CN117476790B - Double-junction coupling type self-driven ultraviolet photoelectric detector and preparation method thereof - Google Patents
Double-junction coupling type self-driven ultraviolet photoelectric detector and preparation method thereof Download PDFInfo
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Abstract
The invention provides a double-junction coupling type self-driven ultraviolet photoelectric detector and a preparation method thereof. According to the double-junction coupling type self-driven ultraviolet photoelectric detector, on the basis of a pn junction n-Ga 2O3:Sn/p-GaN device, an n-ZnO/n-Ga 2O3:Sn heterogeneous nn junction is built again, so that the directions of built-in electric fields of the heterogeneous nn junction and the pn junction are consistent, and the built-in electric fields of the heterogeneous nn junction and the pn junction are used for superposition coupling under illumination to jointly act and separate and transmit photo-generated carriers, so that the comprehensive performance of the detector is improved; through the photoelectric performance test carried out on the device, the device performance of the superposition coupling of the built-in electric field of the heterogeneous nn junction and the pn junction is obviously improved: under the same illumination with 255nm wavelength, the response speed of the device is faster, the response is obviously improved, and the device has ultrahigh detection rate.
Description
Technical Field
The invention relates to an ultraviolet photoelectric detector, in particular to a double-junction coupling type self-driven ultraviolet photoelectric detector and a preparation method thereof.
Background
The photoelectric detector based on Ga 2O3 material separates and transmits photo-generated carriers under illumination by means of the effect of a pn junction built-in electric field to realize self-driving operation under 0V bias. Since the performance of self-driven photodetectors is often closely related to the action of a built-in electric field, which is typically generated in schottky junctions, heterojunctions, or pn junctions, many self-driven photodetectors rely on only one built-in electric field, which tends to have lower photocurrent and responsivity.
The existing self-driven photodetectors based on Ga 2O3 materials suffer from the above-mentioned drawbacks and there is a need for improvements.
Disclosure of Invention
In view of the above, the invention provides a double-junction coupling type self-driven ultraviolet photoelectric detector and a preparation method thereof, which are used for solving the technical problems of low photocurrent and responsivity in the prior art.
In a first aspect, the present invention provides a dual junction coupling type self-driven ultraviolet photodetector, comprising:
A substrate;
a p-type GaN thin film layer positioned on the surface of the substrate;
The Sn-doped n-type Ga 2O3 film layer is positioned on the surface of one side, far away from the substrate, of the p-type GaN film layer, and the orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
the n-type ZnO film layer is positioned on the surface of one side, far from the substrate, of the Sn-doped n-type Ga 2O3 film layer;
The first metal electrode layer is positioned on the surface of one side of the n-type ZnO film layer, which is far away from the substrate;
and the second metal electrode layer is positioned on the surface of the p-type GaN film layer, which is not covered by the Sn-doped n-type Ga 2O3 film layer.
Preferably, in the double-junction coupling type self-driven ultraviolet photoelectric detector, the Sn doping molar content in the Sn doping n-type Ga 2O3 film layer is 0.5-15%.
Preferably, the material of the first metal electrode layer of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises at least one of In, ti, al, mg, fe;
The material of the second metal electrode layer includes at least one of Pt, ni, au, cu, mo, W.
Preferably, the substrate of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises any one of a c-plane sapphire substrate, a magnesium oxide substrate, a gallium nitride substrate, a silicon substrate, a NSTO substrate, a quartz glass substrate, an r-plane sapphire substrate and an a-plane sapphire substrate.
Preferably, the thickness of the p-type GaN film layer of the double-junction coupling type self-driven ultraviolet photoelectric detector is 2000-2200 nm;
The thickness of the Sn doped n-type Ga 2O3 film layer is 100-450 nm;
the thickness of the n-type ZnO film layer is 10-35 nm.
In a second aspect, the invention also provides a preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector, which comprises the following steps:
Providing a substrate;
Sequentially growing a p-type GaN film layer and a Sn-doped n-type Ga 2O3 film layer on a substrate, wherein the orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
Sequentially growing an n-type ZnO film layer and a first metal electrode layer on the Sn-doped n-type Ga 2O3 film layer;
And growing a second metal electrode layer on the surface of the p-type GaN film layer which is not covered by the Sn-doped n-type Ga 2O3 film layer.
Preferably, in the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector, a substrate is placed in a vacuum cavity of a deposition device, a pulse laser deposition method is adopted to ablate a p-type GaN target material and a Sn-doped n-type Ga 2O3 target material, and a p-type GaN film layer and a Sn-doped n-type Ga 2O3 film layer are sequentially deposited and grown on the substrate; wherein, the technological parameters of the deposition process control are as follows: the substrate temperature is 400-600 ℃, the deposition oxygen pressure is 0-5 Pa, the pulse laser energy is 200-250 mJ, and the pulse number is 9000-40000.
Preferably, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector adopts a pulse laser deposition method to ablate a ZnO target material, and the ZnO target material is deposited and grown on the Sn-doped n-type Ga 2O3 film layer to obtain an n-type ZnO film layer; the process parameters of the deposition process control are as follows: the temperature of the substrate is 340-360 ℃, the deposition oxygen pressure is 1-5 Pa, the pulse laser energy is 200-220 mJ, and the pulse number is 1000-3500.
