CN117476790A - 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. The double-junction coupling type self-driven ultraviolet photoelectric detector is based on pn junction n-Ga 2 O 3 On the basis of Sn/p-GaN device, reconstructing n-ZnO/n-Ga 2 O 3 Sn heterojunction, which is formed in both the heterojunction and pn junctionThe built-in electric fields have the same direction, and the built-in electric fields of the two are superposed and coupled under illumination to jointly act and separate and transmit the 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
Ga-based 2 O 3 The photoelectric detector of the material separates and transmits photo-generated carriers under illumination by virtue of the effect of an electric field built in a pn junction so as to realize self-driven 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.
Ga-based 2 O 3 The existing self-driven photoelectric detector of the material has the defects and needs to be matched withThis improves.
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;
sn-doped n-type Ga 2 O 3 A thin film layer located on the surface of the p-type GaN thin film layer far from the substrate side, the Sn doped n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
an n-type ZnO thin film layer positioned on the Sn-doped n-type Ga 2 O 3 The surface of the thin film layer far away from one side of the substrate;
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;
a second metal electrode layer located on the p-type GaN thin film layer and not doped with the Sn 2 O 3 The surface covered by the film layer.
Preferably, the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the Sn doped n-type Ga 2 O 3 The Sn doping mole content in the 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, an 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 Sn doped n-type Ga 2 O 3 The thickness of the 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 Sn-doped n-type Ga on a substrate 2 O 3 A thin film layer doped with n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
doping n-type Ga in Sn 2 O 3 Sequentially growing an n-type ZnO film layer and a first metal electrode layer on the film layer;
in the p-type GaN film layer and not doped with the Sn 2 O 3 And growing a second metal electrode layer on the surface covered by the film layer.
Preferably, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the steps of placing a substrate in a vacuum cavity of a deposition device, and ablating a p-type GaN target material and Sn-doped n-type Ga by adopting a pulse laser deposition method 2 O 3 The target material is sequentially deposited and grown on the substrate to obtain a p-type GaN film layer and Sn-doped n-type Ga 2 O 3 A thin film layer; 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 ZnO target material and dope n-type Ga in Sn 2 O 3 Depositing and growing on the film layer to obtain an n-type ZnO film layer; the process parameters of the deposition process control are that: 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 step of doping n-type Ga with Sn 2 O 3 The preparation method of the target comprises the following steps:
proportionally mixing SnO 2 Powder, ga 2 O 3 Ball milling and mixing the powder to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
sintering the ceramic blank at 800-1300 ℃ to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
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 at 800-1300 ℃ for 2-5 h to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
Compared with the prior art, the preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector has the following beneficial effects:
the double-junction coupling type self-driven ultraviolet photoelectric detector is based on pn junction n-Ga 2 O 3 On the basis of Sn/p-GaN device, reconstructing n-ZnO/n-Ga 2 O 3 Sn heterogeneous nn junction, make the direction of built-in electric field of both heterogeneous nn junction and pn junction identical, utilize built-in electric field superposition coupling of both can cooperate to separate and transmit the photogenerated carrier under illumination, thus promote the comprehensive performance of the detector; through photoelectric performance test of the device, the device is discovered to be connected with n-Ga with pn junction only 2 O 3 n-ZnO/n-Ga coupled by superposition of built-in electric fields of heterogeneous nn and pn junctions, compared to Sn/p-GaN based devices 2 O 3 The Sn/p-GaN-based device performance is obviously improved: under the same illumination with 255nm wavelength, the device has faster response speed, obvious response improvement (135.46 mA/W is increased to 165.56 mA/W), and ultra-high detection rate (1.16X10) 13 Jones). Excellent self-driven detector performance demonstrates the deviceThe piece has great application potential 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 n-ZnO/n-Ga prepared in example 1 2 O 3 XRD full spectrum of Sn/p-GaN film sample;
