CN112951683A - Photoelectric cathode and preparation method and application thereof - Google Patents
Photoelectric cathode and preparation method and application thereof Download PDFInfo
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- CN112951683A CN112951683A CN202110110372.XA CN202110110372A CN112951683A CN 112951683 A CN112951683 A CN 112951683A CN 202110110372 A CN202110110372 A CN 202110110372A CN 112951683 A CN112951683 A CN 112951683A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J1/00—Details of electrodes, of magnetic control means, of screens, or of the mounting or spacing thereof, common to two or more basic types of discharge tubes or lamps
- H01J1/02—Main electrodes
- H01J1/34—Photo-emissive cathodes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
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- H—ELECTRICITY
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- H01J40/00—Photoelectric discharge tubes not involving the ionisation of a gas
- H01J40/02—Details
- H01J40/04—Electrodes
- H01J40/06—Photo-emissive cathodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J9/00—Apparatus or processes specially adapted for the manufacture, installation, removal, maintenance of electric discharge tubes, discharge lamps, or parts thereof; Recovery of material from discharge tubes or lamps
- H01J9/02—Manufacture of electrodes or electrode systems
- H01J9/12—Manufacture of electrodes or electrode systems of photo-emissive cathodes; of secondary-emission electrodes
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Abstract
The invention discloses a photoelectric cathode and a preparation method and application thereof, wherein the photoelectric cathode comprises a substrate layer and a nano-pillar array formed on the surface of the substrate layer by etching; the surface of the nano-pillar array is provided with quantum dots and metal nano-particles. Light from different incident directions is effectively received, the light absorption area is increased by the quantum dots, and the light absorption is enhanced by the arrayed light traps; a direct transmission channel can be provided for photoelectrons in the radial direction, and the photoelectrons can easily run from the cathode body to the surface; the photoelectric conversion material has a large surface area, can effectively improve the surface escape probability of photoelectrons, and shows the characteristics of large photocurrent, high response speed and the like; meanwhile, metal particles such as gold and silver are modified on the surface, a plasma effect is generated on the surface of the quantum dot, and light absorption is promoted; the metal particles and the quantum dots form a heterojunction, so that the transmission of photoelectrons is promoted, and the photoelectric performance of the photocathode is effectively improved.
Description
Technical Field
The invention relates to the technical field of semiconductor photoelectric detectors, in particular to a photoelectric cathode and a preparation method and application thereof.
Background
The photocathode is based on an external photoelectric effect, and when light irradiates on the surface of a material, electrons in the material can escape from the surface of the material after enough photon energy is obtained. The negative electron affinity photocathode has the advantages of high quantum efficiency, small dark emission, adjustable long-wave threshold, large long-wave response expansion potential and the like, and the third-generation low-light-level image intensifier taking the negative electron affinity photocathode as the core greatly expands the long-wave threshold and the sight distance of a night vision instrument. The cathode performance parameters affecting the quantum efficiency of the photocathode mainly include the surface escape probability, the electron diffusion length and the recombination rate of the rear interface.
The conventional photocathode can only respond to incident light in one direction, the thickness of an emitting layer is increased in order to improve light absorption efficiency, so that photoelectrons need to run for a long distance in a body, the sensitivity of a device is low, and the recombination probability of the photoelectrons is high due to inevitable mismatch at the interface of a buffer layer and the emitting layer. On the other hand, in order to expand the response wavelength of the photocathode, a lattice-mismatched emission layer has to be introduced, and a large amount of dislocation cannot be introduced into the emission layer body, so that the photoelectron recombination probability is improved, and the improvement of the quantum efficiency of the traditional photocathode is limited.
Therefore, in order to expand the response wavelength of the photocathode and improve the quantum efficiency and the device sensitivity, a quantum dot and nano-pillar array composite structure photocathode with adjustable response wavelength, high quantum efficiency and high sensitivity is urgently needed.