Preferably, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the following steps of:
ball-milling and mixing SnO 2 powder and Ga 2O3 powder according to a proportion to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
Sintering the ceramic blank at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
Preferably, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the steps of pressing fine powder after ball milling under the pressure of 2-10 MPa to form a ceramic embryo piece with the thickness of 2-5 mm; sintering the ceramic blank for 2-5 hours at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
Compared with the prior art, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector has the following beneficial effects:
According to the double-junction coupling type self-driven ultraviolet photoelectric detector, on the basis of a pn junction n-Ga 2O3:Sn/p-GaN device, an n-ZnO/n-Ga 2O3:Sn heterogeneous nn junction is built again, so that the directions of built-in electric fields of the heterogeneous nn junction and the pn junction are consistent, and the built-in electric fields of the heterogeneous nn junction and the pn junction are used for superposition coupling under illumination to jointly act and separate and transmit photo-generated carriers, so that the comprehensive performance of the detector is improved; through photoelectric performance test carried out on the device, compared with an n-Ga 2O3:Sn/p-GaN-based device with a pn junction, the performance of the n-ZnO/n-Ga 2O3:Sn/p-GaN-based device which is coupled through superposition of built-in electric fields of a heterogeneous nn junction and the pn junction is remarkably improved: under the same illumination with 255nm wavelength, the response speed of the device is faster, the response is obviously improved (135.46 mA/W is increased to 165.56 mA/W), and the device has ultra-high detection rate (1.16X10. 10 13 Jones). The excellent self-driven detector performance shows the great application potential of the device in the field of ultraviolet photoelectric detection. The proposed built-in electric field coupling superposition effect of the heterogeneous nn junction and the pn junction is utilized, the comprehensive performance of the device is improved through a strategy of enhancing separation and transmission of photon-generated carriers, and the method is expected to become a universal method for preparing the high-performance self-driven photoelectric detector.
Drawings
In order to more clearly illustrate the embodiments of the invention or the technical solutions in the prior art, the following description will briefly explain the drawings used in the embodiments or the description of the prior art, and it is obvious that the drawings in the following description are only some embodiments of the invention, and that other drawings can be obtained according to these drawings without inventive effort to a person skilled in the art.
FIG. 1 is a schematic diagram of a dual-junction coupling type self-driven ultraviolet photodetector of the present invention;
FIG. 2 is a XRD total spectrum of a sample of n-ZnO/n-Ga 2O3:Sn/p-GaN thin film prepared in example 1;
FIG. 3 is a FE-SEM sectional view of a sample of an n-ZnO/n-Ga 2O3:Sn/p-GaN thin film prepared in example 1;
FIG. 4 is a graph showing transmission spectra of a single-layer n-Ga 2O3: sn film, a single-layer n-ZnO film, and a single-layer p-GaN film grown on c-Al 2O3, respectively;
FIG. 5 is a graph showing the relationship between (αhν 2) and hv of a single-layer n-Ga 2O3: sn film, a single-layer n-ZnO film, and a single-layer p-GaN film grown on c-Al 2O3, respectively;
FIG. 6 is a graph showing I-V characteristics In a dark state of an n-ZnO/Ga 2O3:Sn/p-GaN device of example 1, showing an In electrode In contact with an n-ZnO thin film and a Ni/Au electrode In contact with a p-GaN thin film;
FIG. 7 is a graph showing the multi-period light response of the n-ZnO/Ga 2O3 Sn/p-GaN double-junction coupling self-driven photodetector of example 1 under 0V bias (a) 255nm and (b) 355nm wavelength illumination;
FIG. 8 is a plot of the single period I-t of the n-ZnO/Ga 2O3 Sn/p-GaN double-junction coupled self-driven photodetector of example 1 under 0V bias (a) 255nm and (b) 355nm wavelength illumination;
FIG. 9 is a graph showing spectral responsivity of an n-ZnO/Ga 2O3:Sn/p-GaN double-junction coupling type self-driven photodetector in example 1;
FIG. 10 is a graph of the broad spectrum ultraviolet band I-t of the device of example 1 for an n-ZnO/Ga 2O3 Sn/p-GaN double-junction coupled self-driven photodetector at 0V bias;
FIG. 11 is a graph showing I-t curves of an n-ZnO/Ga 2O3:Sn/p-GaN double-junction coupled self-driven photodetector of example 1 under different light power densities (a) 255nm and (b) 355nm wavelength illumination.
Detailed Description
The following description of the embodiments of the present invention will be made in detail and with reference to the embodiments of the present invention, but it should be apparent that the described embodiments are only some embodiments of the present invention, and not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the present invention without making any inventive effort, are intended to fall within the scope of the present invention.
