CN1632898A - Middle concentration P-type doping transmission type gallium arsenide optical cathode material and method for preparing same - Google Patents

Middle concentration P-type doping transmission type gallium arsenide optical cathode material and method for preparing same Download PDF

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CN1632898A
CN1632898A CN 200310121794 CN200310121794A CN1632898A CN 1632898 A CN1632898 A CN 1632898A CN 200310121794 CN200310121794 CN 200310121794 CN 200310121794 A CN200310121794 A CN 200310121794A CN 1632898 A CN1632898 A CN 1632898A
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gaas
photocathode material
beryllium
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CN100426439C (en
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王晓峰
曾一平
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Institute of Semiconductors of CAS
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Abstract

This invention relates to semi-conductor material technique used in transparent negative electron affinity gallium arsenide light negative electrode device. This invention source area has two layers of inner layer and surface layer, wherein the inner layer has a window layer outside ad the outside of the surface layer is Se or oxygen actuating layer. The source inner layer is mixed with 1-8x10#+[18]cm#+[-3] in middle concentration and the surface layer is mixed with 5x10#+[16]-1x10#+[17]cm#+[-3] in low concentration.

Description

Middle concentration P type doping transmission-type GaAs photocathode material and preparation method thereof
Technical field
The present invention relates to the semi-conducting material technology, particularly a kind of middle concentration P type doping transmission-type GaAs (GaAs) photocathode material and technology of preparing thereof are used for transmission-type negative electron affinity (NEA) GaAs (GaAs) photocathode device.
Background technology
At present, the level of China's development transmission-type negative electron affinity GaAs photocathode device is: photoelectric sensitivity can reach 1200 μ A/lm.These data and the 3200 μ A/lm that report in the world have very big gap.According to another latest report, the minority diffusion length of external photocathode material can reach 7 μ m.These data show, no matter be device or material, domestic all have sizable gap with comparing abroad.
Because the existence of surface state, the pinning of surface level, P p type gallium arensidep material form very dark downward band curvature after caesium/oxygen activates, so that vacuum level is positioned at below the conduction level on surface, have promptly formed the negative electron affinity surface.The photoelectricity work function on negative electron affinity surface is more much smaller than the photoelectricity work function on positron affinity surface, so the quantum efficiency of negative electron affinity photoemissive material is more much bigger than common photoemissive material.In order to utilize band curvature to obtain best photoelectric emission, not only need the band curvature amount big as much as possible, also need the distance of band curvature and activated surface short as much as possible.This is because influence an energy loss that principal element is the band curvature district of negative electron affinity photocathode material photoelectric emission efficient.When the energy of incident light during greater than the energy gap of P p type gallium arensidep, the electronics on the valence band will be excited on the conduction band.The thermalization in conduction band soon of light activated electronics falls at the bottom of the conduction band then.Near at the bottom of the conduction band, their life-span is quite grown (minority carrier lifetime, 10 -9S).Therefore, they to be diffused into the probability at edge in band curvature district very high.As long as off-energy not when passing the band curvature district, the probability of their effusion vacuum is just very high.But under the effect of band curvature district internal electric field, the energy of electronics increases, and thermoelectronic effect is obvious, and scattering strengthens, and photoelectronic energy loss is very big.In order to reduce energy loss, improve the photoelectric sensitivity of device, often adopt high mixing to reduce the thickness in band curvature district.Height is mixed concentration often 8 * 10 18Cm -3(even 10 19Cm -3) more than, the THICKNESS CONTROL that makes the band curvature district in escape depth (about 20nm), thereby guarantee photoelectronic high escape probability.
But the result of making is based upon on the character basis of sacrificial light cathode material itself like this.The minority carrier lifetime of semi-conducting material and doping content are inversely proportional to.Doping content is high more, and defective that material forms in growth course and dislocation are many more, and minority carrier life time is short more, and minority diffusion length is short more.
From top analysis as can be seen, the bottleneck of transmission-type GaAs (GaAs) photocathode material structural design is the contradiction between surperficial highly doped requirement and the inner low-doped requirement.
