CN113990739A - Transfer printing method of gallium oxide epitaxial layer based on Van der Waals film - Google Patents

Transfer printing method of gallium oxide epitaxial layer based on Van der Waals film Download PDF

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CN113990739A
CN113990739A CN202111244194.6A CN202111244194A CN113990739A CN 113990739 A CN113990739 A CN 113990739A CN 202111244194 A CN202111244194 A CN 202111244194A CN 113990739 A CN113990739 A CN 113990739A
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graphene
pmma
gallium oxide
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sapphire substrate
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宁静
陈丹妮
王东
张进成
马佩军
郝跃
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Xidian University
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Abstract

The invention discloses a transfer printing method of a gallium oxide epitaxial layer based on a Van der Waals film, which mainly solves the problems of complex stripping technology, high cost and low quality of a stripped gallium oxide epitaxial layer in the prior art. The implementation scheme is as follows: firstly, preparing a polycrystalline continuous graphene film on a polished copper foil by adopting a chemical vapor deposition method; then, transferring the graphene film onto a sapphire substrate; growing a gallium oxide epitaxial layer on the graphene film/sapphire substrate by using a pulse laser deposition method; and finally, peeling and transferring the grown gallium oxide epitaxial layer to a target substrate by using a heat release adhesive tape. According to the invention, the stress generated between the substrate and the epitaxial layer due to lattice mismatch is relieved through the graphene, and the epitaxial layer is easily peeled off and transferred to a target substrate through weak van der Waals force existing between the epitaxial layer and the graphene, so that the method can be used for realizing the reutilization of an original substrate or manufacturing a gallium oxide self-supporting substrate and a flexible device.

Description

Transfer printing method of gallium oxide epitaxial layer based on Van der Waals film
Technical Field
The invention belongs to the technical field of microelectronics, and further relates to a transfer printing method of a gallium oxide epitaxial layer, which can be used for manufacturing a gallium oxide electronic device.
Background
The third generation wide bandgap semiconductor material has wide application in the fields of photoelectric devices, electronic devices and the like due to the advantages of large forbidden band width, high electron mobility, large breakdown electric field and the like. The gallium oxide is a new generation semiconductor material for manufacturing high-performance semiconductor devices such as ultrahigh-voltage power devices, deep ultraviolet electronic devices, high-brightness LEDs and the like after the silicon carbide and the gallium nitride. In the conventional mainstream process, the methods for gallium oxide epitaxial layer generally include the following methods: molecular beam epitaxy, pulsed laser deposition, metallorganic chemical vapor deposition, magnetron sputtering, and the like. In the experiment, a metal organic chemical vapor deposition method is usually adopted to prepare heteroepitaxial gallium oxide on a c-plane sapphire or SiC substrate. However, there are serious lattice mismatch and thermal mismatch between the substrate and the gallium oxide, so that the gallium oxide obtained by heteroepitaxy is easy to generate large stress and form high-density dislocations during the growth process, and the dislocations have a serious influence on the performance and reliability of the gallium oxide-based device. Currently, with the development of wearable technology, the flexible semiconductor technology will gradually become the mainstream in the future, and the preparation of flexible high-quality gallium oxide becomes a hot spot. Therefore, the gallium oxide epitaxial layer peeling transfer technology with low dislocation density has great significance for developing flexible devices.
The existing stripping method of the gallium oxide epitaxial layer is generally mechanical grinding or laser stripping, and for the SiC substrate, the substrate cannot be recycled after mechanical grinding, so that the cost of the substrate is high, and the cost is extremely high. For sapphire substrates, because of their high hardness, large amounts of diamond grit are consumed, resulting in high cost and extremely slow speed. The principle of laser lift-off is that laser passes through the sapphire substrate to reach the gallium oxide epitaxial layer, and a local explosion shock wave is generated at the contact surface, so that the gallium oxide epitaxial layer at the contact surface is separated from the sapphire substrate. The laser stripping method has the advantages of short time and recycle of sapphire and a substrate, but has the defect that the periphery of the gallium oxide epitaxial layer is cracked when the gallium oxide epitaxial layer at a decomposition interface is stripped by laser, so that the gallium oxide epitaxial layer with large area and continuity and no damage can be obtained.