Disclosure of Invention
The first technical problem to be solved by the invention is as follows: a photocathode having high quantum efficiency and high sensitivity.
The second technical problem to be solved by the invention is as follows: the preparation method of the photocathode.
The third technical problem to be solved by the invention is as follows: the application of the photocathode is provided.
In order to solve the first technical problem, the invention provides the following technical scheme: a photoelectric cathode comprises a substrate layer and a nano-pillar array formed on the surface of the substrate layer through etching; the nano-pillar array comprises a plurality of nano-pillars, and quantum dots and metal nano-particles grow on the surface of each nano-pillar.
According to some embodiments of the invention, the substrate layer is at least one of Ge, GaAs, InP, GaSb, Si, GaN, and sapphire.
According to some embodiments of the invention, the quantum dots are at least one of GaAs, InGaAs, InGaAsP, InGaSb, InGaN, and InAsSb.
According to some embodiments of the invention, the substrate layer is made of a material having a band gap width greater than a band gap width of the quantum dot matrix quantum dots.
According to some embodiments of the invention, the metal nanoparticles are at least one of gold nanoparticles and silver nanoparticles.
According to some embodiments of the invention, the height of the nanopillars is 200 to 3000nm and the diameter of the nanopillars is 50 to 500 nm.
According to some embodiments of the invention, the quantum dots have a diameter of 5 to 30 nm.
According to some embodiments of the invention, the metal nanoparticles have a diameter of 2 to 10 nm.
The quantum dots can grow mismatched structures, and the materials or components can be changed at will according to the needs. When the thickness of the epitaxial layer is less than the critical thickness, the lattice mismatch is coordinated and unified through the action of elastic strain, and then the epitaxial layer has a uniform structure and optimal electron optical characteristics. Meanwhile, the response cut-off wavelength of the photoelectric detector can be modulated by controlling the size of the quantum dots.
A critical thickness of about 100nm when the free lattice mismatch between the epitaxial layer and the substrate is about 0.01; a critical thickness of about 30nm when the free lattice mismatch between the epitaxial layer and the substrate is about 0.025; a critical thickness of about 10nm when the free lattice mismatch between the epitaxial layer and the substrate is about 0.055; the critical thickness is about 5nm when the free lattice mismatch between the epitaxial layer and the substrate is about 0.08. Wherein the free lattice mismatch is equal to the epitaxial layer lattice parameter minus the substrate lattice parameter divided by the substrate lattice parameter. For example, if the lattice mismatch between In0.3Ga0.7As and GaAs is about 0.022, then its critical thickness is about 40 nm; the lattice mismatch between In0.9Ga0.1As and InP is about 0.025, and the critical thickness is about 30 nm. Therefore, most epitaxial materials have a mismatch with the substrate of less than 0.025 nm, and the critical thickness can reach over 30nm, so long as the epitaxial dimension is less than 30 nm.
The photocathode provided by the embodiment of the invention has at least the following beneficial effects: the quantum dots grow on the surface of the nano-pillar array, and each nano-pillar and the surface quantum dots form a quantum dot matrix structure together; the quantum dot and nano-column array composite structure photocathode effectively receives light from different incident directions, the light absorption area is increased by the quantum dot, and the light absorption is enhanced by the arrayed light trap; a direct transmission channel can be provided for photoelectrons in the radial direction, and the photoelectrons can easily run from the cathode body to the surface; the photocathode has a large surface area, can effectively improve the surface escape probability of photoelectrons, and shows the characteristics of large photocurrent, high response speed and the like; meanwhile, metal particles such as gold and silver are modified on the surface, a plasma effect is generated on the surface of the quantum dot, and light absorption is promoted; the metal particles and the quantum dots form a heterojunction, so that the transmission of photoelectrons is promoted, and the photoelectric performance of the photocathode is effectively improved.
In order to solve the second technical problem, the invention provides the following technical scheme: a method for preparing the photocathode comprises the following steps:
s1, etching a nano-pillar array on the surface of the substrate layer;
s2, manufacturing quantum dots and metal nanoparticles on the surface of the nano-pillar array to obtain the photocathode.