FIG. 3 is n-ZnO/n-Ga prepared in example 1 2 O 3 FE-SEM sectional view of Sn/p-GaN film sample;
FIG. 4 is a graph of the composition of C-Al 2 O 3 On which a monolayer of n-Ga is grown, respectively 2 O 3 A transmission spectrum chart of a Sn film, a single-layer n-ZnO film and a single-layer p-GaN film;
FIG. 5 is a schematic diagram of a C-Al phase 2 O 3 On which a monolayer of n-Ga is grown, respectively 2 O 3 Sn film, monolayer n-ZnO film, monolayer p-GaN film (alpha h v) 2 A graph of the relationship with hv;
FIG. 6 is n-ZnO/Ga in example 1 2 O 3 I-V characteristic curve graph of Sn/p-GaN device In dark state, wherein the inset is I-V characteristic curve graph of In electrode contacted with n-ZnO film and Ni/Au electrode contacted with p-GaN film;
FIG. 7 is n-ZnO/Ga in example 1 2 O 3 Sn/p-GaN double-junction coupling type self-driven photoelectric detector has multi-period light response curves under 0V bias voltage (a) 255nm and (b) 355nm wavelength illumination;
FIG. 8 shows n-ZnO/Ga in example 1 2 O 3 A single period I-t curve of the Sn/p-GaN double-junction coupling type self-driven photoelectric detector under 0V bias voltage (a) 255nm and (b) 355nm wavelength illumination;
FIG. 9 is n-ZnO/Ga in example 1 2 O 3 A spectral responsivity curve of the Sn/p-GaN double-junction coupling type self-driven photoelectric detector;
FIG. 10 shows n-ZnO/Ga in example 1 2 O 3 A wide-spectrum ultraviolet band I-t curve chart of a Sn/p-GaN double-junction coupling type self-driven photoelectric detector under 0V bias voltage;
FIG. 11 is n-ZnO/Ga in example 1 2 O 3 An I-t curve graph of the Sn/p-GaN double-junction coupling type self-driven photoelectric detector under different optical 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;
sn-doped n-type Ga 2 O 3 A thin film layer 3 on the surface of the p-type GaN thin film layer 2 on the side remote from the substrate 1, sn-doped n-type Ga 2 O 3 Orthographic projection of the 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 located on the Sn-doped n-type Ga 2 O 3 The surface of the thin film layer 3 on the side 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;
a second metal electrode layer 6 located on the p-type GaN thin film layer 2 and not doped with Sn 2 O 3 The surface covered by the film layer 3.
It should be noted that the double-junction coupling type self-driven ultraviolet photoelectric detector of the invention comprises a substrate 1, a p-type GaN film layer 2 and Sn doped n-type Ga 2 O 3 A film layer 3, an n-type ZnO film layer 4, a first metal electrode layer 5 and a second metal electrode layer 6; wherein, one side of the p-type GaN film layer 2 is doped with Sn to form n-type Ga 2 O 3 The other side is not covered by Sn-doped n-type Ga 2 O 3 Film layer 3 covers, i.e. Sn-doped n-type Ga 2 O 3 The orthographic projection of the 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 (orthographic projection covers part of the p-type GaN film layer 2 and the other part of the p-type GaN film layer 2 is completely exposed); a second metal electrode layer 6 located on the p-type GaN thin film layer 2 and not doped with Sn 2 O 3 The surface covered by the film layer 3. The double-junction coupling type self-driven ultraviolet photoelectric detector of the invention has the advantages that the p-type GaN film layer 2 and the Sn doped n-type Ga 2 O 3 A pn junction is formed between the film layers 3, and Sn is doped with n-type Ga 2 O 3 The heterogeneous nn junction is formed between the film layer 3 and the n-type ZnO film layer 4, and the invention is based on the pn junction n-Ga 2 O 3 On the basis of Sn/p-GaN device, reconstructing n-ZnO/n-Ga 2 O 3 The Sn heterojunction is in consistent with the built-in electric field direction of the pn junction, and the photo-generated carriers can be separated and transmitted under illumination by utilizing the superposition coupling of the built-in electric fields of the Sn heterojunction and the pn junction, so that the comprehensive performance of the detector is improved. The n-ZnO is n-ZnO film layer 4, n-Ga 2 O 3 Sn is Sn doped with n-type Ga 2 O 3 The film layer 3 and the p-GaN film layer 2 are p-type GaN film layers.
In some embodiments, sn-doped n-type Ga 2 O 3 The Sn doping mole content in the film layer 3 is 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× 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× 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, an 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 2 O 3 。
In some embodiments, the thickness of the p-type GaN thin film layer is 2000-2200 nm, preferably 2100nm.