As shown in fig. 1, the present invention provides a dual-junction coupling type self-driven ultraviolet photodetector, comprising:
A substrate 1;
a p-type GaN thin film layer 2 located on the surface of the substrate 1;
The Sn doped n-type Ga 2O3 film layer 3 is positioned on the surface of the p-type GaN film layer 2, which is far away from the substrate 1, and the orthographic projection of the Sn doped n-type Ga 2O3 film layer 3 on the surface of the p-type GaN film layer 2 does not completely cover the p-type GaN film layer 2;
An n-type ZnO thin film layer 4 which is positioned on the surface of the Sn-doped n-type Ga 2O3 thin film layer 3 on the side far away from the substrate 1;
a first metal electrode layer 5 located on the surface of the n-type ZnO thin film layer 4 on the side away from the substrate 1;
The second metal electrode layer 6 is located on the surface of the p-type GaN thin film layer 2, which is not covered by the Sn-doped n-type Ga 2O3 thin film layer 3.
The double-junction coupling type self-driven ultraviolet photoelectric detector comprises a substrate 1, a p-type GaN film layer 2, a Sn-doped n-type Ga 2O3 film layer 3, an n-type ZnO film layer 4, a first metal electrode layer 5 and a second metal electrode layer 6; one side of the p-type GaN thin film layer 2 is covered by the Sn-doped n-type Ga 2O3 thin film layer 3, and the other side is not covered by the Sn-doped n-type Ga 2O3 thin film layer 3, namely, the orthographic projection of the Sn-doped n-type Ga 2O3 thin film layer 3 on the surface of the p-type GaN thin film layer 2 does not completely cover the p-type GaN thin film layer 2 (the orthographic projection covers a part of the p-type GaN thin film layer 2, and the other part of the p-type GaN thin film layer 2 is completely exposed); the second metal electrode layer 6 is located on the surface of the p-type GaN thin film layer 2, which is not covered by the Sn-doped n-type Ga 2O3 thin film layer 3. According to the double-junction coupling type self-driven ultraviolet photoelectric detector, a pn junction is formed between the p-type GaN film layer 2 and the Sn-doped n-type Ga 2O3 film layer 3, a heterogeneous nn junction is formed between the Sn-doped n-type Ga 2O3 film layer 3 and the n-type ZnO film layer 4, and on the basis of a pn junction n-Ga 2O3:Sn/p-GaN device, the n-ZnO/n-Ga 2O3:Sn heterogeneous nn junction is reconstructed, so that the directions of built-in electric fields of the heterogeneous nn junction and the pn junction are consistent, and photo-generated carriers can be separated and transmitted under illumination by utilizing the superposition coupling of the built-in electric fields of the two, so that the comprehensive performance of the detector is improved. The n-ZnO is the n-type ZnO film layer 4, the n-Ga 2O3 is the Sn doped n-type Ga 2O3 film layer 3, and the p-GaN is the p-type GaN film layer 2.
In some embodiments, the Sn-doped n-type Ga 2O3 thin film layer 3 has a Sn-doped molar content of 0.5-15%.
In some embodiments, the material of the first metal electrode layer 5 comprises at least one of In, ti, al, mg, fe.
In some embodiments, the material of the second metal electrode layer 6 comprises at least one of Pt, ni, au, cu, mo, W.
Specifically, in some embodiments, the first metal electrode layer 5 is arranged on the surface of the n-type ZnO thin film layer 4 in an array, for example, the array may be 1×1, 2×2 … … n×n, or the like.
In some embodiments, the second metal electrode layer 6 is arranged on the surface of the p-type GaN thin film layer 2 in an array, for example, the array may be 1×1,2×2 … … n×n, or the like.
Preferably, the material of the first metal electrode layer 5 is In, and the thickness is 50 to 100nm, preferably 75nm.
Preferably, the material of the second metal electrode layer 6 is Ni/Au, that is, the second metal electrode layer 6 includes a Ni layer and an Au layer sequentially stacked on the surface of the p-type GaN thin film layer 2, and the total thickness of the Ni layer and the Au layer is 80-120nm, preferably 100nm.
In some embodiments, the substrate comprises any one of a c-plane sapphire substrate, a magnesium oxide substrate, a gallium nitride substrate, a silicon substrate, a NSTO substrate, a quartz glass substrate, r-plane sapphire, a-plane sapphire, and has a thickness of 400-500 μm; preferably, the substrate is 430 μm thick c-plane sapphire, i.e., c-Al 2O3.
In some embodiments, the thickness of the p-type GaN thin film layer is 2000-2200 nm, preferably 2100nm.
In some embodiments, the thickness of the Sn-doped n-type Ga 2O3 thin film layer is 100-450 nm, preferably 380nm.
In some embodiments, the n-type ZnO thin film layer has a thickness of 10-35 nm, preferably 30nm.
Based on the same inventive concept, the invention also provides a preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector, which comprises the following steps:
S1, providing a substrate;
S2, growing a p-type GaN film layer and a Sn-doped n-type Ga 2O3 film layer on the substrate in sequence, wherein orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
s3, sequentially growing an n-type ZnO film layer and a first metal electrode layer on the Sn-doped n-type Ga 2O3 film layer;
and S4, growing a second metal electrode layer on the surface of the p-type GaN film layer which is not covered by the Sn-doped n-type Ga 2O3 film layer.