Disclosure of Invention
The invention aims to provide a stripping method of a gallium oxide epitaxial layer on a polycrystalline continuous graphene film aiming at the defects of the prior art, which improves the stripping efficiency and realizes complete stripping transfer of the gallium oxide epitaxial layer through weak van der waals force between graphene and the epitaxial layer.
In order to achieve the purpose, the technical scheme of the invention comprises the following steps:
(1) manufacturing a polycrystalline continuous graphene film by adopting a chemical vapor deposition method, and transferring the polycrystalline continuous graphene film onto a sapphire substrate;
(2) directly extending gallium oxide on the graphene film by adopting a pulse laser deposition method;
(3) adhering the heat-release adhesive tape on the upper surface of the gallium oxide epitaxial layer, and completely stripping the adhesive tape adhered with the gallium oxide epitaxial layer from the original substrate by uniform force, so that the side of the heat-release adhesive tape adhered with the gallium oxide is tightly attached to the target substrate;
(4) and placing the target substrate on a heating table heated to the temperature of 120-150 ℃ until the heat release adhesive tape loses viscosity after foaming, and automatically separating the adhesive tape from the surface of the gallium oxide to obtain the gallium oxide epitaxial layer transferred to the target substrate.
Compared with the prior art, the invention has the following advantages:
firstly, the graphene film is adopted as the insertion layer, and as the graphene is a two-dimensional material with a hexagonal honeycomb lattice structure consisting of carbon atoms, the gallium oxide epitaxial layer can be quickly peeled and transferred to any target substrate by utilizing weak van der waals force between the graphene and the gallium oxide epitaxial layer, so that the reuse of the original substrate can be realized, the cost is saved, the gallium oxide epitaxial layer can be transferred to the flexible substrate, and the preparation of a flexible device or the preparation of a gallium oxide self-supporting substrate can be realized.
Secondly, the physical stripping of the gallium oxide epitaxial layer is carried out by using the heat release adhesive tape, compared with the traditional laser stripping mode, the operation is simpler, the stripping efficiency is improved, the stripping cost is reduced, and the damage degree to the sample is also reduced.
Thirdly, as the graphene film is transferred to the sapphire substrate by the wet method and then the gallium oxide epitaxial layer is grown, the stress generated by lattice mismatch between the substrate and the epitaxial layer is relieved, and the quality of the grown gallium oxide epitaxial layer is improved.
Drawings
FIG. 1 is a flow chart of an implementation of the present invention;
FIG. 2 is a schematic cross-sectional view of a material before peel-off transfer in accordance with the present invention;
FIG. 3 is a schematic cross-sectional view of the material after peeling and transferring in the present invention.
Detailed Description
Embodiments of the present invention will be described in further detail below with reference to the accompanying drawings.
Referring to fig. 1, the present invention is given as follows in three embodiments.
Example 1a 1um thick epitaxial layer of gallium oxide was transferred onto a silicon substrate using a double layer graphene film.
Step 1, growing graphene on the copper foil by adopting a Chemical Vapor Deposition (CVD) method.
1.1) folding the polished copper foil into a pouch with a proper size, putting the pouch into a quartz boat, pushing the quartz boat to a central constant-temperature area of a quartz tube, and opening a vacuum pump to vacuumize to 1 Pa;
1.2) feeding 20sccm of H into the quartz tube2Heating the quartz tube to 700 deg.C, and introducing 20sccm H into the quartz tube2And Ar of 700sccm, and continuing heating until the temperature of the quartz tube reaches 1050 ℃;
1.3) keeping the temperature unchanged, closing all air inlet valves, and pumping the air pressure in the quartz tube to 1Pa by using a vacuum pump;
1.4) keeping the temperature constant, and introducing O of 2sccm into the quartz tube2Maintaining for 2 min;
1.5) keeping the temperature unchanged, closing all air inlet valves, and pumping the quartz tube to 1Pa by using a vacuum pump;
1.6) the temperature is kept constant while introducing 100sccm of H2And 700sccm of Ar for 60 min;
1.7) keeping the temperature constant, closing the Ar valve and simultaneously introducing CH of 1sccm4And 500sccm of H2Maintaining for 60 min;
1.8) Retention of H2And CH4And (3) rapidly cooling the quartz tube to room temperature without changing the flow, and growing the single-layer graphene with the thickness of 0.34nm on the copper foil.
