CN116043317A - Method for regulating and controlling structure and defects of two-dimensional lamellar Van der Waals material and application thereof - Google Patents

Method for regulating and controlling structure and defects of two-dimensional lamellar Van der Waals material and application thereof Download PDF

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CN116043317A
CN116043317A CN202211729460.9A CN202211729460A CN116043317A CN 116043317 A CN116043317 A CN 116043317A CN 202211729460 A CN202211729460 A CN 202211729460A CN 116043317 A CN116043317 A CN 116043317A
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隋峰锐
齐瑞娟
金敏
吕志伟
吴宇宁
越方禹
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East China Normal University
Shanghai Dianji University
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Abstract

The invention discloses a method for regulating and controlling the structure and defects of a two-dimensional layered van der Waals material and application thereof, wherein the method takes doping of lanthanide rare earth elements such as yttrium (Y), dysprosium (Dy) and the like as a means to regulate and control the structure and defects of the two-dimensional layered van der Waals material indium selenide (InSe), so that the structure of the material is effectively optimized, the interlayer acting force of the material is improved, and the generation of intrinsic faults in the material is obviously inhibited. By doping rare earth elements, excellent ferroelectric properties of Gamma (Gamma/Gamma) InSe are discovered for the first time; the material has no deep energy level defect, has excellent electrical property and moderate and adjustable direct band gap (the band gap is equivalent to Si), and the spectral response of the material covers the characteristics of near infrared to ultraviolet range and the like; the material has great application prospect in the field of two-dimensional ferroelectric photovoltaics.

Description

Method for regulating and controlling structure and defects of two-dimensional lamellar Van der Waals material and application thereof
Technical Field
The invention relates to a two-dimensional semiconductor InSe material technology, in particular to a method for regulating and controlling the structure and defects of a two-dimensional layered van der Waals material and application thereof.
Background
Conventional photovoltaic devices rely extensively on interface technology in solids, just like semiconductor PN junctions or schottky junctions, but the number of photons available and the photovoltaic voltage produced by them during photoelectric conversion is limited by the bandgap of the crystalline material. The theory proves that the photoelectric energy conversion efficiency of these devices is limited in theory, the so-called Shockley-Queisser limit. Recent studies have shown that nonlinear optical phenomena known as the bulk photovoltaic effect are prevalent in non-centrosymmetric crystalline materials. At present, the research of the bulk photovoltaic effect is mainly focused on three-dimensional ferroelectric crystals mainly comprising perovskite oxides, and is limited by the thickness and insulator properties of bulk materials, and photocurrent generated by using the bulk photovoltaic effect is usually small.
Two-dimensional materials are closely focused due to their unique material structure and electron transport properties, and are widely used in a variety of fields such as photoelectric devices, catalysts, and biosensors. The two-dimensional material has a sheet structure, and the thickness can reach a single or a few atoms, and is not limited by the thickness and the insulating property of the bulk material. Since the discovery of graphene in 2004, the design dimension of semiconductor electronic and optoelectronic devices is greatly widened by virtue of the abundant band gap structure, unique photoelectric characteristics, van der Waals surfaces without dangling bonds and the like of the two-dimensional material. The two-dimensional indium selenide (InSe) material is taken as a typical III-VI two-dimensional semiconductor material, has excellent electrical property and moderate and adjustable direct band gap (the band gap is equivalent to Si and is a direct band gap semiconductor), and the spectral response covers the range from near infrared to ultraviolet; the candidate material for the future high-mobility optoelectronic devices which is the most competitive is considered as the golden division point of silicon and graphene by the Norbeol prize acquirer Andre Geim. Theoretical calculation shows that the two-dimensional semiconductor InSe has no deep energy level defect (which can be compared with the most-fire organic-inorganic hybrid perovskite material in the photovoltaic field at present), so that the material has great potential in the photovoltaic field. However, due to a large number of naturally-formed stacking faults in the material, the separation and transmission of carriers of the material can be greatly influenced, and the application of the material in the photovoltaic field is greatly limited.