In order to satisfy the requirement of this two aspect, the someone proposes to carry out at material internal low-doped, and carries out highly doped on the surface.According to band theory, we know that it is infeasible doing like this.And practice proves that also this method is impracticable.Low-doped in the body, the concentration gradient of surperficial highly doped formation will form an electronic barrier in being with, thereby will stop photoelectronic diffusion.The somebody proposes to add reverse biased on device, the direct light electronics that is used for by external electric field carries out directed movement, thereby reduces backscattering, improves minority diffusion length and photoelectron escape probability.In order on photocathode, to prepare Ohmic electrode, before caesium/oxygen activation technology, must on photocathode material, plate the very thin metal A g of (steaming) one deck earlier.The activation efficiency of silver-caesium-oxygen (Ag-Cs-O) photocathode is low, and the photoelectric sensitivity of photocathode is low.
Take all factors into consideration, present transmission-type GaAs (GaAs) photocathode still adopts uniform P type height to mix (high 18 orders of magnitude) GaAs and makes active area.
Summary of the invention
The objective of the invention is to improve the performance of photocathode device, on existing material growth technique, activation technology and device preparation technology basis, by changing the structure of transmission-type GaAs photocathode material, improve the photoelectric sensitivity of transmission-type negative electron affinity GaAs photocathode breakthroughly.
For achieving the above object, the present invention proposes a kind of middle concentration P type doping transmission-type GaAs photocathode material and preparation method thereof.The core component of GaAs photocathode material is an active area, forms the negative electron affinity surface after caesium/oxygen activates.GaAs active area of the present invention has two-layer: internal layer and superficial layer.Internal layer is middle doped in concentrations profiled, and superficial layer is a low concentration doping; The outside of internal layer is a Window layer, and the outside of superficial layer is an active coating.
Concentration and low concentration doping are with respect to high-concentration dopant (〉=8 * 10 in described 18Cm -3).The scope of middle doped in concentrations profiled is 1~8 * 10 18Cm -3, the scope of low concentration doping is 5 * 10 16~1 * 10 17Cm -3
Described photocathode material realizes that by molecular beam epitaxy technique P type doped source is beryllium (Be).The structure of photocathode material is epitaxial growth gallium aluminium arsenic-GaAs (Al on gallium arsenide substrate XGa 1-XAs/GaAs) double-heterostructure, the GaAs buffer layer of promptly on gallium arsenide substrate, growing successively, gallium aluminium arsenic reaction barrier layers, GaAs active area and algaas window layer.
Described photocathode material, its gallium arsenide substrate can be semi-insulating GaAs substrate or P p type gallium arensidep substrate or n p type gallium arensidep substrate; GaAs buffer layer does not mix; Gallium aluminium arsenic reaction barrier layers carries out beryllium (Be) doping or does not carry out beryllium (Be) and mix; GaAs active area internal layer is middle doped in concentrations profiled: 1~8 * 10 18Cm -3, superficial layer is a low concentration doping: 5 * 10 16~1 * 10 17Cm -3Algaas window layer carries out beryllium (Be) doping or does not carry out beryllium (Be) and mix.
Described photocathode material is to prepare transmission-type photocathode device by being inverted technology.Its described inversion technology is that algaas window layer is sealed on the optical window material, by chemically treated method gallium arsenide substrate and gallium aluminium arsenic reaction barrier layers are eroded, then such structure is introduced in the special ultra high vacuum device, the surfaces of active regions layer is carried out thermal cleaning and caesium/oxygen activation processing, form the negative electron affinity surface at last.
Described photocathode device comprises vacuum ballistic device and vacuum photoelectricity direct imaging device.Described vacuum ballistic device is photoelectric tube, photomultiplier; Vacuum photoelectricity direct imaging device is image intensifier tube, image converter tube.