In some embodiments, sn-doped n-type Ga 2 O 3 The thickness of the thin film layer is 100 to 450nm, 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 Sn-doped n-type Ga on the substrate in sequence 2 O 3 Thin film layer, sn-doped n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
s3, doping n-type Ga in Sn 2 O 3 Sequentially growing an n-type ZnO film layer and a first metal electrode layer on the film layer;
s4, doping n-type Ga in the p-type GaN film layer without the Sn 2 O 3 And growing a second metal electrode layer on the surface covered by the film layer.
The preparation method of the double-junction coupling type self-driven ultraviolet photoelectric detector comprises the steps of after a p-type GaN film layer grows on a substrate, shielding one part of the p-type GaN film layer, exposing the other part of the p-type GaN film layer, and growing Sn doped n-type Ga on the exposed p-type GaN film layer 2 O 3 A thin film layer doped with n-type Ga 2 O 3 The thin film layer and the original shielding part p-type GaN thin film layer form a step shape, so that Sn is doped with n-type Ga 2 O 3 Orthographic projection of the 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 Sn doped n-type Ga on the p-type GaN film layer 2 O 3 The thin film layer is then doped with n-type Ga by utilizing photoetching, etching technology and other micro-nano processing technology 2 O 3 Etching the film layer to form a mesa at the p-type GaN film layer to dope Sn with n-type Ga 2 O 3 Orthographic projection of the 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 is placed in a vacuum cavity of a deposition device, and Sn doped n-type Ga is ablated by adopting a pulse laser deposition method 2 O 3 The target material grows on the exposed part of the p-type GaN film layer to obtain Sn doped n-type Ga 2 O 3 A thin 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, firing is performed using pulsed laser depositionEtching ZnO target material, doping n-type Ga in Sn 2 O 3 Depositing and growing on the 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.
In some embodiments, a p-type GaN thin film layer, sn-doped n-type Ga are grown sequentially on a substrate 2 O 3 And etching the n-type ZnO film layer by utilizing micro-nano processing technologies such as photoetching and etching technology after the film layer and the n-type ZnO film layer are formed, etching the n-type ZnO film layer to the p-type GaN film layer to form a table top, 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, sn-doped n-type Ga 2 O 3 The preparation method of the target comprises the following steps:
proportionally mixing SnO 2 Powder, ga 2 O 3 Ball milling and mixing the powder to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
sintering the ceramic blank at 800-1300 ℃ to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
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 at 800-1300 ℃ for 2-5 h to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
In some embodiments, snO is 2 Powder, ga 2 O 3 In the step of ball milling and mixing the powder to obtain fine powder, the mole fraction of Sn in the fine powder is 0.5-15%.
Specifically, in some embodiments, sn-doped n-type Ga 2 O 3 Preparation method of target materialA method comprising the steps of:
the SnO is weighed according to the proportion 2 Powder, ga 2 O 3 Placing the powder in a ball milling tank, adding deionized water with the total mass of 55-65% of the powder for ball milling for 6-10 h, and then placing the powder in 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 h; 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 at 800-1300 ℃ for 2-5 h to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
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 dual-junction coupling type self-driven ultraviolet photoelectric detector and the preparation method thereof. This section further illustrates the summary of the invention in connection with specific embodiments, but should not be construed as limiting the invention. 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 invention 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:
a substrate;
a p-type GaN thin film layer located on the surface of the substrate;
sn-doped n-type Ga 2 O 3 A thin film layer on the surface of the p-type GaN thin film layer far from the substrate, and Sn-doped n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
an n-type ZnO thin film layer positioned on the Sn doped n-type Ga 2 O 3 The surface of the thin film layer far away from one side of 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;
a second metal electrode layer positioned on the p-type GaN film layer and not doped with Sn 2 O 3 A surface covered by the film layer;
wherein Sn is doped with n-type Ga 2 O 3 The Sn doping mole content in the 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 being c-plane sapphire, i.e. c-Al 2 O 3 The thickness is 430 mu m;
the thickness of the p-type GaN film layer is 2100nm;