Disclosure of Invention
In view of the above, the invention discloses a preparation method of a two-dimensional ferroelectric photovoltaic and photoelectric detection material based on rare earth element doping defect regulation, which uses lanthanoid elements such as yttrium element, dysprosium element and the like as means to carry out structure and defect regulation on a two-dimensional material InSe, and popularizes the application of the two-dimensional material InSe in the field of ferroelectric photovoltaic and photoelectric detection.
The technical scheme of the invention is as follows:
a method of modulating two-dimensional layered van der waals material structure and defects, the method comprising the steps of:
step 1: synthesizing an InSe polycrystal raw material doped with rare earth elements by adopting a swinging method in a vacuum state;
step 2: placing the synthesized polycrystalline raw material into a double-layer quartz crucible for vacuum treatment;
step 3: sealing the crucible in a vacuum state, and performing vacuum test and fixing the sealed crucible; after the test is normal, the crucible is placed on a down pipe in a hearth of a crystallization furnace, the bottom of the crucible is ensured to be level with a lower thermocouple, and the position of the crucible is fixed;
step 4: controlling the heating speed and the heat preservation time, and taking out after naturally cooling to room temperature when the raw materials completely pass through the growth area, so as to obtain grown crystals;
step 5: carrying out artificial mechanical stripping on the grown crystal;
step 6: mechanically stripping the grown single crystal sample to obtain a thin sheet sample with proper thickness, and testing the ferroelectricity and photovoltaic characteristics of the thin sheet sample;
wherein, the synthesis of the polycrystalline raw material in the step 1 comprises the following steps:
a1: drying In, se and rare earth elements with purity of 4N In an environment of 120 ℃ for 2 hours, and taking out for standby after naturally cooling to room temperature;
a2: according to the pre-designed stoichiometric ratio, accurately calculating the mass of the In element and the rare earth element, weighing, and controlling the weighing precision within a range of +/-0.001 g;
a3: premixing the weighed In element and rare earth element, putting the premixed In element and rare earth element into a cleaned quartz crucible for vacuum treatment, and pumping the mixture at a vacuum pump pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A4: sealing the quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump; after the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a5: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a6: cooling the alloy of the In element and the rare earth element synthesized for the first time to room temperature and then taking out;
a7: calculating and weighing the polycrystalline raw material and Se element synthesized for the first time, placing into a cleaned quartz crucible for vacuum treatment, and pumping at a vacuum pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A8: sealing the double-layer quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump; after the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a9: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and the temperature is kept for 30min, then swinging the furnace for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a10: cooling the polycrystalline raw material synthesized for the second time to room temperature and taking out for standby;
in step 2, the pumping speed of the vacuum pump is 3.6m 3 ·h -1 Vacuumizing at this rate for 20-30min
In step 4, the controlling the heating rate and the heat preservation time specifically includes:
b1: adjusting the crucible to the position of a high-temperature region of a hearth, heating the crystallization furnace to 700 ℃ for 8 hours, and preserving the temperature of the rare earth doped InSe polycrystal raw material synthesized in the step 3 for 8 hours at 700 ℃;
b2: the descent apparatus is then operated at 0.5 mm.h -1 The speed of the InSe monocrystal is reduced, and the InSe monocrystal starts to grow when the temperature of the melt at the bottom is reduced below the melting point;
in step 6, the grown single crystal sample is mechanically stripped to obtain a slice sample with proper thickness, which is specifically as follows:
c1: placing a two-dimensional laminar material sheet to be peeled on a 3M transparent adhesive tape by adopting an adhesive tape peeling method; repeatedly pasting and peeling to change the film into a lamellar film with proper thickness; transferring the laminated sheet on the adhesive tape to a target substrate by using Polydimethylsiloxane (PDMS), slowly peeling off the PDMS after standing for a period of time, and leaving the material on the target substrate;
the two-dimensional layered van der Waals material prepared by the method is applied to the field of ferroelectric photovoltaics.