Described photocathode material is realized by molecular beam epitaxy technique.The growth conditions of material is: the growth temperature of gallium arsenide layer (being resilient coating and active area) is 560~590 ℃; The thickness of GaAs buffer layer is about 100~300nm; The surface layer thickness of GaAs active area is 5~15nm, and interior layer thickness is 1~2 μ m; The growth temperature of algaas layer (being reaction barrier layers and Window layer) is higher 10~50 ℃ than the growth temperature of GaAs; The thickness of gallium aluminium arsenic reaction barrier layers is 0.5~1.5um; The thickness of algaas window layer is at 0.5~2 μ m; Wherein the content of al composition is x=0.15~0.65.The different doping content of GaAs active area is to realize by the source oven temperature degree that changes doping beryllium source.During doped in concentrations profiled, the temperature of beryllium (Be) source stove is controlled at 800~950 ℃; During low concentration doping, the temperature of beryllium (Be) source stove is controlled at 700~800 ℃.
Described molecular beam epitaxy technique has adopted the interface to pause and the gradual method of underlayer temperature when gallium aluminium arsenic and GaAs interface growth, has guaranteed GaAs/gallium aluminium arsenic monoatomic layer interfaces transition.During the interface of growth internal layer of active area and superficial layer, adopt the interface to pause, mix again after waiting the temperature of doped source stove to be reduced to desired temperature simultaneously, can avoid the diffusion of beryllium (Be), to form precipitous concentration gradient interface at the interface.
This band structure with middle doped in concentrations profiled transmission-type GaAs photocathode of double-layer structure has special character.This material structure utilizes band curvature that concentration gradient forms and limited surface layer thickness, the band curvature district is limited in the escape depth (about 20nm), thereby satisfied the requirement of device to the minority diffusion length grown and high effusion efficient simultaneously.
The band curvature that doped in concentrations profiled and superficial layer low concentration doping form in the active area internal layer is downward, activates the back because the band curvature direction that the surface level pinning forms is identical with superficial layer, so formed the accumulation layer of electronics near superficial layer.The band curvature district that concentration gradient and surface level pinning form is distributed in the superficial layer near interface of whole superficial layer and internal layer, and two parts overlap on together, all have strong electric field strength (10 5The V/cm order of magnitude); And total band curvature district≤20nm.
This material structure passes through the width in control surface band curvature district artificially, makes the band curvature district on low concentration doping surface be limited in a very narrow space, has farthest reduced the influence of thermoelectronic effect to photoelectron effusion efficient.In addition, the strong internal electric field of band curvature formation helps the raising of photoelectron effusion efficient.
The characteristics of this material structure are: on the one hand, owing to realized surperficial low concentration doping, thus reduced the doping content in the body as much as possible, help improving the minority diffusion length of material; On the other hand, near the strong internal electric field that forms material surface quickens photoelectron, makes the probability of photoelectron tunnelling effusion vacuum increase.
The present invention mixes the GaAs photocathode material with the even P type height that adopts at present and compares, and doping content is low, and defective and dislocation that material forms in epitaxial process are few, and perfection of lattice is good, the crystal mass height.Correspondingly, the life-span of minority carrier will prolong, and minority diffusion length will increase, and the probability that photoelectron is diffused into the band curvature area edge will improve.The doping content on doping content in the body and surface differs 1~2 order of magnitude, and the electric field strength in the band curvature district that band curvature district that concentration gradient forms and surface level pinning form is all 10 5The V/cm order of magnitude.In the band curvature district, photoelectronic drift speed is greater than diffusion rate, and internal electric field quickens photoelectron is directed forward, has reduced photoelectronic backscattering, greatly improve photoelectronic escape probability.From top analysis as can be seen, probability and photoelectronic escape probability that photoelectron is diffused into the band curvature area edge all will be improved, and the photoelectric sensitivity of transmission-type negative electron affinity GaAs photocathode will have breakthrough raising.
The structure diagram of description of drawings Fig. 1 transmission-type negative electron affinity photocathode; Wherein, (a) material growth structure schematic diagram; (b) be inverted process schematic representation;
The operation principle schematic diagram of concentration P type undoped gallium arsenide (GaAs) photocathode among Fig. 2;
The band structure schematic diagram of concentration P type undoped gallium arsenide (GaAs) photocathode among Fig. 3.
Embodiment
Below in conjunction with Fig. 1, Fig. 2, Fig. 3 describe CONSTRUCTED SPECIFICATION and the working condition according to concentration P type doping transmission-type GaAs (GaAs) photocathode material in the concrete enforcement of the present invention in detail.