And 2, transferring the double-layer graphene to the sapphire substrate.
2.1) manually coating a layer of polymethyl methacrylate (PMMA) film on the surface of the copper foil with the graphene, and uniformly spin-coating PMMA by using a spin coater, namely setting the rotation speed of the spin coater as low speed of 1000 revolutions per second for 30 seconds, and then increasing the rotation speed to 3000 revolutions per second for 60 seconds to obtain the copper foil with the PMMA subjected to spin coating;
2.2) placing the copper foil coated with PMMA in a spin coating manner on a heating table, setting the temperature of the heating table to be 50 ℃, and drying for 20min to solidify the PMMA film;
2.3) cutting the copper foil with the solidified PMMA into two small pieces with the same size, placing the small pieces in a 64g/L ammonium persulfate solution, enabling one surface of the graphene to face upwards, soaking for 8 hours, and removing the metal substrate to obtain two single-layer graphene films with the PMMA;
2.4) transferring PMMA/graphene in two pieces of ammonium persulfate solution into deionized water by using a clean glass sheet, soaking for 30min, and fishing out one small piece of PMMA/single-layer graphene by using the sapphire substrate to obtain the sapphire substrate covering PMMA/single-layer graphene;
2.5) adding 100ml of acetone solution into a glass container, completely submerging the PMMA/single-layer graphene/sapphire substrate, and soaking for 12 hours to dissolve and fully remove PMMA, so as to obtain the single-layer graphene/sapphire substrate with the PMMA removed;
2.6) transferring the single-layer graphene/sapphire substrate without PMMA from the acetone solution to an ethanol solution for standing for 30min, then fishing out the single-layer graphene/sapphire substrate, and naturally airing to finish the transfer of the single-layer graphene;
2.7) using the sapphire substrate of the single-layer graphene obtained in the step 2.4), and then fishing out a second PMMA/single-layer graphene film placed in deionized water to obtain a sapphire substrate covering PMMA/double-layer graphene;
2.8) repeating the structure of 2.7) by 2.5) -2.6), removing the polymethyl methacrylate (PMMA) covered on the graphene, and finishing the transfer of the second layer of graphene to obtain the double-layer graphene/sapphire substrate.
And 3, growing a gallium oxide epitaxial layer with the thickness of 1um on the double-layer graphene/sapphire substrate by a pulse laser deposition method.
3.1) placing the sapphire substrate transferred with the graphene into a reaction chamber, raising the temperature of the reaction chamber to 800 ℃, and adjusting the pressure of the reaction chamber to 10 DEG-8Torr;
3.2) keeping the temperature of the reaction chamber unchanged, and introducing oxygen to maintain the pressure of the reaction chamber at 5 mTorr;
3.3) Using sintered beta-Ga2O3The pellet is used as a target material, excimer laser beams with the wavelength of 248nm are used for irradiating after being focused, and the distance between the gallium oxide target material and the substrate is set to be 80 mm;
3.4) setting the repetition frequency of the laser pulse to be 5Hz, setting the energy of each pulse to be 300mJ, and depositing a gallium oxide epitaxial layer on the double-layer graphene/sapphire substrate by using 20000 repeated laser pulses;
3.5) taking out the sample after the temperature of the reaction chamber is reduced to the room temperature, and obtaining the gallium oxide epitaxial layer with the thickness of 1um which grows on the double-layer graphene/sapphire substrate, as shown in figure 2.
And 4, transferring the gallium oxide epitaxial layer with the thickness of 1um to the silicon substrate.