sn-doped n-type Ga 2 O 3 The thickness of the 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 is placed in a vacuum cavity of a deposition device, and Sn doped n-type Ga is ablated by adopting a pulse laser deposition method 2 O 3 The target material grows on the exposed part of the p-type GaN film layer to obtain Sn doped n-type Ga 2 O 3 A thin 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 the ZnO target material by adopting a pulse laser deposition method, doping n-type Ga in Sn 2 O 3 Depositing and growing on the 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;
wherein Sn is doped with n-type Ga 2 O 3 The preparation method of the target comprises the following steps:
the SnO is weighed according to the proportion 2 Powder, ga 2 O 3 Placing the powder in a ball milling tank, adding deionized water accounting for 60% of the total mass of the powder for ball milling for 8 hours, and then placing the powder in 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; sintering the ceramic blank at 1300 ℃ for 4 hours to obtain the Sn doped n-type Ga 2 O 3 Target material, wherein Sn is doped with n-type Ga 2 O 3 The mole fraction of Sn in the 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;
sn-doped n-type Ga 2 O 3 A thin film layer on the surface of the p-type GaN thin film layer far from the substrate, and Sn-doped n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
a first metal electrode layer positioned on the Sn doped n-type Ga 2 O 3 The surface of the thin film layer far away from one side of the substrate;
a second metal electrode layer positioned on the p-type GaN film layer and not doped with Sn 2 O 3 A surface covered by the film layer;
wherein Sn is doped with n-type Ga 2 O 3 The Sn doping mole content in the 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 being c-plane sapphire, i.e. c-Al 2 O 3 The thickness is 430 mu m;
the thickness of the p-type GaN film layer is 2100nm;
sn-doped n-type Ga 2 O 3 The thickness of the thin film layer was 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 is placed in a vacuum cavity of a deposition device, and Sn doped n-type Ga is ablated by adopting a pulse laser deposition method 2 O 3 The target material grows on the exposed part of the p-type GaN film layer to obtain Sn doped n-type Ga 2 O 3 A thin 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, doping n-type Ga into Sn by utilizing a vacuum evaporation method 2 O 3 Growing a first metal electrode (In) on the target material, and growing a second metal electrode (Ni/Au) on the p-type GaN film layer;
wherein Sn is doped with n-type Ga 2 O 3 Target materialThe preparation method of (2) comprises the following steps:
the SnO is weighed according to the proportion 2 Powder, ga 2 O 3 Placing the powder in a ball milling tank, adding deionized water accounting for 60% of the total mass of the powder for ball milling for 8 hours, and then placing the powder in 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; sintering the ceramic blank at 1300 ℃ for 4 hours to obtain the Sn doped n-type Ga 2 O 3 Target material, wherein Sn is doped with n-type Ga 2 O 3 The mole fraction of Sn in the target is 1%.
Performance testing
For n-ZnO/n-Ga prepared in example 1 2 O 3 Sn/p-GaN film sample (i.e., n-type ZnO film layer/Sn-doped n-type Ga 2 O 3 Film layer/p-type GaN film layer) was subjected to a 2θ full spectrum test, and the results are shown in fig. 2.
As can be seen from FIG. 2, c-Al is removed 2 O 3 (0006) Substrate peak and diffraction peak of p-GaN film, and epsilon-Ga 2 O 3 Three characteristic diffraction peaks corresponding to the (002), (004) and (006) crystal planes. 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 thin film in the detector of example 1, for n-ZnO/n-Ga 2 O 3 FE-SEM section scan test was performed on Sn/p-GaN film samples. As shown in FIG. 3, wherein ZnO film, n-Ga 2 O 3 The thicknesses of the Sn film and the p-GaN film are respectively 30nm, 380nm and 2100nm, and the reason that the thickness of the ZnO film at the uppermost layer is thinner is that the ZnO band gap is relative to Ga 2 O 3 And the device is smaller, so that on one hand, the phenomenon that ZnO absorbs deep ultraviolet light to influence the performance of the device is avoided, and on the other hand, a certain thickness is needed to construct a heterojunction.
To evaluate the optical band gap of each thin film in the detector of example 1, the same growth conditions and methods were used for c-Al, respectively 2 O 3 Growing a monolayer of n-Ga 2 O 3 Sn film (i.e. Sn-doped n-Ga 2 O 3 Thin film layer) and a single layer of ZnO thin film, a single layer of p-GaN thin film. 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. Calculating film absorptivity alpha from the transmission spectrum, and determining (alpha hv) according to Tauc formula 2 Extrapolation of the linear portion of the hv relationship curve to intersect the abscissa axis yields the thin film optical bandgap E g Size (equal to the intersection abscissa hv).