The preparation of transmission-type photocathode has utilized inversion technology.Because the very thin thickness (about 2 μ m) of P p type gallium arensidep active area must have a supporter.At first, utilize molecular beam epitaxy (MBE) gallium aluminium arsenic-GaAs double-heterostructure (the growth structure schematic diagram is seen Fig. 1 (a)) of on gallium arsenide substrate, growing.Then this structure is inverted heat-sealing on the optical window material, the optical window material is as the supporter (be inverted technology and see Fig. 1 (b)) of active area.After being inverted heat-sealing, carry out series of chemical treatments, gallium arsenide substrate is all eroded up to reaction barrier layers.Such inverted structure is incorporated in the special ultra high vacuum device, the GaAs activated surface is carried out thermal cleaning and caesium/oxygen (Cs/O) activation, to form the negative electron affinity surface.
For guaranteeing the precision control of component, thickness and doping, need accurately control growth furnace temperature and underlayer temperature.In order to obtain complete, precipitous doped interface, when interface growth, adopted the interface to pause and the gradual method of underlayer temperature, guaranteed GaAs/gallium aluminium arsenic monoatomic layer interfaces transition.Middle doped in concentrations profiled need be raised to the doped source stove higher temperature, the temperature of doped source stove need be reduced during low concentration doping.Pause in the employing interface, and etc. the temperature of doped source stove mix again after being reduced to desired temperature, can avoid the diffusion of beryllium (Be), to form precipitous concentration gradient interface at the interface.
Sample generates substrate can adopt semi-insulated gallium arsenide substrate or P p type gallium arensidep substrate or n p type gallium arensidep substrate.Before substrate carries out molecular beam epitaxial growth, must carry out a series of clean, comprise deoil, burn into flushing and dried up for four steps.Press the order of ethanol-acetone-trichloroethylene-acetone-ethanol, substrate is immersed in the above-mentioned organic solvent successively, water-bath ebuillition of heated 3~5 minutes is rinsed well repeatedly with deionized water then.Corrosive liquid is H 2SO 4: H 2O 2: H 2O=5: 1: 1, etching time was 3~5 minutes.Then, rinse well repeatedly with deionized water.The aluminium delivery of packing into after with nitrogen substrate being dried up is gone into Sample Room and is prepared growth.
Substrate carries out the low temperature degasification at Sample Room, and temperature is 150~250 ℃; Send into pretreatment chamber then and carry out high-temperature degassing, 400~450 ℃ of temperature; Send into the growth room at last.Before growth, also need to carry out the deoxygenated layer and handle.Usually the exfoliation temperature of gallium arsenide substrate surface oxide layer is at 560~590 ℃.Can determine that according to the infrared temperature of substrate and the variation of high-energy electron diffiraction (RHEED) pattern whether oxide layer comes off, the decomposition of oxide layer shows as high-energy electron diffiraction (RHEED) is converted into GaAs by oxide layer circular 2 * 4 structure stripeds again.So far, just epitaxial growth can have been begun.
The growth temperature of gallium arsenide layer is at 560~590 ℃.The growth temperature of algaas layer is higher 10~50 ℃ than the growth temperature of gallium arsenide layer.Algaas layer (Al xGa 1-xAs) content of al composition is x=0.15-0.65 in.The thickness t of GaAs buffer layer 1About 100-300nm.Gallium aluminium arsenic reaction barrier layers t 2Thickness at 0.5-1.5um, Window layer t 3Thickness at 0.5-2 μ m.
Present embodiment selects the doping content and the growth thickness of GaAs active area to be respectively: the doping content N of superficial layer 1Be 5 * 10 16~1 * 10 17Cm -3, growth thickness Y 1Be 5~15nm, source oven temperature degree T 1It is 700~800 ℃; The doping content N of internal layer 2Be 1~8 * 10 18Cm -3, growth thickness Y 2Be 1~2 μ m, source oven temperature degree T 2It is 800~950 ℃.Consider that activation technology need clean and the processing of deoxidation layer, growth thickness Y material 1Can grow into about 30nm.
GaAs buffer layer does not mix.Gallium aluminium arsenic reaction barrier layers and Window layer can be mixed, and also can not mix.
