CN111180546B - Multilayer monocrystalline silicon nano-film/graphene photoelectric detector and preparation method thereof - Google Patents
Multilayer monocrystalline silicon nano-film/graphene photoelectric detector and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a multilayer monocrystalline silicon nano-film/graphene photoelectric detector and a preparation method thereof, wherein the photoelectric detector adopts a multilayer monocrystalline silicon nano-film/graphene laminated structure on the basis of excellent performance of the monocrystalline silicon/graphene Schottky heterojunction photoelectric detector, and on the basis of flexibility, the multilayer structure increases the contact area between graphene and the monocrystalline silicon nano-film in the same region on one hand; meanwhile, the thickness is increased, the absorption capacity of the device on long-wavelength light is improved, and the response of the device on the long-wavelength light is improved; and the monocrystalline silicon nano-film is of a porous structure, so that the reflection of the monocrystalline silicon nano-film to light is reduced, and the absorption of the device to light is improved. The multi-layer monocrystalline silicon nano-film/graphene Van der Waals heterojunction photoelectric detector structure can improve the detection performance of a device, and provides a scheme for optimizing the performance of the device in the field.
Description
Technical Field
The invention relates to the field of photoelectric detectors, in particular to a multilayer monocrystalline silicon nano-film/graphene photoelectric detector and a preparation method thereof.
Background
The basic principle of the photoelectric sensor is based on the photoelectric effect, when light irradiates on some substance, the energy of photons can be transferred to electrons, so that the state of the electrons is changed, the electrical characteristics of the substance are correspondingly changed, and the device for converting optical signals into electric signals is achieved. The photoelectric detector has wide application in the fields of communication, medical treatment and health, computer technology, space technology and the like.
The monocrystalline silicon/graphene Schottky heterojunction photoelectric detector has the advantages of high sensitivity, high optical response, high response speed and the like, and has important application in the aspects of high-speed signal modulation, weak signal detection and the like. The traditional monocrystalline silicon/graphene schottky heterojunction photoelectric detector has excellent performance, but cannot be flexible, the application field is greatly limited, and particularly in the biomedical field, wearable flexible electronic devices show vigorous activity; and other types of flexible photoelectric detectors have detection performance inferior to that of silicon-based photoelectric detectors on one hand, have higher preparation cost on the other hand, and cannot be compatible with the existing integrated circuit process. For a single-layer monocrystalline silicon nano-film-graphene heterojunction photoelectric detector, because the thickness of the monocrystalline silicon nano-film is hundreds of nanometers, although the monocrystalline silicon nano-film has larger response to short-wavelength light, the device has lower absorption ratio to long-wavelength light and smaller response; the monocrystalline silicon has certain reflection to light, so that the absorption of the photoelectric detector to light is reduced; and the single-layer monocrystalline silicon nano-film-graphene flexible photoelectric detector is easy to break and slide in the preparation process, and the yield is not high.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a multilayer monocrystalline silicon nano-film/graphene photoelectric detector and a preparation method thereof, the photoelectric detector has more light absorption, larger response and more stable performance on the basis of keeping the flexible characteristic of a single-layer monocrystalline silicon nano-film/graphene flexible photoelectric detector, and the specific technical scheme is as follows:
a multilayer monocrystalline silicon nano-film/graphene photoelectric detector comprises a substrate, two bottom metal interconnection wires, a monocrystalline silicon nano-film, graphene and two top metal interconnection wires, wherein a plurality of contact electrodes are formed at the contact position of the bottom layer metal interconnection lead and the top layer metal interconnection lead and the monocrystalline silicon nano-film, the other bottom layer metal interconnection lead and the top layer metal interconnection lead and the graphene form another two contact electrodes, the monocrystalline silicon nano-films and the graphene are alternately stacked to form a plurality of layers of monocrystalline silicon nano-films and a plurality of layers of graphene, an overlapping area is formed between each layer of monocrystalline silicon nano-film and the graphene contacted with the upper surface and the lower surface of each layer of monocrystalline silicon nano-film, monocrystalline silicon/graphene Schottky heterojunctions are respectively formed, and signals generated at the Schottky heterojunctions are respectively led out through the bottom layer metal interconnection lead and the top layer metal interconnection lead.