The invention has the beneficial effects that:
the invention discloses a method for regulating and controlling the structure and defects of a two-dimensional van der Waals layered material by element doping and application thereof in the field of ferroelectric photovoltaics, wherein the method takes actinide rare earth elements such as yttrium element, dysprosium element and the like as a means to regulate and control the structure and the defects of a narrow-band gap two-dimensional material InSe, the InSe structure after doping and controlling is greatly optimized, and intrinsic faults are effectively inhibited; the severe interface or in-vivo defect composite loss caused by the defects is avoided, and the photoelectric property of the material is greatly improved; in addition, the InSe material prepared by the method has unique ferroelectric property, so that the two-dimensional material semiconductor InSe becomes an ideal material in the application fields of ferroelectric photovoltaics and photoelectric detection. By the method disclosed by the patent, the direct band gap semiconductor InSe material equivalent to the Si band gap is expected to become the ferroelectric photovoltaic material with the highest potential of the new generation.
Drawings
FIG. 1 is a schematic diagram of a double-layered quartz crucible in step 2;
FIG. 2 is a schematic view of the in-plane structure and polarization direction of InSe mentioned in step 6;
FIG. 3 is a schematic view of the structure of the photovoltaic device in step 6;
FIG. 4 is a photograph of undoped InSe and Y-doped, dy-doped InSe single crystals in the examples;
FIG. 5 is a scanning electron microscope topography and transmission electron microscope cross-section of undoped and Y-doped Dy-doped single crystal InSe in an embodiment;
FIG. 6 is an atomic arrangement image of undoped and Y-doped Dy-doped single crystal InSe cross-section samples in the examples;
FIG. 7 is an optical microscope photograph of a sample of a Y-doped, dy-doped InSe thin layer obtained by mechanical exfoliation and the corresponding ferroelectric results in the examples;
FIG. 8 is a schematic diagram of a Y-doped single crystal InSe optoelectronic device and corresponding optical current spectra in an embodiment;
Detailed Description
The present invention will be described in detail with reference to specific examples.
Example 1
A method for regulating and controlling two-dimensional van der Waals layered material structure and defect by element doping and a method for growing InSe monocrystal by rare earth Y element doping Bridgman method are taken as an example in the field of ferroelectric photovoltaics, and the method comprises the following specific steps:
step 1: in synthesis under vacuum state by swing method 0.52 Se 0.48 Y 0.01 Polycrystalline raw material;
synthesis of In 0.52 Se 0.48 Y 0.01 The polycrystalline raw materials comprise:
a1: drying In, se and Y with purity of 4N In an environment of 120 ℃ for 2 hours, and taking out for standby after naturally cooling to room temperature;
a2: according to a pre-designed stoichiometric ratio In 0.52 Se 0.48 Y 0.01 Accurately calculating the mass of the In element and the mass of the Y element, weighing, and controlling the weighing precision within a range of +/-0.001 g;
a3: premixing the weighed In element and the weighed Y element, putting the premixed In element and the weighed Y element into a cleaned quartz crucible for vacuum treatment, wherein the pumping speed of a vacuum pump is 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A4: and (5) sealing the quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump. After the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a5: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a6: cooling the first synthesized InY alloy to room temperature and taking out;
a7: calculating and weighing the polycrystalline raw material and Se element synthesized for the first time, placing into a cleaned quartz crucible for vacuum treatment, and pumping at a vacuum pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A8: and (3) sealing the double-layer quartz crucible in a vacuum state (as shown in figure 1), and vacuumizing for 30min by a vacuum pump. After the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a9: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a10: cooling the polycrystalline raw material synthesized for the second time to room temperature and then taking out;