4.1) slowly adhering the heat release adhesive tape on the upper surface of the gallium oxide epitaxial layer, and completely stripping the adhesive tape adhered with the gallium oxide epitaxial layer from the original substrate by uniform force;
4.2) tightly attaching the surface of the heat release adhesive tape, which is adhered with the gallium oxide, to the silicon substrate, heating the heating table to 120 ℃, and then integrally placing the target substrate on the heating table until the heat release adhesive tape loses viscosity after foaming, so that the adhesive tape can automatically separate from the surface of the gallium nitride;
and 4.3) removing the stripped adhesive tape by using tweezers or other tools to enable the gallium oxide epitaxial layer to remain on the silicon substrate, thereby realizing the stripping transfer of the gallium oxide epitaxial layer, as shown in FIG. 3.
Example 2a gallium oxide epitaxial layer 2um thick was transferred onto a polyethylene terephthalate PET flexible substrate using a four layer graphene film.
And step A, growing graphene on the copper foil by adopting a chemical vapor deposition CVD method.
The specific implementation of this step is the same as step 1 in example 1.
And B, transferring four layers of graphene to the sapphire substrate.
B1) Spin-coating and curing PMMA on the surface of the copper foil with the graphene:
the specific implementation of this step is the same as steps 2.1) -2.2) in example 1;
B2) cutting the copper foil with the solidified PMMA into four small pieces with the same size, placing the small pieces in a 64g/L ammonium persulfate solution, enabling one surface of the graphene to face upwards, soaking for 8 hours, and removing a metal substrate to obtain four single-layer graphene films with the PMMA;
B3) transfer of single layer graphene onto sapphire substrate and dissolution of PMMA:
the specific implementation of this step is the same as steps 2.4) -2.6) in example 1;
B4) fishing a second PMMA/single-layer graphene film by using the sapphire substrate transferred with the single-layer graphene to obtain a substrate covering PMMA/double-layer graphene, and repeating B3) to complete the transfer of the second-layer graphene to obtain the sapphire substrate transferred with the double-layer graphene; then fishing a third layer of graphene by using the sapphire substrate transferred with the double-layer graphene, and repeating B3), thereby completing the transfer of the third layer of graphene and obtaining the sapphire substrate transferred with the three layers of graphene; and fishing a fourth layer of graphene by using the sapphire substrate transferred with the three layers of graphene, and repeating B3) to obtain the sapphire substrate transferred with the four layers of graphene.
And C, growing a gallium oxide epitaxial layer with the thickness of 2um on the four-layer graphene/sapphire substrate by a pulse laser deposition method.
C1) Placing the patterned sapphire substrate covered with graphene into a reaction chamber, raising the temperature of the reaction chamber to 850 ℃, and adjusting the pressure of the reaction chamber to 10 DEG-8Torr;
C2) Keeping the temperature of the reaction chamber unchanged, introducing oxygen and keeping the pressure of the reaction chamber at 6 mTorr;
C3) by means of sintered beta-Ga2O3The pellet is used as a target material, excimer laser beams with the wavelength of 248nm are used for irradiating after being focused, and the distance between the gallium oxide target material and the substrate is kept at 90 mm;
C4) setting the repetition frequency of laser pulses to be 5Hz, setting the energy of each pulse to be 300mJ, and depositing a gallium oxide epitaxial layer on a four-layer graphene/sapphire substrate by utilizing 25000 repeated laser pulses;
C5) and (3) cooling the temperature of the reaction chamber to room temperature, and taking out a sample to obtain a gallium oxide epitaxial layer with the thickness of 2um, which grows on the four-layer graphene/sapphire substrate, as shown in figure 2.
And D, transferring the gallium oxide epitaxial layer with the thickness of 2um to a polyethylene terephthalate (PET) flexible substrate.
D1) Slowly adhering the heat release adhesive tape on the upper surface of the gallium oxide epitaxial layer, and completely stripping the adhesive tape adhered with the gallium oxide epitaxial layer from the original substrate by uniform force;
D2) one surface of the heat release adhesive tape, which is adhered with the gallium oxide, is tightly attached to a polyethylene terephthalate (PET) flexible substrate, the heating table is heated to 130 ℃, then the target substrate is integrally placed on the heating table until the heat release adhesive tape loses viscosity after foaming, and the adhesive tape can automatically separate from the surface of the gallium oxide;
D3) and (3) taking off the stripped adhesive tape by using tweezers or other tools, and leaving the gallium oxide epitaxial layer on the polyethylene terephthalate PET flexible substrate to realize the stripping transfer of the gallium oxide epitaxial layer, as shown in figure 3.
