CN113990970A - Graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector and preparation method and application thereof - Google Patents
Graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector and preparation method and application thereof Download PDFInfo
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Abstract
The invention belongs to the technical field of photoelectric detectors and discloses graphene/WS2‑WSe2A heterojunction/graphene photoelectric detector, a preparation method and applications thereof are provided. The structure of the photoelectric detector is electrode/graphene/WS2‑WSe2Heterojunction/graphene/electrode; the graphene and WSe2‑WS2The heterojunction not being in contact with the electrode and WS2And WSe2Are not in contact. The method is to use SiO2Mechanical stripping method for obtaining single-layer or several-layer WS on/Si substrate2And then WSe is treated by PDMS2Transfer to SiO2WS of/Si2Then adding graphiteTransfer of alkenes to WS separately2And WSe2And finally, photoetching two ends of the graphene, and plating metal electrodes to manufacture the photoelectric detector. Under the irradiation of light power with the wavelength of 405nm and the power of 2mW, the switching ratio of the photoelectric detector reaches about 121 times, and is improved by 0.45 time compared with the switching ratio of a detector without graphene at two ends.
Description
Technical Field
The invention belongs to the technical field of photoelectric detectors, and particularly relates to graphene (Gr)/tungsten disulfide (WS)2) Tungsten diselenide (WSe)2) A heterojunction/graphene photoelectric detector, a preparation method and applications thereof are provided.
Background
Two-dimensional materials, such as graphene and transition metal dichalcogenides, have received much attention in the past decade because of their unique electronic structure and physical properties. Meanwhile, van der waals heterostructures composed of two-dimensional materials and conventional semiconductors have been showing excellent photoelectric properties, and have been receiving attention in recent years. Mechanical lift-off is the most successful technique for obtaining high quality single or few layers of nanocrystals from their native multilayer structure or their growth substrate. Meanwhile, the charge carrier of the graphene shows huge intrinsic mobility, and in addition, the single-layer graphene shows 7^10 within a wide range of 300-2500 nm5cm-1The graphene has high optical absorption coefficient far higher than the excellent optical properties of the traditional semiconductor materials, and provides wide prospects in the aspects of various functional devices such as light-emitting diodes, solar cells, photocatalysts, biosensors, photodetectors and the like by taking graphene as a supporting material and/or an active material. In order to enable the sensor to have better signal quality, eliminate more environmental interference and extract signal information, the photoelectric performance of the photoelectric detector is improved by adding single-layer graphene at two ends of a heterojunction.
Disclosure of Invention
In order to overcome the defects and shortcomings of the prior art, the invention provides graphene/tungsten disulfide (WS)2) Tungsten diselenide (WSe)2) Heterojunction/graphene photodetectors.
It is another object of the present invention to provide the abovegraphene/WS2-WSe2A preparation method of a heterojunction/graphene photoelectric detector is provided. The method proves that the switching ratio reaches 121 times through the test of the probe station, and is higher than that of the pure WS2-WSe2The heterojunction photoelectric detector improves the on-off ratio of the photoelectric detector, and is favorable for promoting the two-dimensional WS2、WSe2And other two-dimensional materials in the fields of optical detection and the like.
The purpose of the invention is realized by the following technical scheme:
a graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector is structurally characterized in that the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector is in an electrode/graphene/WS structure2-WSe2Heterojunction/graphene/electrode; the graphene and WSe2-WS2The heterojunction not being in contact with the electrode and WS2And WSe2Are not in contact.
Preferably, said WS2And WSe2The thickness of the film is 1-50 nm; the thickness of the graphene is 1-20 nm; the electrode is Ti/Au or Cr/Au.
The WS2-WSe2The preparation method of the heterojunction photoelectric detector comprises the following specific steps:
s1, respectively soaking SiO in acetone solution, isopropanol solution and deionized water2A Si substrate, and ultrasonic treatment is carried out for 5min after soaking each time;
s2, using adhesive tape to bond WS2And WSe2Respectively mechanically stripping to obtain strips with a thickness of 1-50 nmWS2And WSe2A thin layer; using PDMS to treat WS2Thin layer transfer to SiO2Separating PDMS and SiO on a/Si substrate2a/Si substrate, such that WS2Thin layer on SiO2On a/Si substrate, then WSe was applied with PDMS2Thin layer transfer to WS2Heating the thin layer at 90-110 ℃ to obtain WS2-WSe2A heterojunction;
s3, transferring two pieces of graphene to be respectively put on the WSe by PDMS2Thin layer and WS2On the thin layer, two pieces of graphene are not compatible with WSe2-WS2A heterojunction region in contact with the first substrate,preparing graphene/WS2-WSe2Heterojunction/graphene;
s4, preparing the graphene/WS2-WSe2SiO of heterojunction/graphene2Placing the Si substrate on a spin coater, sucking the photoresist and dropping the photoresist on a silicon wafer, and heating the silicon wafer at 100-110 ℃ under a dark condition after photoresist is spun; then, respectively photoetching electrodes on the two graphene, wherein the electrodes and the WS2And WSe2The Cr/Ti layer and the Au layer are evaporated on the electrode by electron beams without contact;
s5, soaking the integral substrate in acetone, removing the photoresist, washing and drying, and annealing at 200 ℃ in a glove box to obtain the graphene/WS2-WSe2Heterojunction/graphene photodetectors.