From FIG. 5, znO, ga can be estimated 2 O 3 The optical band gaps of the 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 shows the dark state of n-ZnO/Ga prepared in example 1 2 O 3 I-V curve test of Sn/p-GaN device, the test curve shows that the device has obvious rectifying effect, namely unidirectional conductivity, and the starting voltage is about 2.2V. The reason for rectification is from n-ZnO and n-Ga 2 O 3 Sn heterojunction with n-Ga 2 O 3 The pn junction of Sn and p-GaN co-acts.
For comparison of n-ZnO/n-Ga in example 1 2 O 3 Sn/p-GaN double-junction coupling type self-driven photodetector with respect to the n-Ga having only pn junction in comparative example 1 2 O 3 Sn/p-GaN self-driven ultraviolet photoelectric detectorThe device was tested for its optoelectronic properties 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 2.2X10 4 . FIG. 7 (b) is a repetitive photoresponse test under light of wavelength 355nm for a plurality of cycles, it can be seen that the photocurrent at the device suddenly increased to 1150nA with a photodarkening ratio of about 2.3X10 5 . By comparison of n-Ga with pn junction only 2 O 3 The photoelectric performance of the Sn/p-GaN self-driven ultraviolet photoelectric detector can be seen that the n-ZnO/n-Ga with heterogeneous nn junction and pn junction simultaneously 2 O 3 The Sn/p-GaN double-junction coupling type self-driven photoelectric detector has obviously improved photocurrent of the device no matter under the illumination with the wavelength of 255nm or 355 nm.
Calculation of n-ZnO/n-Ga by I-t curve 2 O 3 Response time of Sn/p-GaN double-junction coupling type self-driven photoelectric detector under the illumination of 255nm and 355nm wavelength respectively. As shown in FIG. 8 (a), under 255nm wavelength illumination, τ rise ＝0.31s，τ decay =0.39 s, τ under 355nm wavelength illumination as shown in fig. 8 (b) rise ＝0.04s，τ decay =0.06 s, the response speed of the device is fast. n-Ga having only pn junction in comparative example 1 2 O 3 The photoelectric performance of the Sn/p-GaN self-driven ultraviolet photoelectric detector can be seen as n-ZnO/n-Ga with double-junction coupling 2 O 3 The response time of the Sn/p-GaN device is shorter, so that the Sn/p-GaN device has 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 showed that the peak response of the device of example 1 was at 260nm and the responsivity was 178.24mA/W. By comparison of n-Ga 2 O 3 Sn/p-GaN device with double junction coupled n-ZnO/n-Ga 2 O 3 The responsivity of the Sn/p-GaN device is obviously improvedLifting.
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 detector prepared in example 1 of the present application, the detector prepared in comparative example 1, and the Ga-based materials reported in the prior literature 2 O 3 And comparing the self-driving performance parameters of the photoelectric detector of the material under the 0V bias. The results are shown in Table 1 below.
TABLE 1 self-driven detection Performance of different photodetectors at 0V bias
As can be seen by comparison of Table 1, n-ZnO/n-Ga-based 2 O 3 The Sn/p-GaN double-junction coupling type self-driven photoelectric detector has excellent performance, which shows that the superposition coupling of the heterogeneous nn junction and the pn junction is a promising method for improving the performance of the self-driven photoelectric detector.