Example 3a gallium oxide epitaxial layer 3um thick was transferred onto a diamond substrate using a six-layer graphene film.
Growing graphene on the copper foil by adopting a Chemical Vapor Deposition (CVD) method.
The specific implementation of this step is the same as step 1 in example 1.
Transferring six layers of graphene on the sapphire substrate:
2a) spin-coating and curing PMMA on the surface of the copper foil with the graphene:
the specific implementation of this step is the same as steps 2.1) -2.2) in example 1;
2b) cutting the copper foil with the solidified PMMA into six small pieces with the same size, placing the small pieces in a 64g/L ammonium persulfate solution, enabling one surface of the graphene to face upwards, soaking for 8 hours, and removing a metal substrate to obtain six single-layer graphene films with the PMMA;
2c) transfer of single layer graphene onto sapphire substrate and dissolution of PMMA:
the specific implementation of this step is the same as steps 2.4) -2.6) in example 1;
2d) preparing a six-layer graphene/sapphire substrate:
fishing a second PMMA/single-layer graphene film by using the sapphire substrate transferred with the single-layer graphene to obtain a substrate covering PMMA/double-layer graphene, and repeating the step 2c) to finish the transfer of the second-layer graphene to obtain the sapphire substrate transferred with the double-layer graphene;
fishing a third layer of graphene by using the sapphire substrate transferred with the double-layer graphene, and repeating the step 2c) to finish the transfer of the third layer of graphene to obtain the sapphire substrate transferred with the three layers of graphene;
fishing a fourth layer of graphene by using the sapphire substrate transferred with the three layers of graphene, and repeating the step 2c) to obtain the sapphire substrate transferred with the four layers of graphene;
fishing a fifth layer of graphene by using the sapphire substrate transferred with the four layers of graphene, and repeating the step 2c) to obtain the sapphire substrate transferred with the five layers of graphene;
fishing a sixth layer of graphene from the sapphire substrate transferred with the five layers of graphene, and repeating the step 2c) to obtain the sapphire substrate transferred with the six layers of graphene;
and step three, growing a gallium oxide epitaxial layer with the thickness of 3um on the six-layer graphene/sapphire substrate by a pulse laser deposition method.
3a) Placing a six-layer graphene/sapphire substrate in a reaction chamber, raising the temperature of the reaction chamber to 900 ℃, and adjusting the pressure of the reaction chamber to 10 DEG C-8Torr;
3b) Keeping the temperature of the reaction chamber unchanged, introducing oxygen and keeping the pressure of the reaction chamber at 7 mTorr;
3c) by means of sintered beta-Ga2O3The pellet is used as a target material, excimer laser beams with the wavelength of 248nm are used for irradiating after being focused, and the distance between the gallium oxide target material and the substrate is kept at 100 mm;
3d) setting the repetition frequency of laser pulses to be 5Hz, setting the energy of each pulse to be 300mJ, and depositing a gallium oxide epitaxial layer on a six-layer graphene/sapphire substrate by using 30000 repeated laser pulses;
3e) and (3) cooling the temperature of the reaction chamber to room temperature, and taking out a sample to obtain a gallium oxide epitaxial layer with the thickness of 3um, which grows on the six-layer graphene/sapphire substrate, as shown in figure 2.
And step four, transferring the gallium oxide epitaxial layer with the thickness of 3um to the diamond substrate.
4a) Slowly adhering the heat release adhesive tape on the upper surface of the gallium oxide epitaxial layer, and completely stripping the adhesive tape adhered with the gallium oxide epitaxial layer from the original substrate by uniform force;
4b) tightly attaching the surface of the heat release adhesive tape, which is adhered with the gallium oxide, to the diamond substrate, heating the heating table to 150 ℃, and then integrally placing the target substrate on the heating table until the heat release adhesive tape loses viscosity after foaming, so that the adhesive tape can automatically separate from the surface of the gallium oxide;
4c) and (3) taking off the stripped adhesive tape by using tweezers or other tools, and leaving the gallium oxide epitaxial layer on the diamond substrate to realize the stripping transfer of the gallium oxide epitaxial layer, as shown in figure 3.