step 2: will synthesize good In 0.52 Se 0.48 Y 0.01 Placing the polycrystalline raw material into a double-layer quartz crucible (inner layer of phi 18mm and outer layer of phi 27 mm) for vacuum treatment, wherein the pumping speed of the vacuum pump is 3.6m 3 ·h -1 Vacuumizing for 30min at the speed;
step 3: and (3) sealing the crucible in a vacuum state, and carrying out vacuum test and fixing on the sealed crucible. After the test is normal, the crucible is placed on a down pipe in a hearth of a crystallization furnace, the bottom of the crucible is ensured to be level with a lower thermocouple, and the position of the crucible is fixed;
step 4: controlling the heating speed and the heat preservation time, and taking out after naturally cooling to room temperature when the raw materials completely pass through the growth area, so as to obtain grown crystals;
the control of the temperature rising speed and the heat preservation time specifically comprises the following steps:
b1: adjusting the crucible to the position of a high-temperature region of a hearth, heating the crystallization furnace to 700 ℃ for 8 hours, and preserving the temperature of the Y-doped InSe polycrystal raw material synthesized in the step 3 for 8 hours at 700 ℃;
b2: the descent apparatus is then operated at 0.5 mm.h -1 The speed of the InSe monocrystal is reduced, and the InSe monocrystal starts to grow when the temperature of the melt at the bottom is reduced below the melting point; the appearance of the obtained single crystal sample is shown in figure 4, and the scanning electron microscope image and the transmission electron microscope structural analysis image are shown in figures 5 and 6, so that the appearance of the InSe single crystal is greatly changed by rare earth Y element impurities, the appearance of the InSe single crystal is greatly reduced in the microstructure, and the interlayer acting force is enhanced.
Step 5: carrying out artificial mechanical stripping on the grown crystal, cutting and polishing a sample with a required size, and sealing and storing the prepared sample by using a vacuum bag;
step 6: mechanically stripping the grown single crystal sample to obtain a slice sample with proper thickness, and researching ferroelectric and photovoltaic characteristics of the slice sample;
mechanically stripping the grown single crystal sample to obtain a thin sheet sample with proper thickness, and researching ferroelectric and photovoltaic properties of the thin sheet sample, wherein the thin sheet sample is specifically as follows:
c1: the two-dimensional laminar material sheet to be peeled is peeled by tape peelingPlacing on a 3M transparent adhesive tape; repeatedly pasting and peeling to change the film into a lamellar film with proper thickness; the layered sheet on the tape was further transferred to a target Substrate (SiO) with Polydimethylsiloxane (PDMS) 2 (Si, etc.), slowly peeling off PDMS after standing for a period of time to leave the material on the target substrate;
c2: detecting a ferroelectric signal of a sample under an externally applied excitation voltage by using a piezoelectric power microscope (PFM), and verifying the ferroelectric property of the material (shown in figure 7);
c3, in view of the fact that gamma InSe with a non-inversion symmetry center has an armchair (armchair) in the plane, wherein the direction is in-plane polarization direction and Zigzag (Zigzag) two-atom arrangement, the armchair direction is further locked by adopting a Second Harmonic (SHG) means;
and C4: adopting a thermal evaporation method to evaporate gold-plating stages to a block or lamellar two-dimensional InSe material along the direction of the armchair; obtaining an in-plane photovoltaic device (as shown in fig. 8);
and C5, testing the photoelectric spectrum and the photovoltaic related parameters of the photoelectric device prepared in the step C4, wherein the photoelectric spectrum signal is excellent and the characteristics of no deep energy level defect and the like are shown as shown in figure 8.