The photocathode material of above-mentioned growth is inverted heat-sealing on the optical window material, after caesium/oxygen activates the surfaces of active regions layer, generates the negative electron affinity surface.The operation principle schematic diagram of middle concentration P type undoped gallium arsenide (GaAs) photocathode is seen Fig. 2.Survey light from the one side incident of active area internal layer, the electronics of active area inside obtains enough energy, overcomes surface potential barrier and is transmitted into the vacuum from the little caesium of work function/oxygen activated surface.Photoelectric tube, photomultiplier equal vacuum ballistic device and image intensifier tube, image converter tube equal vacuum photoelectricity direct imaging device all utilize this external photoelectric effect to realize opto-electronic conversion.
Fig. 3 is the band structure schematic diagram of middle doped in concentrations profiled GaAs (GaAs) photocathode.As can be seen from Figure 3, because the doping content of surfaces of active regions layer is lower than the doping content of active area internal layer, so near the band curvature superficial layer is downward.When caesium/oxygen (Cs/O) activates, because the band curvature that the surface level pinning forms also is downward.Concentration gradient and caesium/oxygen (Cs/O) activate the band curvature district that forms and overlap on together.Total band curvature sector width is x, at the x that is distributed as of active area internal layer 2, at the x that is distributed as of surfaces of active regions layer 1(x 1=Y 1).As long as total band curvature sector width x is limited in the 20nm, less than photoelectronic escape depth (about 20nm), thermoelectronic effect just can be ignored to the influence of photoelectron effusion efficient.The electric field strength E of surfaces of active regions layer and internal layer 1, E 2All 10 5The V/cm order of magnitude.Under so strong electric field action, photoelectron was subjected to directed the acceleration before the tunnelling active coating, and escape probability will increase greatly.

Claims (16)

1. concentration P type doping transmission-type GaAs photocathode material in a kind, it is characterized in that the active differentiation of photocathode material is two-layer: internal layer and superficial layer, active area internal layer are middle doped in concentrations profiled, superficial layer is a low concentration doping; The outside of internal layer is a Window layer, and the outside of superficial layer is an active coating.
2. GaAs photocathode material as claimed in claim 1 is characterized in that, the middle doped in concentrations profiled scope of active area internal layer is 1~8 * 10 18Cm -3, the low concentration doping scope of superficial layer is 5 * 10 16~1 * 10 17Cm -3
3. photocathode material as claimed in claim 1 is characterized in that, its surface energy band buckled zone is divided into band curvature district and superficial layer band curvature district two parts of internal layer, and two parts overlap on together, all has highfield intensity; And total band curvature district≤20nm.
4. photocathode material as claimed in claim 3 is characterized in that, the internal electric field that described two parts band curvature district has, and its electric field strength is all 10 5The V/cm order of magnitude.
5. concentration P type doping transmission-type GaAs photocathode material preparation method in a kind is characterized in that, growth realizes that by molecular beam epitaxy technique P type doped source is a beryllium.
6. photocathode material preparation method as claimed in claim 5 is characterized in that described growth is by molecular beam epitaxy technique, epitaxial growth gallium aluminium arsenic-GaAs double-heterostructure on gallium arsenide substrate.
7. photocathode material preparation method as claimed in claim 6 is characterized in that, described gallium aluminium arsenic-GaAs double-heterostructure, be on gallium arsenide substrate, growth successively: GaAs buffer layer, gallium aluminium arsenic reaction barrier layers, GaAs active area and algaas window layer.
8. photocathode material preparation method as claimed in claim 7 is characterized in that, the growth conditions of described GaAs buffer layer and active area is: growth temperature is at 560~590 ℃; Wherein the thickness of GaAs buffer layer is about 100~300nm; The thickness of GaAs active area internal layer is 1~2 μ m, and the thickness of superficial layer is 5~15nm.
9. photocathode material preparation method as claimed in claim 7 is characterized in that, the growth conditions of described reaction barrier layers and Window layer is: growth temperature is higher 10~50 ℃ than the growth temperature of GaAs buffer layer and active area; Thickness 0.5~the 1.5um of gallium aluminium arsenic reaction barrier layers 1The thickness of gallium aluminium arsenic window is at 0.5~2 μ m; The content of al composition is x=0.15~0.65.