According to the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector, after a p-type GaN film layer grows on a substrate, one part of the p-type GaN film layer is shielded, the other part of the p-type GaN film layer is exposed, an Sn-doped n-type Ga 2O3 film layer grows on the exposed p-type GaN film layer, the Sn-doped n-type Ga 2O3 film layer and the original shielded part of the p-type GaN film layer form a step shape, and therefore orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer; or after growing the p-type GaN film layer on the substrate, continuously growing the Sn-doped n-type Ga 2O3 film layer on the p-type GaN film layer, then etching the Sn-doped n-type Ga 2O3 film layer by utilizing micro-nano processing technologies such as photoetching and etching technologies, and etching to form a mesa at the p-type GaN film layer, so that orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer.
In some embodiments, step S2 specifically includes: placing a substrate in a vacuum cavity of a deposition device, ablating a p-type GaN target material by adopting a pulse laser deposition method, and depositing and growing on the substrate to obtain a p-type GaN film layer; then, one part of the p-type GaN film layer is shielded and the other part is exposed, then the substrate with the p-type GaN film layer grown is placed in a vacuum cavity of a deposition device, a pulse laser deposition method is adopted to ablate an Sn-doped n-type Ga 2O3 target material, and an Sn-doped n-type Ga 2O3 film layer is grown on the exposed part of the p-type GaN film layer; wherein, in the pulse laser deposition process, the controlled process parameters are as follows: the substrate temperature is 400-600 ℃, the deposition oxygen pressure is 0-5 Pa, the pulse laser energy is 200-250 mJ, and the pulse number is 9000-40000.
In some embodiments, a pulse laser deposition method is adopted to ablate the ZnO target material, and an n-type ZnO film layer is obtained by deposition and growth on the Sn-doped n-type Ga 2O3 film layer; the process parameters of the deposition process control are as follows: the temperature of the substrate is 340-360 ℃, the deposition oxygen pressure is 1-5 Pa, the pulse laser energy is 200-220 mJ, and the pulse number is 1000-3500.
In some embodiments, after a p-type GaN film layer, a Sn-doped n-type Ga 2O3 film layer and an n-type ZnO film layer are sequentially grown on a substrate, etching the n-type ZnO film layer to form a mesa by utilizing micro-nano processing technologies such as photoetching and etching technologies, then growing on the n-type ZnO film layer by utilizing a vacuum evaporation method to obtain a first metal electrode, and growing on the p-type GaN film layer to obtain a second metal electrode. The first metal electrode layer and the second metal electrode layer are finally formed by using processes such as mask, photoetching and the like.
In some embodiments, the first metal electrode layer and the second metal layer may be prepared by chemical vapor deposition, physical vapor deposition, evaporation, or the like.
In some embodiments, the method for preparing the Sn-doped n-type Ga 2O3 target includes:
ball-milling and mixing SnO 2 powder and Ga 2O3 powder according to a proportion to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
Sintering the ceramic blank at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
In some embodiments, the fine powder after ball milling is pressed into ceramic embryo pieces with the thickness of 2-5 mm under the pressure of 2-10 MPa; sintering the ceramic blank for 2-5 hours at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
In some embodiments, in the step of ball-milling and mixing the SnO 2 powder and the Ga 2O3 powder to obtain a fine powder, the mole fraction of Sn in the fine powder is 0.5 to 15%.
Specifically, in some embodiments, the preparation method of the Sn-doped n-type Ga 2O3 target includes the following steps:
Putting the SnO 2 powder and the Ga 2O3 powder which are weighed according to the proportion into a ball milling tank, adding deionized water accounting for 55-65% of the total mass of the powder for ball milling for 6-10 hours, and putting the powder into a vacuum drying oven for drying treatment to obtain dry powder, namely fine powder, wherein the specific drying temperature is 100-130 ℃ and the drying time is 6-12 hours; then adding absolute ethyl alcohol accounting for 1-5% of the total mass of the powder into the dried fine powder, grinding and stirring uniformly, and pressing into ceramic embryo pieces with the thickness of 2-5 mm under the pressure of 2-10 MPa; sintering the ceramic blank for 2-5 hours at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
In some embodiments, prior to placing the substrate in the vacuum chamber of the pulsed laser deposition system, the method further comprises ultrasonically cleaning the substrate with acetone, absolute ethanol, and deionized water in that order.
The following further describes the double-junction coupling type self-driven ultraviolet photoelectric detector and the preparation method thereof according to the specific embodiments. This section further illustrates the summary of the application in connection with specific embodiments, but should not be construed as limiting the application. The technical means employed in the examples are conventional means well known to those skilled in the art, unless specifically stated. Unless specifically stated otherwise, the reagents, methods and apparatus employed in the present application are those conventional in the art.