According to some embodiments of the present invention, the manufacturing method of the nanopillar array in step S1 is a mask plasma etching method or a mask anisotropic wet etching method.
According to some embodiments of the present invention, the fabricating of the nanopillar array in step S1 is performed by performing a cleaning process, which includes:
(1) selecting acetone as a cleaning agent, and carrying out first ultrasonic cleaning;
(2) selecting ethanol as a cleaning agent, and performing secondary ultrasonic cleaning;
(3) selecting hydrochloric acid as a cleaning agent, and cleaning for the third time, wherein the cleaning time is 1-2 min;
(4) selecting BOE buffer etching liquid as a cleaning agent, and cleaning for the fourth time, wherein the cleaning time is 1-2 min;
(5) selecting water as cleaning agent, cleaning until no particles and residual solution exist, and drying.
The acetone and the ethanol are both organic solvents and are used for removing organic impurities; hydrochloric acid is used for removing oxides; the BOE buffer etching liquid is used for removing other impurities; the water is mainly used for removing other residual cleaning agents.
According to some embodiments of the invention, the BOE buffer etching solution is HF and NH4F, mixing the solution; preferably, the volume ratio of the hydrogen fluoride solution to the ammonium fluoride solution is 5-7: 1.
According to some embodiments of the invention, the drying method is nitrogen blow drying.
According to some embodiments of the present invention, the quantum dot manufacturing method in step S2 is one of vapor deposition (CVD), Metal Organic Chemical Vapor Deposition (MOCVD), or Molecular Beam Epitaxy (MBE).
According to some embodiments of the present invention, the temperature range during the quantum dot growth process in the step S2 is 400-700 ℃.
The quantum dots adopt proper growth temperature and growth rate in the growth process, and the growth temperature, growth rate and growth time depend on different growth modes, substrates, materials and quantum dot sizes.
According to some embodiments of the present invention, the method for manufacturing the metal nanoparticles in step S3 is a sol-gel method or a sputtering method.
In order to solve the third technical problem, the technical solution provided by the present invention is: the application of the photocathode in the photoelectric detector.
When a semiconductor material gradually decreases from a bulk phase to a nanometer scale of an electronic scale of the material, wherein the movement of carriers is limited by strong quantum closure, the structure of electrons also changes from a continuous energy band structure of the bulk phase to a fission energy level similar to atoms. When the energy of the incident photon is larger than the energy required for the electron in the quantum dot bound state to generate the excited transition, the electron in the quantum dot bound state is excited by the outside to transition from the original bound state to the excited state or the continuous state. The ground state bound energy of the quantum dots can be changed by controlling the size of the quantum dots, so that the response cut-off wavelength of the photoelectric detector is controlled.
Drawings
Fig. 1 is a schematic structural diagram of a photocathode according to a first embodiment of the present invention;
FIG. 2 is a partially enlarged structural view of the area A shown in FIG. 1;
FIG. 3 is a schematic view of a reflective photo-cathode structure according to a second embodiment of the present invention;
fig. 4 is a schematic structural diagram of a transmissive photocathode according to a third embodiment of the present invention.
Detailed Description
In order to explain technical contents, achieved objects, and effects of the present invention in detail, the following description is made with reference to the accompanying drawings in combination with the embodiments. The test methods used in the examples are all conventional methods unless otherwise specified; the materials, reagents and the like used are commercially available reagents and materials unless otherwise specified.
The first embodiment of the invention is as follows: the photocathode shown in FIG. 1 comprises an InP substrate layer and a nano-pillar array formed on the surface of the substrate layer by etching; the nano-pillar array comprises a plurality of nano-pillars, and In grows on the surface of each nano-pillar0.8GaAs quantum dots and Au nanoparticles. Wherein the height of the nano-column is 1000nm, and the diameter of the nano-column is 200 nm; in therein0.8The diameter of the GaAs quantum dot is 20 nm; the diameter of the Au nanoparticles was 5 nm.