The foregoing description is only three specific examples of the present invention and is not intended to limit the invention, so that it will be apparent to those skilled in the art that various changes and modifications in form and detail may be made therein without departing from the spirit and scope of the invention.

Claims (7)

1. A transfer printing method of gallium oxide epitaxial layer based on Van der Waals film is characterized by comprising the following steps:
(1) manufacturing a polycrystalline continuous graphene film by adopting a chemical vapor deposition method, and transferring the polycrystalline continuous graphene film onto a sapphire substrate;
(2) directly extending gallium oxide on the graphene film by adopting a pulse laser deposition method;
(3) adhering the heat-release adhesive tape on the upper surface of the gallium oxide epitaxial layer, and completely stripping the adhesive tape adhered with the gallium oxide epitaxial layer from the original substrate by uniform force, so that the side of the heat-release adhesive tape adhered with the gallium oxide is tightly attached to the target substrate;
(4) and placing the whole target substrate on a heating table heated to the temperature of 120-150 ℃ until the heat release adhesive tape loses viscosity after foaming, and the adhesive tape can automatically separate from the surface of the gallium oxide.
2. The method according to claim 1, wherein the chemical vapor deposition method for preparing the single-layer polycrystalline continuous graphene thin film in (1) is implemented as follows:
(1a) folding the copper foil which is subjected to electrochemical polishing into a pouch with a proper size, putting the pouch into a quartz boat, pushing the quartz boat to a central constant-temperature area of a quartz tube, and opening a vacuum pump to vacuumize to 0.9-2 Pa;
(1b) introducing H of 20sccm into a quartz tube2Heating the quartz tube to 700 deg.C, and introducing 20sccm H into the quartz tube2And Ar of 700sccm, and continuing heating until the temperature of the quartz tube reaches 1045 ℃;
(1c) keeping the temperature unchanged, stopping all ventilation, and pumping the air pressure in the quartz tube to 0.9-1Pa by using a vacuum pump;
(1d) keeping the temperature constant, and introducing O of 2sccm into the quartz tube2Maintaining for 2 min;
(1e) keeping the temperature unchanged, stopping all ventilation, and pumping the quartz tube to 0.9-1Pa by using a vacuum pump;
(1f) while keeping the temperature constant, introducing 100sccm of H2And 700sccm of Ar for 60 min;
(1g) the temperature was kept constant, all aeration was stopped, and 1sccm of CH was added simultaneously4And 500sccm of H2Maintaining for 60 min;
(1h) stopping all ventilation, introducing Ar of 700sccm, and quickly cooling the quartz tube to room temperature to obtain the single-layer polycrystalline continuous graphene film growing on the copper foil.
3. The method of claim 1, wherein the transferring of the polycrystalline continuous graphene thin film onto the sapphire substrate in (1) is carried out as follows:
(1i) manually coating a layer of polymethyl methacrylate (PMMA) film on the surface of the copper foil on which the graphene grows by using a plastic suction pipe, and uniformly spin-coating PMMA by using a spin coater to obtain the copper foil on which PMMA is spin-coated;
(1j) placing the copper foil coated with PMMA on a heating table, setting the temperature of the heating table to be 50-60 ℃, and baking for 20-30min to cure the PMMA film;
(1k) cutting the copper foil with the solidified PMMA into 2-8 small pieces with the same size, placing the small pieces in 68g/L ammonium persulfate solution, enabling one surface of the copper foil covered with the graphene to face upwards, soaking for 4-8 hours, and removing the metal substrate to obtain a plurality of single-layer polycrystalline continuous graphene thin films covered with the PMMA;
(1l) transferring PMMA/single-layer polycrystalline graphene in a plurality of pieces of ammonium persulfate solution into deionized water by using a clean glass slide, soaking for 10-30min, and fishing out one piece of PMMA/single-layer polycrystalline graphene by using a sapphire substrate to obtain the sapphire substrate covering PMMA/single-layer polycrystalline graphene;