Example two
A method for regulating and controlling two-dimensional van der Waals layered material structure and defect by element doping and a method for growing InSe monocrystal by rare earth Dy element doping Bridgman method are taken as an example in the field of ferroelectric photovoltaics, and the method comprises the following specific steps:
step 1: in synthesis under vacuum state by swing method 0.52 Se 0.48 Dy 0.01 Polycrystalline raw material;
synthesis of In 0.52 Se 0.48 Dy 0.01 The polycrystalline raw materials comprise:
a1: drying In, se and Dy with purity of 4N In the environment of 120 ℃ for 2 hours, and taking out for standby after naturally cooling to room temperature;
a2: according to a pre-designed stoichiometric ratio In 0.52 Se 0.48 Dy 0.01 Accurately calculating the mass of In element and Dy element, weighing, and controlling the weighing precision within a range of +/-0.001 g;
a3: weighing In element and D Y Premixing the elements, putting the elements into a cleaned quartz crucible for vacuum treatment, wherein the pumping speed of a vacuum pump is 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A4: and (5) sealing the quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump. After the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a5: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a6: cooling the InDy alloy synthesized for the first time to room temperature and then taking out;
a7: calculating and weighing the polycrystalline raw material and Se element synthesized for the first time, placing into a cleaned quartz crucible for vacuum treatment, and pumping at a vacuum pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A8: and (3) sealing the double-layer quartz crucible in a vacuum state (as shown in figure 1), and vacuumizing for 30min by a vacuum pump. After the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a9: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a10: cooling the polycrystalline raw material synthesized for the second time to room temperature and then taking out;
step 2: will synthesize good In 0.52 Se 0.48 Dy 0.01 Placing the polycrystalline raw material into a double-layer quartz crucible (inner layer of phi 18mm and outer layer of phi 27 mm) for vacuum treatment, wherein the pumping speed of the vacuum pump is 3.6m 3 ·h -1 Vacuumizing for 30min at the speed;
step 3: and (3) sealing the crucible in a vacuum state, and carrying out vacuum test and fixing on the sealed crucible. After the test is normal, the crucible is placed on a down pipe in a hearth of a crystallization furnace, the bottom of the crucible is ensured to be level with a lower thermocouple, and the position of the crucible is fixed;
step 4: controlling the heating speed and the heat preservation time, and taking out after naturally cooling to room temperature when the raw materials completely pass through the growth area, so as to obtain grown crystals;
the control of the temperature rising speed and the heat preservation time specifically comprises the following steps:
b1: adjusting the crucible to the position of a high-temperature region of a hearth, heating the crystallization furnace to 700 ℃ for 8 hours, and preserving the temperature of the Dy doped InSe polycrystal raw material synthesized in the step 3 for 8 hours at 700 ℃;
b2: the descent apparatus is then operated at 0.5 mm.h -1 The speed of the InSe monocrystal is reduced, and the InSe monocrystal starts to grow when the temperature of the melt at the bottom is reduced below the melting point;
step 5: carrying out artificial mechanical stripping on the grown crystal, cutting and polishing a sample with a required size, and sealing and storing the prepared sample by using a vacuum bag;
step 6: mechanically stripping the grown single crystal sample to obtain a slice sample with proper thickness, and researching ferroelectric and photovoltaic characteristics of the slice sample;
the appearance of the obtained single crystal sample is shown in figure 4, and the scanning electron microscope image and the transmission electron microscope structure analysis image are shown in figures 5 and 6, so that the appearance of the InSe single crystal can be greatly changed by rare earth Dy element impurities, the appearance of the InSe single crystal is greatly reduced in the microstructure, and the interlayer acting force is enhanced; and Dy doped InSe samples also had ferroelectric properties undetectable by undoped samples (fig. 7).
It will be understood that modifications and variations will be apparent to those skilled in the art from the foregoing description, and it is intended that all such modifications and variations be included within the scope of the following claims.