10. photocathode material preparation method as claimed in claim 7 is characterized in that, described gallium arsenide substrate can be semi-insulating GaAs substrate or P p type gallium arensidep substrate or n p type gallium arensidep substrate; GaAs buffer layer does not mix; Gallium aluminium arsenic reaction barrier layers carries out the beryllium doping or does not carry out beryllium and mix; GaAs active area internal layer is that middle concentration beryllium mixes 1~8 * 10 18Cm -3, superficial layer mixes 5 * 10 for the low concentration beryllium 16~1 * 10 17Cm -3Algaas window layer carries out the beryllium doping or does not carry out beryllium and mix.
11., it is characterized in that during middle doped in concentrations profiled, the temperature of beryllium source stove is controlled at 800~950 ℃ as claim 1 or 10 described photocathode material preparation methods; During low concentration doping, the temperature of beryllium source stove is controlled at 700~800 ℃.
12. photocathode material preparation method as claimed in claim 5 is characterized in that, has adopted the interface to pause and the gradual method of underlayer temperature when interface growth, has guaranteed GaAs/gallium aluminium arsenic monoatomic layer interfaces transition.
13. photocathode material preparation method as claimed in claim 12, it is characterized in that, adopt the interface to pause, mix again after waiting the doped source furnace temperature to be reduced to desired temperature simultaneously, can avoid the diffusion of beryllium, to form precipitous concentration gradient interface at the interface.
14. photocathode material preparation method as claimed in claim 5 is characterized in that, is to prepare transmission-type photocathode device by being inverted technology, comprises vacuum ballistic device and vacuum photoelectricity direct imaging device.
15. photocathode material preparation method as claimed in claim 14 is characterized in that, is to be inverted heat-sealing on the optical window material by Window layer, utilizes corrosion technology that substrate and reaction barrier layers are removed then, at last the surfaces of active regions layer is activated.
16. photocathode material preparation method as claimed in claim 15 is characterized in that, the activation of described surfaces of active regions layer activates by caesium/oxygen and to form the negative electron affinity surface.
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CN103123885A (en) * 2013-01-24 2013-05-29 中国电子科技集团公司第五十五研究所 Variable doping structure of transmission-type photoelectric cathode material for enhancing thermal stability
CN103295855A (en) * 2013-05-29 2013-09-11 南京理工大学 Index-doped reflecting-type GaAs (gallium arsenide) photoelectric cathode and production method thereof
CN104112633A (en) * 2014-07-23 2014-10-22 四川天微电子有限责任公司 GaAs photoelectric cathode activation process
CN107622930A (en) * 2017-08-25 2018-01-23 北方夜视技术股份有限公司 Microchannel template photomultiplier, bialkali photocathode and the preparation method of high-quantum efficiency
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CN103123885A (en) * 2013-01-24 2013-05-29 中国电子科技集团公司第五十五研究所 Variable doping structure of transmission-type photoelectric cathode material for enhancing thermal stability
CN103123885B (en) * 2013-01-24 2015-04-15 中国电子科技集团公司第五十五研究所 Variable doping structure of transmission-type photoelectric cathode material for enhancing thermal stability
CN103295855A (en) * 2013-05-29 2013-09-11 南京理工大学 Index-doped reflecting-type GaAs (gallium arsenide) photoelectric cathode and production method thereof
CN104112633A (en) * 2014-07-23 2014-10-22 四川天微电子有限责任公司 GaAs photoelectric cathode activation process
CN107622930A (en) * 2017-08-25 2018-01-23 北方夜视技术股份有限公司 Microchannel template photomultiplier, bialkali photocathode and the preparation method of high-quantum efficiency
CN107622930B (en) * 2017-08-25 2018-10-30 北方夜视技术股份有限公司 Microchannel template photomultiplier, bialkali photocathode and the preparation method of high-quantum efficiency
CN107895681A (en) * 2017-12-06 2018-04-10 中国电子科技集团公司第十二研究所 A kind of photocathode and preparation method thereof

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