(1m) adding 100-200ml of acetone solution into a glass container, completely submerging the PMMA/single-layer polycrystalline graphene/sapphire substrate, and soaking for 12-24 hours to dissolve and fully remove PMMA, so as to obtain the single-layer polycrystalline graphene/sapphire substrate with PMMA removed;
(1n) transferring the single-layer polycrystalline graphene/sapphire substrate without PMMA from the acetone solution to an ethanol solution, standing for 10-30min, taking out the single-layer polycrystalline graphene/sapphire substrate, and naturally airing to finish the transfer of the single-layer polycrystalline graphene film;
(1o) using the single-layer polycrystalline graphene/sapphire substrate obtained in the step (1n) and then fishing a second PMMA/single-layer graphene film placed in deionized water to obtain a covered PMMA/double-layer polycrystalline graphene/sapphire substrate;
(1p) adding 100-200ml of acetone solution into a glass container to completely submerge the PMMA/double-layer polycrystalline graphene/sapphire substrate, and soaking for 12-24 hours to dissolve the PMMA/double-layer polycrystalline graphene/sapphire substrate to obtain the double-layer polycrystalline graphene/sapphire substrate with PMMA removed; transferring the PMMA-removed double-layer polycrystalline graphene/sapphire substrate from the acetone solution to an ethanol solution, standing for 10-30min, taking out the double-layer polycrystalline graphene/sapphire substrate, and naturally airing to finish the transfer of the double-layer polycrystalline graphene film;
(1q) repeating (1o) - (1p) for the structure of (1n), so that a multilayer polycrystalline graphene/sapphire substrate can be obtained, and the transfer of the multilayer polycrystalline graphene film is completed.
4. The method of claim 1, wherein the epitaxial growth of gallium oxide directly on the multilayer graphene film using pulsed laser deposition as described in (2) is achieved by:
(2a) placing the sapphire substrate with the transferred graphene film on a reaction chamber substrate, raising the temperature of the reaction chamber to 800-850 ℃, and adjusting the pressure of the reaction chamber to 10-8-10-9Torr;
(2b) Keeping the temperature of the reaction chamber unchanged, introducing oxygen and keeping the pressure of the reaction chamber at 5-7 mTorr;
(2c) by means of sintered beta-Ga2O3The small ball is used as a target material, and is focused by an excimer laser beam with the wavelength of 248nmIrradiating, and keeping the distance between the gallium oxide target material and the substrate at 80-90 mm;
(2d) setting the repetition frequency of laser pulses to be 5Hz, setting the energy of each pulse to be 300mJ, and depositing a gallium oxide epitaxial layer on the sapphire substrate transferred with the graphene film by utilizing 25000 repeated laser pulses;
(2e) and cooling the temperature of the reaction chamber to room temperature, and taking out the sample to obtain the gallium oxide epitaxial layer growing on the graphene film.
5. The method according to claim 3, wherein the spin coating of PMMA is performed uniformly by the spin coater in (1i), by adjusting the rotation speed of the spin coater, i.e. the rotation speed of the spin coater is set to be a low rotation speed of 1000 rpm for 10s, and then the rotation speed is increased to 3000 rpm for 60 s.
6. The method according to claim 1, wherein the sapphire substrate in (1) has a thickness of 0.43-0.5 mm.
7. The method of claim 1, wherein the target substrate in (3) is one of a silicon substrate, a polyethylene terephthalate (PET) flexible substrate, and a diamond substrate.
CN202111244194.6A 2021-10-26 2021-10-26 Transfer printing method of gallium oxide epitaxial layer based on Van der Waals film Pending CN113990739A (en)

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CN113394306A (en) * 2021-05-18 2021-09-14 浙江大学 Reusable ZnO single crystal substrate based on graphene and method for preparing ZnO film
CN115161775A (en) * 2022-07-01 2022-10-11 常州第六元素半导体有限公司 Transfer method of graphene film
CN115418718A (en) * 2022-09-07 2022-12-02 武汉大学 Product based on two-dimensional spinel type ferrite film and preparation method and application thereof

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113394306A (en) * 2021-05-18 2021-09-14 浙江大学 Reusable ZnO single crystal substrate based on graphene and method for preparing ZnO film
CN115161775A (en) * 2022-07-01 2022-10-11 常州第六元素半导体有限公司 Transfer method of graphene film
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