Preferably, the heating time in the step S2 is 4-5 min.
Preferably, the rotating speed in the step S4 is 5000-7000 r/min; the heating time is 4-5 min.
Preferably, the thickness of the Cr/Ti layer in the step S4 is 10-15 nm; the thickness of the Au layer is 50-60 nm.
Preferably, the annealing time in the step S5 is 20-25 min.
Due to the unique photon and electronic characteristics of graphene, the generation and transmission of photocarriers of the graphene are fundamentally different from those of the traditional semiconductor photodetector. Despite only one atomic thickness, it can absorb about 2% of incident light in a wide wavelength range, the carriers of graphene exhibit a huge intrinsic mobility, and graphene can maintain a very high current density, which results in very high bandwidth, zero source-drain bias and dark current operation, and good internal quantum efficiency of graphene. Thus adding graphene to WS2-WSe2The photoelectric performance of the heterojunction is improved by two ends of the heterojunction
Compared with the prior art, the invention has the following beneficial effects:
1. the invention constructs the graphene/WS2-WSe2A heterojunction/graphene photoelectric detector is characterized in that due to high carrier mobility of graphene, the graphene is added to a transmission lineThe photoelectric performance of the photoelectric detector can be improved by two ends of the heterojunction. Under the irradiation of light power with the wavelength of 405nm and the power of 2mW, the on-off ratio of the photoelectric detector is 120-122, and is improved by 0.45 times compared with the on-off ratio of a detector without graphene at two ends.
2. The photoelectric detector is particularly sensitive to the light with the wavelength of 405nm through the gain of Gr to the heterojunction under the light with the wavelength of 405nm and has obvious change under different light powers at 1V. Through gate voltage regulation and control, under the irradiation of 405nm light, the photosensitivity R lambda is 0.56A/W, and the external quantum efficiency EQE reaches 1.63 multiplied by 1010The normalized detectivity D reaches 4.44058 × 1011And (4) Jones.
Drawings
FIG. 1 shows Gr/WS of example 12-WSe2heterojunction/Gr photodetector.
Fig. 2 is an ivdark image of the photodetector of example 1.
Fig. 3 is an ivlight diagram of the photodetector of embodiment 1 under white light.
FIG. 4 is an iv plot of the photodetector of example 1 at different optical powers of 405 nm.
Fig. 5 is an it diagram of the photodetector of example 1 under different bias voltages and gate voltages Vg.
FIG. 6 is a graph of the variation of the Voc \ Isc of the photodetector of example 1 with the optical power density.
FIG. 7 depicts Gr-WS from example 12-WSe2-Gr heterojunction photodetector transfer curve.
Fig. 8 is it diagram of the photodetector of example 1 under different gate voltage control of 405 nm.
Fig. 9 is an it diagram of the photodetector of example 1 at different optical powers of 405 nm.
Detailed Description
The following examples are presented to further illustrate the present invention and should not be construed as limiting the invention. Unless otherwise specified, the technical means used in the examples are conventional means well known to those skilled in the art. Reagents, methods and apparatus used in the present invention are conventional in the art unless otherwise indicated.
Example 1
1. Cleaning SiO2a/Si substrate; and respectively soaking the silicon wafer by using an acetone solution, an isopropanol solution and deionized water, and carrying out ultrasonic treatment for 5 minutes after each soaking.
2. A little WS2、WSe2And respectively placing the two adhesive tapes on the two adhesive tapes, and mechanically stripping to select a slightly flashing material area on the adhesive tape as much as possible, wherein the area can be generally used for tearing out a large-area thin layer.
3. Cutting a small-area PDMS square block with scissors, tearing off a soft layer at one end of the PDMS, and attaching a middle layer to the WS2Pressing the hard layer at the other end of the PDMS for 30 seconds by using a forceps, separating the PDMS from the adhesive tape, and repeatedly using the method to gradually find out the appropriate WS under the microscope2Selecting a material with a large area and a flat material surface, attaching PDMS to a previously washed SiO2/Si substrate, and pressing with tweezers for 30 seconds to separate PDMS and SiO2/Si substrate, WS2Thin layer on SiO2On a/Si substrate.