The invention adopts PLD (pulsed laser deposition) technology to dope Ga with 1 mol% Sn 2 O 3 Target material and ZnO target material, substrate temperature is 500 ℃, and deposition oxygen pressure is 0Pa. To extend to c-Al 2 O 3 Deposition of n-Ga on p-GaN thin films 2 O 3 Sn film, then depositing a layer of ZnO film, and respectively preparing Ni/Au electrode and In electrode forming ohmic contact on the film by using vacuum evaporation so as to construct a novel n-ZnO/n-Ga 2 O 3 Sn/p-GaN double-junction coupling type self-driven ultraviolet photoelectric detectionA measuring device. 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 of the device, the device is discovered to be connected with n-Ga with pn junction only 2 O 3 n-ZnO/n-Ga coupled by superposition of built-in electric fields of heterogeneous nn and pn junctions, compared to Sn/p-GaN based devices 2 O 3 The Sn/p-GaN-based device performance is obviously improved: under the same illumination with 255nm wavelength, the device has faster response speed, obvious response improvement (135.46 mA/W is increased to 165.56 mA/W), and ultra-high detection rate (1.16X10) 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;
sn-doped n-type Ga 2 O 3 A thin film layer located on the surface of the p-type GaN thin film layer far from the substrate side, the Sn doped n-type Ga 2 O 3 Orthographic projection of the film layer on the surface of the p-type GaN film layer does not completely cover the p-type GaN film layer;
an n-type ZnO thin film layer positioned on the Sn-doped n-type Ga 2 O 3 The surface of the thin film layer far away from one side of the substrate;
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;
a second metal electrode layer positioned onThe p-type GaN film layer is not doped with the Sn and is doped with n-type Ga 2 O 3 The surface covered by the film layer.
2. The dual-junction coupled self-driven ultraviolet photodetector of claim 1, wherein said Sn-doped n-type Ga 2 O 3 The Sn doping mole content in the 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, an 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 Sn doped n-type Ga 2 O 3 The thickness of the 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 Sn-doped n-type Ga on a substrate 2 O 3 A thin film layer doped with n-type Ga 2 O 3 Thin film layer is arranged on the p-typeThe orthographic projection of the surface of the GaN film layer does not completely cover the p-type GaN film layer;
doping n-type Ga in Sn 2 O 3 Sequentially growing an n-type ZnO film layer and a first metal electrode layer on the film layer;
in the p-type GaN film layer and not doped with the Sn 2 O 3 And growing a second metal electrode layer on the surface covered by the film layer.
7. The method for manufacturing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 6, wherein the substrate is placed in a vacuum cavity of a deposition device, and a pulse laser deposition method is adopted to ablate the p-type GaN target material and the Sn-doped n-type Ga 2 O 3 The target material is sequentially deposited and grown on the substrate to obtain a p-type GaN film layer and Sn-doped n-type Ga 2 O 3 A thin film layer; 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 manufacturing the double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 6, wherein the ZnO target is ablated by adopting a pulse laser deposition method, and n-type Ga is doped in Sn 2 O 3 Depositing and growing on the 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.
9. The method for manufacturing a double-junction coupling type self-driven ultraviolet photoelectric detector according to claim 7, wherein the Sn-doped n-type Ga 2 O 3 The preparation method of the target comprises the following steps:
proportionally mixing SnO 2 Powder, ga 2 O 3 Ball milling and mixing the powder to obtain fine powder;
pressing the fine powder after ball milling into ceramic green sheets;
sintering the ceramic blank at 800-1300 ℃ to obtain Sn doped ceramicn-type Ga 2 O 3 And (3) a target material.
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 at 800-1300 ℃ for 2-5 h to obtain Sn doped n-type Ga 2 O 3 And (3) a target material.
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| US20040113156A1 (en) * | 2002-11-27 | 2004-06-17 | Matsushita Electric Industrial Co., Ltd. | Semiconductor light emitting device and method for fabricating the same |
| CN109427937A (en) * | 2017-08-31 | 2019-03-05 | 晶元光电股份有限公司 | Semiconductor device and method for manufacturing the same |
| 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 |
| CN116666487A (en) * | 2023-04-07 | 2023-08-29 | 复旦大学 | GaN/Ga with self-powered working mode 2 O 3 pn junction ultraviolet photoelectric detector and its preparing method |
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| US20040113156A1 (en) * | 2002-11-27 | 2004-06-17 | Matsushita Electric Industrial Co., Ltd. | Semiconductor light emitting device and method for fabricating the same |
| CN109427937A (en) * | 2017-08-31 | 2019-03-05 | 晶元光电股份有限公司 | Semiconductor device and method for manufacturing the same |
| 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 |
| CN116666487A (en) * | 2023-04-07 | 2023-08-29 | 复旦大学 | GaN/Ga with self-powered working mode 2 O 3 pn junction ultraviolet photoelectric detector and its preparing method |
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