Further, the thickness of the monocrystalline silicon nano film is 100 nm-300 nm, the thickness of the bottom layer metal interconnection lead is 30 nm-100 nm, and the thickness of the top layer metal interconnection lead is 300 nm-500 nm.
Further, the monocrystalline silicon nano-film is obtained by stripping from silicon on an insulator and is of a porous structure.
Further, the monocrystalline silicon nano-film is transferred to the metal contact electrode on the flexible substrate by a wet transfer method.
Furthermore, the number of layers of the monocrystalline silicon nano-film is 3, and the number of layers of the graphene is 3.
The preparation method of the photoelectric detector specifically comprises the following steps:
s1, photoetching and developing the bottom layer metal interconnection wire pattern on the substrate;
s2, evaporating metal by an electron beam, and washing away photoresist to form a bottom layer metal interconnection lead;
s3, transferring the monocrystalline silicon nano film to one end of the substrate bottom layer metal interconnection wire by a wet transfer method;
s4, photoetching and developing the monocrystalline silicon nano film pattern, and etching the exposed monocrystalline silicon;
s5, transferring the graphene to one end of the metal interconnection wire at the other bottom layer of the substrate;
s6, photoetching and developing the graphene pattern, and etching the exposed graphene;
s7: repeating the steps S3-S6;
s8: photoetching and developing the top layer interconnection wire pattern;
s9: and evaporating metal by an electron beam, and washing away the photoresist to form a top metal interconnection wire.
Further, the substrate material is polyimide;
further, the bottom layer metal interconnection wire is composed of Cr and Au, and when the electron beam in S2 is evaporated, the Cr is evaporated first, and then the Au is evaporated.
Further, the top metal interconnection wire is made of Au;
further, in step S7, the number of repetitions is 3.
The invention has the following beneficial effects:
according to the multilayer monocrystalline silicon nano-film/graphene heterojunction photoelectric detector provided by the invention, on the basis of ensuring the flexibility characteristic of the single-layer monocrystalline silicon/graphene schottky heterojunction photoelectric detector, the responsivity of the device to long-wavelength light is improved, the reflection of the device to light is reduced due to the existence of the porous structure, the detection performance of the device is improved, meanwhile, the multilayer monocrystalline silicon nano-film/graphene photoelectric detector is more stable in structure, and the rate of finished products of device preparation is higher.
The preparation method of the multilayer monocrystalline silicon nano-film/graphene heterojunction photoelectric detector is based on a mature silicon-based electronic technology process, so that the yield of devices prepared by the preparation method is high, and meanwhile, all steps of the process method do not involve high-temperature operation steps (the temperature of all process steps is lower than 230 ℃), so that the photoelectric detector can be prepared on a flexible substrate based on the process provided by the invention, and the traditional silicon-based photoelectric detector is introduced into the technical field of flexible electronics.
Drawings
Fig. 1 is a cross-sectional view of a device of the present invention.
Fig. 2 is a top view of a device of the present invention.
Fig. 3 is a flow chart of the device fabrication of the present invention.
In the figure: 1. the structure comprises a polyimide substrate, 2, a bottom layer metal interconnection wire, 3, a monocrystalline silicon nano film, 4, graphene, 5 and a top layer metal interconnection wire.
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings and preferred embodiments, and the objects and effects of the present invention will become more apparent, it being understood that the specific embodiments described herein are merely illustrative of the present invention and are not intended to limit the present invention. The invention provides a multilayer monocrystalline silicon nano-film/graphene photoelectric detector and a preparation method thereof, as shown in figure 1-2, the detector comprises: the structure comprises a polyimide substrate 1, a bottom layer metal interconnection lead 2, a monocrystalline silicon nano film 3, graphene 4 and a top layer metal interconnection lead 5.