Example 1
The embodiment of the application provides a double-junction coupling type self-driven ultraviolet photoelectric detector, which comprises the following components:
A substrate;
A p-type GaN thin film layer located on the surface of the substrate;
The Sn doped n-type Ga 2O3 film layer is positioned on the surface of the p-type GaN film layer, which is far away from the substrate, and the orthographic projection of the Sn doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
The n-type ZnO film layer is positioned on the surface of one side of the Sn-doped n-type Ga 2O3 film layer, which is far away from the substrate;
the first metal electrode layer is positioned on the surface of one side of the n-type ZnO film layer far away from the substrate;
the second metal electrode layer is positioned on the surface of the p-type GaN film layer, which is not covered by the Sn-doped n-type Ga 2O3 film layer;
Wherein, the Sn doping mole content in the Sn doping n-type Ga 2O3 film layer is 1%;
the material of the first metal electrode layer is In, and the thickness is 75nm;
the second metal electrode layer is made of Ni/Au, namely the second metal electrode layer comprises a Ni layer and an Au layer which are sequentially laminated on the surface of the p-type GaN film layer, wherein the thickness of the Ni layer is 80nm, and the thickness of the Au layer is 20nm;
The substrate is c-plane sapphire, namely c-Al 2O3, and the thickness is 430 mu m;
the thickness of the p-type GaN film layer is 2100nm;
the thickness of the Sn doped n-type Ga 2O3 film layer is 380nm;
the thickness of the n-type ZnO film layer is 30nm.
The preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the following steps of:
S1, providing a c-plane sapphire substrate, sequentially ultrasonically cleaning the substrate with acetone, absolute ethyl alcohol and deionized water, and drying the substrate with nitrogen for later use;
S2, placing the substrate in a vacuum cavity of a deposition device, ablating a p-type GaN target material by adopting a pulse laser deposition method, and depositing and growing a p-type GaN film layer on the substrate; then, one part of the p-type GaN film layer is shielded and the other part is exposed, then the substrate with the p-type GaN film layer grown is placed in a vacuum cavity of a deposition device, a pulse laser deposition method is adopted to ablate an Sn-doped n-type Ga 2O3 target material, and an Sn-doped n-type Ga 2O3 film layer is grown on the exposed part of the p-type GaN film layer; wherein, in the pulse laser deposition process, the controlled process parameters are as follows: the temperature of the substrate is 500 ℃, the deposition oxygen pressure is 0Pa, the pulse laser energy is 240mJ, and the pulse number is 36000;
s3, ablating a ZnO target material by adopting a pulse laser deposition method, and depositing and growing on the Sn-doped n-type Ga 2O3 film layer to obtain an n-type ZnO film layer; the process parameters of the deposition process control are as follows: the substrate temperature is 350 ℃, the deposition oxygen pressure is 2Pa, the pulse laser energy is 210mJ, and the pulse number is 3000;
S4, growing a first metal electrode (In) on the n-type ZnO film layer by utilizing a vacuum evaporation method, and growing a second metal electrode (Ni/Au) on the p-type GaN film layer;
The preparation method of the Sn-doped n-type Ga 2O3 target comprises the following steps:
Putting the SnO 2 powder and the Ga 2O3 powder which are weighed according to the proportion into a ball milling tank, adding deionized water accounting for 60% of the total mass of the powder for ball milling for 8 hours, and putting the powder into a vacuum drying oven for drying treatment to obtain dry powder, namely fine powder, wherein the specific drying temperature is 120 ℃ and the drying time is 9 hours; then adding absolute ethyl alcohol accounting for 3% of the total mass of the powder into the dried fine powder, grinding and stirring uniformly, and pressing into ceramic green sheets with the thickness of 3mm under the pressure of 6 MPa; and sintering the ceramic green sheet for 4 hours at 1300 ℃ to obtain the Sn doped n-type Ga 2O3 target, wherein the mole fraction of Sn in the Sn doped n-type Ga 2O3 target is 1%.
Comparative example 1
This comparative example provides a self-driven ultraviolet photodetector comprising:
A substrate;
A p-type GaN thin film layer located on the surface of the substrate;
The Sn doped n-type Ga 2O3 film layer is positioned on the surface of the p-type GaN film layer, which is far away from the substrate, and the orthographic projection of the Sn doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
The first metal electrode layer is positioned on the surface of one side of the Sn-doped n-type Ga 2O3 film layer, which is far away from the substrate;
the second metal electrode layer is positioned on the surface of the p-type GaN film layer, which is not covered by the Sn-doped n-type Ga 2O3 film layer;
Wherein, the Sn doping mole content in the Sn doping n-type Ga 2O3 film layer is 1%;
the material of the first metal electrode layer is In, and the thickness is 75nm;
the second metal electrode layer is made of Ni/Au, namely the second metal electrode layer comprises a Ni layer and an Au layer which are sequentially laminated on the surface of the p-type GaN film layer, wherein the thickness of the Ni layer is 80nm, and the thickness of the Au layer is 20nm;
The substrate is c-plane sapphire, namely c-Al 2O3, and the thickness is 430 mu m;
the thickness of the p-type GaN film layer is 2100nm;
The thickness of the Sn doped n-type Ga 2O3 film layer is 380nm.
The preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the following steps of:
S1, providing a c-plane sapphire substrate, sequentially ultrasonically cleaning the substrate with acetone, absolute ethyl alcohol and deionized water, and drying the substrate with nitrogen for later use;
S2, placing the substrate in a vacuum cavity of a deposition device, ablating a p-type GaN target material by adopting a pulse laser deposition method, and depositing and growing a p-type GaN film layer on the substrate; then, one part of the p-type GaN film layer is shielded and the other part is exposed, then the substrate with the p-type GaN film layer grown is placed in a vacuum cavity of a deposition device, a pulse laser deposition method is adopted to ablate an Sn-doped n-type Ga 2O3 target material, and an Sn-doped n-type Ga 2O3 film layer is grown on the exposed part of the p-type GaN film layer; wherein, in the pulse laser deposition process, the controlled process parameters are as follows: the temperature of the substrate is 500 ℃, the deposition oxygen pressure is 0Pa, the pulse laser energy is 240mJ, and the pulse number is 36000;
S3, growing a first metal electrode (In) on the Sn-doped n-type Ga 2O3 target material by utilizing a vacuum evaporation method, and growing a second metal electrode (Ni/Au) on the p-type GaN film layer;
The preparation method of the Sn-doped n-type Ga 2O3 target comprises the following steps:
Putting the SnO 2 powder and the Ga 2O3 powder which are weighed according to the proportion into a ball milling tank, adding deionized water accounting for 60% of the total mass of the powder for ball milling for 8 hours, and putting the powder into a vacuum drying oven for drying treatment to obtain dry powder, namely fine powder, wherein the specific drying temperature is 120 ℃ and the drying time is 9 hours; then adding absolute ethyl alcohol accounting for 3% of the total mass of the powder into the dried fine powder, grinding and stirring uniformly, and pressing into ceramic green sheets with the thickness of 3mm under the pressure of 6 MPa; and sintering the ceramic green sheet for 4 hours at 1300 ℃ to obtain the Sn doped n-type Ga 2O3 target, wherein the mole fraction of Sn in the Sn doped n-type Ga 2O3 target is 1%.
Performance testing
The n-ZnO/n-Ga 2O3 Sn/p-GaN thin film sample prepared in example 1 (i.e., n-type ZnO thin film layer/Sn-doped n-type Ga 2O3 thin film layer/p-type GaN thin film layer) was subjected to a 2-theta full spectrum test, and the results are shown in FIG. 2.
As can be seen from FIG. 2, in addition to the c-Al 2O3 (0006) substrate peak and the diffraction peak of the p-GaN film, there are three characteristic diffraction peaks corresponding to the (002), (004) and (006) crystal planes of ε -Ga 2O3. Since the (002) diffraction peak of ZnO overlaps with the p-GaN diffraction peak, no characteristic peak of ZnO was observed in the XRD pattern.
To further understand the thickness of each layer of film in the probe in example 1, FE-SEM cross-section scan test was performed on n-ZnO/n-Ga 2O3:Sn/p-GaN film samples. As shown in FIG. 3, the thicknesses of the ZnO film, the n-Ga 2O3 Sn film and the p-GaN film are respectively 30nm, 380nm and 2100nm, and the reason that the ZnO film is thinner at the uppermost layer is that the ZnO band gap is smaller than that of Ga 2O3, so that on one hand, the ZnO is prevented from absorbing deep ultraviolet light to influence the performance of the device, and on the other hand, a certain thickness is needed to construct a heterojunction.
To evaluate the optical band gap of each film in the detector in example 1, a single layer of n-Ga 2O3: sn film (i.e., sn-doped n-type Ga 2O3 film layer) and a single layer of ZnO film, a single layer of p-GaN film were grown on c-Al 2O3 using the same growth conditions and method, respectively. The optical properties of each film were then evaluated by testing the transmission spectrum of each film, and the results are shown in fig. 4 to 5.
The transmission spectrum of each single-layer film is shown in fig. 4, and the transmission spectrum shows that each single-layer film has good light transmittance in the visible light and near infrared regions, and the higher light transmittance of the film has the advantages of higher anti-interference capability and high sensitivity for preparing the detector. The absorption rate alpha of the film is calculated by the transmission spectrum, and the linear part of the relation curve of (alpha hv) 2 and hv is extrapolated to intersect with the axis of abscissa according to the Tauc formula, so that the size of the optical band gap E g of the film (equal to the axis of abscissa hv of intersection) can be obtained.
From the graph of FIG. 5, it can be estimated that the optical band gaps of ZnO, ga 2O3, sn and GaN films are 3.3eV,4.83eV and 3.4eV, respectively.
The contact type between the electrode and the corresponding film is verified before photoelectric test, so that the influence caused by the contact barrier between the electrode and the film is eliminated. A Keithley 2635B source list is used for applying a scanning voltage of-2V to two In electrodes on an n-ZnO film, and a scanning voltage of-2V to two Ni/Au electrodes on a p-GaN film, as shown In a small inset of figure 6, the non-contact potential barrier between the corresponding electrode and the two films can be judged through an I-V curve between the electrode and the films, and the contact type is ohmic contact. Fig. 6 is an I-V curve test of the n-ZnO/Ga 2O3: sn/p-GaN device prepared in example 1 in the dark state, which shows that the device has a remarkable rectifying effect, i.e., unidirectional conductivity, and an on-voltage of about 2.2V. The reason for the rectification is from the fact that the heterogeneous nn junction of n-ZnO and n-Ga 2O3:Sn cooperates with the pn junction of n-Ga 2O3:Sn and p-GaN.