4. Cutting a small-area PDMS square block by using scissors, tearing off a soft layer at one end of the PDMS, and attaching an intermediate layer to the WSe2The hard layer at the other end of the PDMS was pressed with tweezers for 30 seconds to separate the PDMS from the tape, and then the hard layer at the other end of the PDMS was peeled off with tweezers to attach the side without the material to the center of the glass slide.
5. Using a transfer platform to transfer WSe2Stick to WS2And (5) pasting for 5 minutes, and adjusting the temperature of the transfer platform to 90 ℃ to finish the transfer.
6. Cutting two small-area PDMS blocks with scissors, tearing off the soft layer at one end of PDMS, attaching the middle layer to Gr adhesive tape, pressing the hard layer at the other end of PDMS with forceps for 30 seconds, separating PDMS from the adhesive tape, repeating the method, gradually finding suitable Gr thin layer under microscope, preferably 1 or 2-3 layers of Gr with large area, and attaching PDMS to WSe of SiO2/Si substrate transferred previously2-WS2One of the heterojunctions is connected with WSe2And WS2On top, neither Gr slice touches the heterojunction region.
7. And (3) placing the transferred silicon wafer on a spin coater, sucking a small amount of photoresist by using a suction pipe, dripping the photoresist on the silicon wafer, and setting the rotating speed to be about 5000r/min by using EZ4 spincoat. And (3) putting the silicon wafer after the glue homogenizing into a heating table at 100 ℃ for heating for 4 minutes, and covering the silicon wafer with a cover during the heating to avoid the influence of external light.
8. Placing the silicon chip after drying the photoresist into a photoetching machine to photoetching electrodes, photoetching the electrodes on two Grs respectively, and making two electrodes WS2、WSe2All are not in contact with the camera, focus, time on set 3500->confirm->auto->uv-on->start starts the lithography.
9. Evaporating the photoetched electrode electron beam, and evaporating a 10nmCr layer and a 50nmAu layer;
10. soaking in acetone for 10 minutes, removing the photoresist, absorbing water by using a needle tube for washing, and leading a gold film to fall off due to the washing operation along with the dissolution of the photoresist by the acetone, putting the silicon wafer into deionized water after cleaning the silicon wafer, blowing the water on the surface of the silicon wafer by using a nitrogen gun, putting the silicon wafer under a microscope for measuring the length and width data between electrodes, calculating the area, and then putting the silicon wafer into a rubber drying machine for annealing at the temperature of 150 ℃ and 200 ℃ for 20 minutes.
FIG. 1 shows Gr/WS of example 12-WSe2heterojunction/Gr photodetector. The device is WS2-WSe2The heterojunction photoelectric detector has the structure of electrode/graphene/WS2-WSe2Heterojunction/graphene/electrode; the graphene and WSe2-WS2The heterojunction not being in contact with the electrode and WS2And WSe2Are not in contact. Fig. 2 is an ivdark image of the photodetector of example 1. As can be seen from FIG. 2, the line of the iv plot is gentle and the variation is within one order of magnitude, which illustrates WS with graphene added at both ends2-WSe2The linear region is particularly good in the absence of light for heterojunction photodetectors. Fig. 3 is an ivlight diagram of the photodetector of embodiment 1 under white light. Wherein, (a) is the iv curve diagram of the photodetector, and (b) the a curve is processed logarithmically. As can be seen from fig. 3, the rectification ratio of the detector is 15 compared with the current in the linear region of the amplification region. The rectification ratio of the device is relatively large. FIG. 4 is an iv plot of the photodetector of example 1 at different optical powers of 405 nm.As can be seen from fig. 4, the photocurrent becomes larger and the trend becomes more obvious with the increase of the optical power density at the same voltage with the increase of the optical power density, which shows that the iv diagram of the photodetector under different optical powers of 405nm light shows the gain of the Gr-to-heterojunction. The photodetector is particularly sensitive to 405nm light, and the change is very obvious under different optical powers at 1V. Fig. 5 is an it diagram of the photodetector of example 1 under different bias voltages and gate voltages Vg. As can be seen from FIG. 5, under the irradiation of 405nm light, the gate voltage is controlled, the on-off ratio is 121 times, the photosensitivity R lambda is 0.56A/W, and the external quantum efficiency EQE is 1.63 × 1010The normalized detectivity D reaches 4.44058 × 1011And (4) Jones. Fig. 6 is a graph of the open circuit voltage (Voc) \ short circuit current (Isc) as a function of optical power density for the photodetector of example 1. As can be seen from FIG. 6, the open-circuit voltage monotonically decreases with the optical power density and the short-circuit current monotonically increases, and the maximum value can reach 0.28V and 70nA, which indicates that the device has good photovoltaic performance. FIG. 7 depicts Gr-WS from example 12-WSe2-Gr heterojunction photodetector transfer curve. As can be seen from FIG. 7, IdsFollowing VgThe change is obvious, and the regulation performance of the grid voltage on the source and drain current is good. Fig. 8 is it diagram of the photodetector of example 1 under different gate voltage control of 405 nm. As can be seen from FIG. 8, the control of the gate voltage and bias voltage by controlled variables illustrates the I of the device for bothdsThe method has regulation and control capability and obvious grid voltage regulation and control. Fig. 9 is an it diagram of the photodetector of example 1 at different optical powers of 405 nm. As can be seen from FIG. 9, the it diagram of the device changes significantly at different optical power densities of 405nm, and the gain of the it diagram becomes more significant at the increase of the unit optical power density with the increase of the optical power, which illustrates that the graphene-WS is under the laser of 405nm2-WSe2The graphene heterojunction photoelectric detector has a good on-off ratio, an ultrahigh response rate and a high normalized detection rate.