The contact positions of one bottom layer metal interconnection lead 2 and one top layer metal interconnection lead 5 and the monocrystalline silicon nano film 3 form a plurality of contact electrodes, the other bottom layer metal interconnection lead 2 and the other top layer metal interconnection lead 5 and the graphene 4 form another plurality of contact electrodes, the monocrystalline silicon nano film 3 and the graphene 4 are alternately stacked to form a plurality of layers of monocrystalline silicon nano films and a plurality of layers of graphene, an overlapped region is arranged between each layer of monocrystalline silicon nano film and the graphene to form a plurality of monocrystalline silicon/graphene Schottky heterojunctions, and signals generated at the Schottky heterojunctions are respectively led out 5 through the bottom layer metal interconnection lead 2 and the top layer metal interconnection lead.
After the thickness of the monocrystalline silicon is reduced to a nanometer level, the bending radius of the monocrystalline silicon becomes very small, and good flexibility is shown.
The single atomic layer graphene 4 is prepared on the copper foil substrate by a CVD method, has excellent performances of high light transmittance and wide spectrum absorption, and is in contact with the surface of monocrystalline silicon to form an ultra-shallow Schottky heterojunction.
Polyimide has excellent flexibility, high insulating property and good biocompatibility, so that the substrate is made of the polyimide.
In this embodiment, the monocrystalline silicon nano-film is transferred to the bottom metal interconnection wire contact electrode on the polyimide substrate by a wet transfer method. The monocrystalline silicon nano-film is obtained by stripping silicon on an insulator and has a porous structure.
In order to improve the conductivity of the metal interconnection wire and ensure the integrity of the monocrystalline silicon nano-film and the graphene when contacting with the bottom metal interconnection wire, the thickness of the bottom metal interconnection wire cannot be too thick or too thin, and is preferably 30nm to 100 nm.
In order to further reduce the contact resistance between the monocrystalline silicon nano-film and the metal interconnection wire and enable signals of each layer of monocrystalline silicon nano-film and each layer of graphene to be transmitted through the metal interconnection wire better, the thickness of the top layer interconnection wire is preferably 300-500 nm.
In order to ensure the availability of the monocrystalline silicon thin film and the flexibility of the multilayer monocrystalline silicon nano thin film, the thickness of the monocrystalline silicon nano thin film is preferably 100 nm-300 nm, and the number of layers of the monocrystalline silicon nano thin film is preferably 3.
The invention also provides a preparation method of the multilayer monocrystalline silicon nano-film/graphene photoelectric detector, as shown in figure 3, a polyimide substrate is prepared, a bottom layer metal interconnection wire pattern is photoetched and developed on the substrate, metal is evaporated and deposited by an electron beam, photoresist is washed off to form a bottom layer metal interconnection wire pattern, a monocrystalline silicon nano-film is transferred to one end of a bottom layer metal interconnection wire, etching forming is carried out, graphene is transferred to one end of another bottom layer metal interconnection wire, the processes of transferring and etching the monocrystalline silicon nano-film and transferring and etching the graphene are repeatedly carried out to form a multilayer monocrystalline silicon nano-film/graphene stacked structure, then a top layer metal interconnection wire pattern is photoetched and developed, metal is evaporated by the electron beam, and the photoresist is washed off to form a top layer metal interconnection wire. The monocrystalline silicon nano-film is obtained by stripping top silicon on the insulator, and the steps are photoetching top silicon patterns on the insulator, etching the top silicon on the insulator to the oxygen burying layer, putting into corrosive liquid to corrode the oxygen burying layer, stripping the top monocrystalline silicon nano-film, cleaning and transferring. The graphene obtaining step comprises the steps of spin-coating a supporting layer on a copper foil substrate with the grown graphene, corroding the copper foil substrate, and cleaning the graphene for transfer printing.