Claims (8)

1. A method for controlling the structure and defects of a two-dimensional layered van der waals material, comprising the steps of:
step 1: synthesizing an InSe polycrystal raw material doped with rare earth elements by adopting a swinging method in a vacuum state;
step 2: placing the synthesized polycrystalline raw material into a double-layer quartz crucible for vacuum treatment;
step 3: sealing the crucible in a vacuum state, and performing vacuum test and fixing the sealed crucible; after the test is normal, the crucible is placed on a down pipe in a hearth of a crystallization furnace, the bottom of the crucible is ensured to be level with a lower thermocouple, and the position of the crucible is fixed;
step 4: controlling the heating speed and the heat preservation time, and taking out after naturally cooling to room temperature when the raw materials completely pass through the growth area, so as to obtain grown crystals;
step 5: carrying out artificial mechanical stripping on the grown crystal;
step 6: the grown single crystal sample was mechanically peeled off to obtain a thin sheet sample of a proper thickness, and the ferroelectric and photovoltaic properties thereof were tested.
2. The method of claim 1, wherein synthesizing the polycrystalline feedstock in step 1 comprises:
a1: drying In, se and rare earth elements with purity of 4N In an environment of 120 ℃ for 2 hours, and taking out for standby after naturally cooling to room temperature;
a2: according to the pre-designed stoichiometric ratio, accurately calculating the mass of the In element and the rare earth element, weighing, and controlling the weighing precision within a range of +/-0.001 g;
a3: premixing the weighed In element and rare earth element, putting the premixed In element and rare earth element into a cleaned quartz crucible for vacuum treatment, and pumping the mixture at a vacuum pump pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A4: sealing the quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump; after the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a5: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a6: cooling the alloy of the In element and the rare earth element synthesized for the first time to room temperature and then taking out;
a7: calculating and weighing the polycrystalline raw material and Se element synthesized for the first time, placing into a cleaned quartz crucible for vacuum treatment, and pumping at a vacuum pumping speed of 3.6m 3 ·h -1 Vacuum was applied at this rate for 30min under vacuum conditions 10 -3 pa;
A8: sealing the double-layer quartz crucible in a vacuum state, and vacuumizing for 30min by a vacuum pump; after the crucible is sealed, in order to ensure the tightness of the crucible, a simple vacuum degree test is carried out;
a9: placing the sealed crucible into a swinging furnace and fixing, firstly, using 200 ℃ h -1 The temperature rise rate of (2) is increased to 800 ℃ and kept for 30min, and then the furnace is swayed for 15 r.min -1 Is swayed for 30min to fully mix the raw materials;
a10: and cooling the polycrystalline raw material synthesized for the second time to room temperature, and taking out for standby.
3. The method according to claim 1, wherein in step 2, the vacuum pump pumping rate is 3.6m 3 ·h -1 Vacuum was applied at this rate for 20-30min.
4. The method according to claim 1, wherein in step 4, the controlling the temperature rising speed and the temperature keeping time specifically includes:
b1: adjusting the crucible to the position of a high-temperature region of a hearth, heating the crystallization furnace to 700 ℃ for 8 hours, and preserving the temperature of the rare earth doped InSe polycrystal raw material synthesized in the step 3 for 8 hours at 700 ℃;
b2: the descent apparatus is then operated at 0.5 mm.h -1 And (2) the speed of the InSe monocrystal starts to grow when the temperature of the melt at the bottom is reduced below the melting point.
5. The method according to claim 1, wherein in step 6, the grown single crystal sample is mechanically peeled to obtain a thin sheet sample with a proper thickness, specifically as follows:
c1: placing a two-dimensional laminar material sheet to be peeled on a 3M transparent adhesive tape by adopting an adhesive tape peeling method; repeatedly pasting and peeling to change the film into a lamellar film with proper thickness; the layered sheet on the tape was further transferred to the target substrate with Polydimethylsiloxane (PDMS), and after standing for a period of time, the PDMS was slowly peeled off leaving the material on the target substrate.
6. The method of claim 1, wherein In step 1, the polycrystalline feedstock is In 0.52 Se 0.48 Y 0.01 Or In 0.52 Se 0.48 Dy 0.01
7. A two-dimensional layered van der waals material prepared according to the method of any one of claims 1 to 6.
8. Use of a material according to claim 7 in the field of ferroelectric photovoltaics.
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