To compare the performance of the n-ZnO/n-Ga 2O3:Sn/p-GaN double-junction coupled self-driven photodetector in example 1 with respect to the performance of the n-Ga 2O3:Sn/p-GaN self-driven ultraviolet photodetector having only a pn junction in comparative example 1, the photoelectric performance of the device was tested at a bias voltage of 0V. The photoelectric response of the device was tested by applying light with a light wavelength of 255nm and 355nm to the device, as shown in fig. 7. The dark current of the device was only 5pA, and fig. 7 (a) is a repeated photo-response test under light of 255nm wavelength for a plurality of cycles, and it can be seen that the photo-current of the device suddenly increased to 110nA, and the photo-dark ratio was about 2.2×10 4. Fig. 7 (b) is a repeated photo-response test under light of wavelength 355nm for a plurality of cycles, and it can be seen that the photo-current at the device suddenly increased to 1150nA with a photo-dark ratio of about 2.3×10 5. By comparing the photoelectric performance of the self-driven ultraviolet photoelectric detector with the n-Ga 2O3:Sn/p-GaN with the pn junction, the photoelectric current of the device of the self-driven ultraviolet photoelectric detector with the n-ZnO/n-Ga 2O3:Sn/p-GaN double-junction coupling type with the heterogeneous nn junction and the pn junction is obviously improved no matter under the illumination with the wavelength of 255nm or 355 nm.
The response time of the n-ZnO/n-Ga 2O3:Sn/p-GaN double-junction coupling type self-driven photoelectric detector under the illumination with the wavelengths of 255nm and 355nm is calculated through an I-t curve. As shown in fig. 8 (a), τ rise＝0.31s,τdecay =0.39 s under 255nm wavelength illumination, and as shown in fig. 8 (b), τ rise＝0.04s,τdecay =0.06 s under 355nm wavelength illumination, the response speed of the device is fast. Comparing the photoelectric performance of the self-driven ultraviolet photodetector with the n-Ga 2O3: sn/p-GaN with pn junction in comparative example 1, it can be seen that the response time of the n-ZnO/n-Ga 2O3: sn/p-GaN device with double junction coupling is shorter, thus having a certain advantage in the response speed of the detector.
To evaluate the responsivity R of the devices prepared in example 1 and comparative example 1 at different wavelengths of light, different wavelengths of light were applied to the devices, and the responses of the calculated devices were tested, and the results are shown in fig. 9. The calculation results show that the peak response of the device in example 1 is 260nm and the responsivity is 178.24mA/W. By comparing n-Ga 2O3:Sn/p-GaN devices, the responsiveness of the n-ZnO/n-Ga 2O3:Sn/p-GaN devices with double-junction coupling is remarkably improved.
The response band is wider from the responsivity spectrum of the device, and the I-t curves of the detector in example 1 under the irradiation of ultraviolet band with wide spectrum are tested respectively. As shown in fig. 10, the device is shown to have good detection effect in a wide ultraviolet range.
FIG. 11 is a graph of I-t for the device of example 1 under illumination at 255nm and 355nm wavelengths at different optical power densities at a bias of 0V, and it can be seen that the prepared probe exhibits excellent stability and repeatability at different illumination intensities, and the photocurrent of the device increases with increasing optical power density of illumination.
Further, the applicant lists the self-driving performance parameter comparisons at 0V bias for the detector prepared in example 1 of the present application, the detector prepared in comparative example 1, and the photodetectors based on Ga 2O3 material reported in the prior literature. The results are shown in Table 1 below.
TABLE 1 self-driven detection Performance of different photodetectors at 0V bias
As can be seen from the comparison of the table 1, the performance of the self-driven photoelectric detector based on the n-ZnO/n-Ga 2O3:Sn/p-GaN double-junction coupling type is superior, which shows that the superposition coupling of the heterogeneous nn junction and the pn junction is a very promising method for improving the performance of the self-driven photoelectric detector.
The invention adopts PLD (pulsed laser deposition) technology, adopts Ga 2O3 target material and ZnO target material with Sn doped mole content of 1%, and has substrate temperature of 500 ℃ and deposition oxygen pressure of 0Pa. An n-Ga 2O3:Sn film is deposited on a p-GaN film which is epitaxially grown on c-Al 2O3, then a ZnO film is deposited, and a Ni/Au electrode and an In electrode which form ohmic contact are respectively prepared on the film by vacuum evaporation, so that a novel n-ZnO/n-Ga 2O3:Sn/p-GaN double-junction coupling type self-driven ultraviolet photoelectric detector is constructed. The crystal structure of the thin film, the thickness of each layer of the thin film, and the optical characteristics thereof were studied. Through photoelectric performance test carried out on the device, compared with an n-Ga 2O3:Sn/p-GaN-based device with a pn junction, the performance of the n-ZnO/n-Ga 2O3:Sn/p-GaN-based device which is coupled through superposition of built-in electric fields of a heterogeneous nn junction and the pn junction is remarkably improved: under the same illumination with 255nm wavelength, the response speed of the device is faster, the response is obviously improved (135.46 mA/W is increased to 165.56 mA/W), and the device has ultra-high detection rate (1.16X10. 10 13 Jones). The excellent self-driven detector performance shows the great application potential of the device in the field of ultraviolet photoelectric detection. The proposed built-in electric field coupling superposition effect of the heterogeneous nn junction and the pn junction is utilized, the comprehensive performance of the device is improved through a strategy of enhancing separation and transmission of photon-generated carriers, and the method is expected to become a universal method for preparing the high-performance self-driven photoelectric detector.