The manufacturing process comprises the following steps:
s1: and photoetching and developing a bottom layer metal interconnection wire pattern on the polyimide substrate.
S2: and putting the developed substrate into an electron beam evaporation device for evaporating a layer of metal, wherein the electron beam evaporation process is Cr/Au5nm/60 nm. And sequentially putting the substrate subjected to metal evaporation into acetone and isopropanol solution to wash away the residual photoresist to form a metal interconnection wire, and then putting the metal interconnection wire into deionized water to clean.
And S3, pulling the square monocrystalline silicon nano-film (preferably, 5mm by 5mm) floating on the water surface, stripped from the SOI, out of the water by using a polyimide substrate in a wet transfer mode, and placing the square monocrystalline silicon nano-film at one end of a bottom metal interconnection wire on the substrate.
1) And photoetching and etching a square hole array with the side length of 5 microns and the interval of 400 microns on the SOI top layer silicon, etching a square groove with the side width of 20 microns and the side length of 5 millimeters on the periphery of the square hole array, and etching the square hole array and the square groove to the SOI buried oxide layer.
2) And soaking the etched SOI in a buffer oxide etching solution, after the buried oxide layer is corroded, slightly shaking the liquid, suspending the monocrystalline silicon nano film on the liquid surface, fishing up the monocrystalline silicon nano film by using a glass slide, transferring the monocrystalline silicon nano film into deionized water, soaking for a period of time, and washing away the buffer oxide etching solution. (Note: this step involves buffering the oxide etchant, which is dangerous and should be done with safety precautions).
3) The monocrystalline silicon nano film suspended on the surface of deionized water is fished by a polyimide substrate attached to a glass substrate, at the moment, a layer of metal interconnection wire is evaporated on the polyimide substrate, and the size of the monocrystalline silicon nano film is also larger (5 mm x 5mm), so that the monocrystalline silicon nano film can be transferred to an electrode at a fixed point in a naked eye distinguishing mode, the actually required monocrystalline silicon nano film for forming the photoelectric detector is far smaller than the size of a square, and the monocrystalline silicon nano films at other places can be etched in an etching mode.
And S4, carrying out photoetching and developing on the monocrystalline silicon nano film transferred to the substrate to expose the monocrystalline silicon nano film outside the required area, and placing the sample into an ICP etching machine to etch the monocrystalline silicon nano film outside the required area.
And S5, after spin-coating a PMMA supporting layer on the monoatomic layer graphene grown on the copper foil substrate by CVD, etching the copper foil substrate, fishing up the monoatomic layer graphene from water at a fixed point by using the polyimide substrate through a wet transfer method, placing the monoatomic layer graphene at one end of a bottom layer metal interconnection wire at the other side, and forming a certain overlapping area with the etched monocrystalline silicon nano film.
1) And spin-coating a PMMA supporting layer on the surface of the copper foil attached with the CVD grown graphene, and heating and curing.
2) And (3) placing the copper foil covered with the PMMA supporting layer into a solution prepared from copper sulfate pentahydrate and hydrochloric acid, and etching off the copper foil substrate.
3) After the copper foil substrate is completely etched, the monoatomic layer graphene is attached to the surface of the PMMA supporting layer and floats on the solution.
4) And (3) fishing out the PMMA attached with the graphene by using a glass slide, putting the PMMA in deionized water, standing for a period of time, fishing out the PMMA, putting the PMMA in new deionized water, repeating the steps for several times, and rinsing the graphene.
5) The graphene was site-transferred to the other electrode with a polyimide substrate attached to a glass substrate.
And S6, washing off the PMMA supporting layer on the surface of the graphene transferred to the substrate, photoetching and developing to expose the graphene outside the required area, and etching the exposed graphene with the monoatomic layer by using an ICP etching machine.
