer graphene device prepared according to the method of any one of claims 1 to 9, wherein: the double-layer graphene device sequentially comprises from bottom to top: a silicon substrate; a silicon dioxide layer; a first molecular layer formed over the silicon dioxide layer; a bilayer graphene layer formed over the first molecular layer; the second molecular layer is formed above the double-layer graphene layer; and an electrode formed over the second molecular layer and in contact with the bilayer graphene.
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