The relative position relationship between the InGaAs quantum dots and the Au nanoparticles is shown in FIG. 2.
A method for preparing the photocathode with the quantum dot and nano-pillar array composite structure comprises the following steps:
s1, etching a nano-pillar array on the surface of the substrate layer by adopting a mask plasma etching method;
s2, selecting acetone as a cleaning agent, and carrying out first ultrasonic cleaning on the nano-pillar array; selecting ethanol as a cleaning agent, and carrying out secondary ultrasonic cleaning on the nano-pillar array; selecting hydrochloric acid as a cleaning agent, and cleaning the nano-column array for the third time, wherein the cleaning time is about 2 min; selecting BOE buffer etching liquid (the volume ratio of hydrogen fluoride solution to ammonium fluoride solution is 6:1) as a cleaning agent, and cleaning the nano-column array for the fourth time for about 2 min; selecting water as a cleaning agent, cleaning the nano-pillar array until no particles and residual solution exist, and drying the nano-pillar array by using nitrogen;
s3, growing quantum dots and metal nanoparticles on the surface of the nano-pillar array to obtain a photocathode; the production mode of the quantum dots is a metal organic chemical vapor deposition method, and the growth method of the metal nano particles is a sol-gel method.
The second embodiment of the invention is as follows: a photocathode as shown in fig. 3, which comprises a GaAs substrate layer and a nano-pillar array etched on the surface of the substrate layer; the surface of the nano-pillar array has In0.3GaAs quantum dots and Ag nanoparticles. Wherein the height of the nano-column is 2000nm, and the diameter of the nano-column is 300 nm; in therein0.3The diameter of the GaAs quantum dot is 30 nm; the diameter of the Ag nanoparticles was 8 nm.
The preparation method of this example is the same as that of the first example.
The third embodiment of the invention is as follows: the photocathode shown in fig. 4 comprises a GaSb substrate layer and a nano-pillar array formed on the surface of the substrate layer by etching; the surface of the nano-pillar array has In0.5GaSb quantum dots and Au nanoparticles. Wherein the height of the nano-column is 300nm, and the diameter of the nano-column is 50 nm; wherein the diameter of the InGaAs quantum dot is 10 nm; the diameter of the Au nanoparticles was 4 nm.
The preparation method of this example is the same as that of the first example.
When a semiconductor material gradually decreases from a bulk phase to a nanometer scale of an electronic scale of the material, wherein the movement of carriers is limited by strong quantum closure, the structure of electrons also changes from a continuous energy band structure of the bulk phase to a fission energy level similar to atoms. When the energy of the incident photon is larger than the energy required for the electron in the quantum dot bound state to generate the excited transition, the electron in the quantum dot bound state is excited by the outside to transition from the original bound state to the excited state or the continuous state. The ground state bound energy of the quantum dots can be changed by controlling the size of the quantum dots, so that the response cut-off wavelength of the photoelectric detector is controlled.
On the other hand, the quantum dots can grow mismatched structures, and the materials or components can be changed at will according to needs. When the thickness of the epitaxial layer is less than the critical thickness, the lattice mismatch is coordinated and unified through the action of elastic strain, and then the epitaxial layer has a uniform structure and optimal electron optical characteristics. Meanwhile, the response cut-off wavelength of the photoelectric detector can be modulated by controlling the size of the quantum dots.