S7: repeating the process steps of S3-S6 three times to prepare a three-layer monocrystalline silicon nano-film/graphene photoelectric detector;
s8: carrying out photoetching and developing processes on the substrate again to form a top metal interconnection wire pattern;
s9: putting the sample into an electron beam evaporation device, and evaporating a layer of metal by using an electron beam evaporation process, wherein the electron beam evaporation process is Au 300 nm. And sequentially putting the substrate subjected to metal evaporation into acetone and isopropanol solutions to wash away the residual photoresist to form a top metal interconnection wire, and then putting the top metal interconnection wire into deionized water to clean.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and although the invention has been described in detail with reference to the foregoing examples, it will be apparent to those skilled in the art that various changes in the form and details of the embodiments may be made and equivalents may be substituted for elements thereof. All modifications, equivalents and the like which come within the spirit and principle of the invention are intended to be included within the scope of the invention.
Claims (10)
1. A multilayer monocrystalline silicon nanometer membrane/graphite alkene photoelectric detector which characterized in that: the single-crystal silicon/graphene Schottky heterojunction is formed by alternately stacking the single-crystal silicon nano films and the graphene to form a plurality of layers of single-crystal silicon nano films and a plurality of layers of graphene, an overlapped area is arranged between each layer of single-crystal silicon nano film and the graphene contacted with the upper surface and the lower surface of each layer of single-crystal silicon nano film to respectively form a single-crystal silicon/graphene Schottky heterojunction, and signals generated at the Schottky heterojunction are respectively led out through the bottom-layer metal interconnection lead and the top-layer metal interconnection lead.
2. The multilayer monocrystalline silicon nanomembrane/graphene photodetector of claim 1, wherein the monocrystalline silicon nanomembrane film has a thickness of 100nm to 300nm, the bottom metal interconnection wire has a thickness of 30nm to 100nm, and the top metal interconnection wire has a thickness of 300nm to 500 nm.
3. The multilayer single-crystal silicon nanomembrane/graphene photodetector of claim 1, wherein the single-crystal silicon nanomembrane is exfoliated from silicon-on-insulator and is a porous structure.
4. The multilayer single crystalline silicon nanomembrane/graphene photodetector of claim 1, wherein the single crystalline silicon nanomembrane is transferred to the metal contact electrode on the substrate by a wet transfer method.
5. The multilayer monocrystalline silicon nanomembrane/graphene photodetector of claim 1, wherein the number of monocrystalline silicon nanomembranes is 3, and the number of graphene layers is 3.
6. A method for preparing a photodetector according to claim 1, characterized in that it comprises in particular the following steps:
s1, photoetching and developing the bottom layer metal interconnection wire pattern on the substrate;
s2, evaporating metal by an electron beam, and washing away photoresist to form a bottom layer metal interconnection lead;
s3, transferring the square monocrystalline silicon nano film which is peeled from the SOI and floats on the water surface to one end of the substrate bottom layer metal interconnection wire by a wet transfer method;
s4, photoetching and developing the monocrystalline silicon nano film pattern, and etching the exposed monocrystalline silicon;
s5, transferring the graphene to one end of the metal interconnection wire at the other bottom layer of the substrate;
s6, photoetching and developing the graphene pattern, and etching the exposed graphene;
s7: repeating the steps S3-S6;
s8: photoetching and developing the top layer interconnection wire pattern;
s9: and evaporating metal by an electron beam, and washing away the photoresist to form a top metal interconnection wire.
7. The method of claim 6, wherein the substrate material is polyimide.
8. The method of claim 6, wherein the bottom metal interconnection is made of Cr and Au, and the evaporation of the electron beam in S2 is performed by first evaporating Cr and then evaporating Au.
9. The method of claim 6, wherein the top metal interconnection is made of Au.
10. The method for manufacturing a photodetector as claimed in claim 6, wherein the repetition number of the step S7 is 3.
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