Comparative example 1
The difference from example 1 is that: preparation of WS2-WSe2Heterojunction, but no graphene added at both ends. The photoelectric detector has a switching ratio of only 83 under 405nm light irradiation, and a photosensitivity Rλ＝-0.002329301External quantum efficiency EQE of 4.5X 107Normalized detectivity D is 2.5944283975 × 1010And (4) Jones.
graphene/WS constructed by the invention2-WSe2Heterojunction/graphite alkene photoelectric detector, because the high carrier mobility of graphite alkene, graphite alkene adds can improve photoelectric detector's photoelectric properties at the both ends of traditional heterojunction. Under the irradiation of light power with the wavelength of 405nm and the power of 2mW, the on-off ratio of the photoelectric detector is 120-122, and is improved by 0.45 times compared with the on-off ratio of a detector without graphene at two ends. The photosensitivity R lambda is 0.56A/W, and the external quantum efficiency EQE reaches 1.63 multiplied by 1010The normalized detectivity D reaches 4.44058 × 1011Jones, also showed a significant improvement over comparative example 1.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations and simplifications are intended to be included in the scope of the present invention.
Claims (7)
1. The graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector is characterized in that the structure of the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photoelectric detector is electrode/graphene/WS2-WSe2Heterojunction/graphene/electrode; the graphene and WSe2-WS2The heterojunction not being in contact with the electrode and WS2And WSe2Are not in contact.
2. The graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector of claim 1, wherein said WS2And WSe2The thickness of the film is 1-50 nm; the thickness of the graphene is 1-20 nm; the electrode is Ti/Au or Cr/Au.
3. The preparation method of the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector according to claim 1 or 2, characterized by comprising the following specific steps:
s1, respectively soaking SiO in acetone solution, isopropanol solution and deionized water2A Si substrate, and ultrasonic treatment is carried out for 5min after soaking each time;
s2, using adhesive tape to bond WS2And WSe2Respectively mechanically stripping to obtain strips with a thickness of 1-50 nmWS2And WSe2A thin layer; using PDMS to treat WS2Thin layer transfer to SiO2Separating PDMS and SiO on a/Si substrate2a/Si substrate, such that WS2Thin layer on SiO2On a/Si substrate, then WSe was applied with PDMS2Thin layer transfer to WS2Heating the thin layer at 90-110 ℃ to obtain WS2-WSe2A heterojunction;
s3, transferring two pieces of graphene to be respectively put on the WSe by PDMS2Thin layer and WS2On the thin layer, two pieces of graphene are not compatible with WSe2-WS2Contact with heterojunction region to obtain graphene/WS2-WSe2Heterojunction/graphene;
s4, preparing the graphene/WS2-WSe2SiO of heterojunction/graphene2Placing the Si substrate on a spin coater, sucking the photoresist and dropping the photoresist on a silicon wafer, and heating the silicon wafer at 100-110 ℃ under a dark condition after photoresist is spun; then, respectively photoetching electrodes on the two graphene, wherein the electrodes and the WS2And WSe2The Cr/Ti layer and the Au layer are evaporated on the electrode by electron beams without contact;
s5, soaking the integral substrate in acetone, removing photoresist, washing and drying, and annealing in a glove box at 100-200 ℃ to obtain graphene/WS2-WSe2Heterojunction/graphene photodetectors.
4. The method for preparing the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector as claimed in claim 3, wherein the heating time in the step S2 is 4-5 min.
5. The method for preparing the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector according to claim 3, wherein the rotation speed in step S4 is 5000-7000 r/min; the heating time is 4-5 min.
6. The method for preparing the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector according to claim 3, wherein the thickness of the Cr or Ti layer in the step S4 is 10-15 nm; the thickness of the Au layer is 50-60 nm.
7. The method for preparing the graphene/tungsten disulfide-tungsten diselenide heterojunction/graphene photodetector as claimed in claim 3, wherein the annealing time in the step S5 is 20-25 min.
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