In conclusion, the photocathode with the quantum dot and nano-pillar array composite structure provided by the invention effectively receives light from different incident directions, the light absorption area of the quantum dots is increased, and the light absorption of the arrayed light trap is enhanced; a direct transmission channel can be provided for photoelectrons in the radial direction, and the photoelectrons can easily run from the cathode body to the surface; the photocathode has a large surface area, can effectively improve the surface escape probability of photoelectrons, and shows the characteristics of large photocurrent, high response speed and the like; meanwhile, metal particles such as gold and silver are modified on the surface, a plasma effect is generated on the surface of the quantum dot, and light absorption is promoted; the metal particles and the quantum dots form a heterojunction, so that the transmission of photoelectrons is promoted, and the photoelectric performance of the photocathode is effectively improved. The above description is only an embodiment of the present invention, and not intended to limit the scope of the present invention, and all equivalent changes made by using the contents of the present specification and the drawings, or applied directly or indirectly to the related technical fields, are included in the scope of the present invention.
Claims (10)
1. A photocathode, comprising: the nano-pillar array comprises a substrate layer and a nano-pillar array formed on the surface of the substrate layer by etching; the nano-pillar array comprises a plurality of nano-pillars, and quantum dots and metal nano-particles grow on the surface of each nano-pillar.
2. A photocathode according to claim 1, wherein: the substrate layer is at least one of Ge, GaAs, InP, GaSb, Si, GaN and sapphire.
3. A photocathode according to claim 1, wherein: the quantum dots are at least one of GaAs, InGaAs, InGaAsP, InGaSb, InGaN and InAsSb.
4. A photocathode according to claim 1, wherein: the band gap width of the preparation material of the substrate layer is larger than that of the quantum dots.
5. A photocathode according to claim 1, wherein: the metal nanoparticles are at least one of gold nanoparticles and silver nanoparticles.
6. A photocathode according to claim 1, wherein: the height of the nano column is 200-3000 nm, and the diameter of the nano column is 50-500 nm.
7. A photocathode according to claim 1, wherein: the diameter of the quantum dot is 5-30 nm.
8. A photocathode according to claim 1, wherein: the diameter of the metal nanoparticles is 2-10 nm.
9. A method of preparing the photocathode of any one of claims 1 to 8, characterized in that: comprises the following steps:
s1, etching a nano-pillar array on the surface of the substrate layer;
s2, manufacturing quantum dots and metal nanoparticles on the surface of the nano-pillar array to obtain the photocathode.
10. Use of a photocathode according to any one of claims 1 to 8 in a photodetector.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114944438A (en) * | 2022-06-08 | 2022-08-26 | 绍兴埃鼎智能科技有限公司 | Novel photoelectric device |
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| CN107507901A (en) * | 2017-07-31 | 2017-12-22 | 南方科技大学 | LED photoelectric device based on surface plasmon enhancement and preparation method thereof |
| CN107583642A (en) * | 2017-09-15 | 2018-01-16 | 合肥师范学院 | Graphene quantum dot loaded Ag TiO2The preparation method of nano-array |
| CN111939935A (en) * | 2020-08-18 | 2020-11-17 | 合肥工业大学 | SnS2Quantum dot/Si binary nano array photoelectric catalyst and preparation method thereof |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103325663A (en) * | 2012-03-23 | 2013-09-25 | 北京邮电大学 | Preparation method of composite nanofiltration heterostructure capable of generating quantum dots on side wall of nanowire |
| CN106486560A (en) * | 2016-11-08 | 2017-03-08 | 电子科技大学 | Plasma drop epitaxial GaAs quantum dot solar battery and its manufacture method |
| CN107507901A (en) * | 2017-07-31 | 2017-12-22 | 南方科技大学 | LED photoelectric device based on surface plasmon enhancement and preparation method thereof |
| CN107583642A (en) * | 2017-09-15 | 2018-01-16 | 合肥师范学院 | Graphene quantum dot loaded Ag TiO2The preparation method of nano-array |
| CN111939935A (en) * | 2020-08-18 | 2020-11-17 | 合肥工业大学 | SnS2Quantum dot/Si binary nano array photoelectric catalyst and preparation method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114944438A (en) * | 2022-06-08 | 2022-08-26 | 绍兴埃鼎智能科技有限公司 | Novel photoelectric device |
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Application publication date: 20210611 |