The foregoing description of the preferred embodiments of the invention is not intended to be limiting, but rather is intended to cover all modifications, equivalents, alternatives, and improvements that fall within the spirit and scope of the invention.
Claims (10)
1. The utility model provides a pair of knot coupling formula self-driven ultraviolet photodetector which characterized in that includes:
A substrate;
a p-type GaN thin film layer positioned on the surface of the substrate;
The Sn-doped n-type Ga 2O3 film layer is positioned on the surface of one side, far away from the substrate, of the p-type GaN film layer, and the orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
the n-type ZnO film layer is positioned on the surface of one side, far from the substrate, of the Sn-doped n-type Ga 2O3 film layer;
The first metal electrode layer is positioned on the surface of one side of the n-type ZnO film layer, which is far away from the substrate;
and the second metal electrode layer is positioned on the surface of the p-type GaN film layer, which is not covered by the Sn-doped n-type Ga 2O3 film layer.
2. The dual-junction coupling type self-driven ultraviolet photoelectric detector according to claim 1, wherein the Sn doping molar content in the Sn doped n-type Ga 2O3 film layer is 0.5-15%.
3. The dual junction coupled self-driven ultraviolet photodetector of claim 1, wherein the material of said first metal electrode layer comprises at least one of In, ti, al, mg, fe;
The material of the second metal electrode layer includes at least one of Pt, ni, au, cu, mo, W.
4. The dual-junction coupled self-driven ultraviolet photodetector of claim 1, wherein said substrate comprises any one of a c-plane sapphire substrate, a magnesium oxide substrate, a gallium nitride substrate, a silicon substrate, a NSTO substrate, a quartz glass substrate, an r-plane sapphire substrate, and an a-plane sapphire substrate.
5. The dual-junction coupled self-driven ultraviolet photodetector as defined in any one of claims 1 to 4, wherein the thickness of the p-type GaN thin film layer is 2000 to 2200nm;
The thickness of the Sn doped n-type Ga 2O3 film layer is 100-450 nm;
the thickness of the n-type ZnO film layer is 10-35 nm.
6. A method for manufacturing a double-junction coupling type self-driven ultraviolet photoelectric detector according to any one of claims 1 to 5, comprising the following steps:
Providing a substrate;
Sequentially growing a p-type GaN film layer and a Sn-doped n-type Ga 2O3 film layer on a substrate, wherein the orthographic projection of the Sn-doped n-type Ga 2O3 film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
Sequentially growing an n-type ZnO film layer and a first metal electrode layer on the Sn-doped n-type Ga 2O3 film layer;
And growing a second metal electrode layer on the surface of the p-type GaN film layer which is not covered by the Sn-doped n-type Ga 2O3 film layer.
7. The method for preparing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 6, wherein a substrate is placed in a vacuum cavity of a deposition device, a pulse laser deposition method is adopted to ablate a p-type GaN target material and a Sn-doped n-type Ga 2O3 target material, and a p-type GaN film layer and a Sn-doped n-type Ga 2O3 film layer are obtained by deposition and growth on the substrate in sequence; wherein, the technological parameters of the deposition process control are as follows: the substrate temperature is 400-600 ℃, the deposition oxygen pressure is 0-5 Pa, the pulse laser energy is 200-250 mJ, and the pulse number is 9000-40000.
8. The method for preparing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 6, wherein a pulse laser deposition method is adopted to ablate a ZnO target material, and an n-type ZnO film layer is obtained by deposition and growth on an Sn-doped n-type Ga 2O3 film layer; the process parameters of the deposition process control are as follows: the temperature of the substrate is 340-360 ℃, the deposition oxygen pressure is 1-5 Pa, the pulse laser energy is 200-220 mJ, and the pulse number is 1000-3500.
9. The method for preparing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 7, wherein the method for preparing the Sn-doped n-type Ga 2O3 target comprises the following steps:
ball-milling and mixing SnO 2 powder and Ga 2O3 powder according to a proportion to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
Sintering the ceramic blank at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
10. The method for manufacturing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 9, wherein the fine powder after ball milling is pressed into ceramic embryo sheets with the thickness of 2-5 mm under the pressure of 2-10 MPa; sintering the ceramic blank for 2-5 hours at 800-1300 ℃ to obtain the Sn doped n-type Ga 2O3 target.
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| CN115295677A (en) * | 2022-08-19 | 2022-11-04 | 上海电机学院 | High responsivity beta-Ga 2 O 3 Base heterojunction self-powered ultraviolet detector and preparation method and application thereof |
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| CN115295677A (en) * | 2022-08-19 | 2022-11-04 | 上海电机学院 | High responsivity beta-Ga 2 O 3 Base heterojunction self-powered ultraviolet detector and preparation method and application thereof |
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