CN105789399B - P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof - Google Patents

P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof Download PDF

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CN105789399B
CN105789399B CN201610286126.9A CN201610286126A CN105789399B CN 105789399 B CN105789399 B CN 105789399B CN 201610286126 A CN201610286126 A CN 201610286126A CN 105789399 B CN105789399 B CN 105789399B
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type
zno
substrate
injection layer
hole injection
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CN105789399A (en
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杜国同
夏晓川
梁红伟
董鑫
包俊飞
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Jinhua Jida Photoelectric Technology Research Institute Co Ltd
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/02Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
    • H01L33/14Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a carrier transport control structure, e.g. highly-doped semiconductor layer or current-blocking structure
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/005Processes
    • H01L33/0083Processes for devices with an active region comprising only II-VI compounds
    • H01L33/0087Processes for devices with an active region comprising only II-VI compounds with a substrate not being a II-VI compound
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/02Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
    • H01L33/26Materials of the light emitting region
    • H01L33/28Materials of the light emitting region containing only elements of Group II and Group VI of the Periodic Table

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  • Manufacturing & Machinery (AREA)
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Abstract

The invention belongs to light emitting semiconductor device and its preparing technical field, is related to several p-type broad stopbands oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof.Device is formed by substrate, in the n ZnO luminescent layers of substrate Epitaxial growth, the hole injection layer prepared on n ZnO luminescent layers, the Top electrode prepared on hole injection layer, the bottom electrode that is prepared below substrate successively, it is characterised in that:Substrate is the conductive Si single-chips of n-type, and hole injection layer is p-type broad stopband oxide semiconductor film materials, and thickness range is 200nm~2000nm, and carrier (hole) concentration range is 2 × 1017~5 × 1019/cm3.The present invention can solve ZnO material p-type doping difficult problem, while device is simple using vertical stratification technique, can further expand the application of device.

Description

P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof
Technical field
The invention belongs to light emitting semiconductor device and its preparing technical field, and in particular to a kind of p based on zno-based material Molded breadth forbidden band oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof.
Background technology
GaN material has wider application prospect in solid-state illumination field.ZnO and GaN band gap and lattice is normal Number is sufficiently close to, and has close photoelectric characteristic.But compared with GaN, there is ZnO higher fusing point and exciton bind energy, exciton to increase Benefit is higher, epitaxial growth temperature is low, cost is low, easy etching and make to be easier the processing of the rear road of epitaxial wafer, make the system of device For more convenient etc..Therefore, the luminescent device such as zno-based luminous tube, laser, which is succeeded in developing, is possible to substitution or part substitution GaN Base photoelectric device, bigger application prospect is had, particularly ZnO is purple, ultraviolet light photo device more people are paid attention to.
But due to undoped with ZnO material be often presented that n-type is conductive (being labeled as n-ZnO), and its carrier (electronics) is dense Degree generally 5 × 1017~2 × 1019/cm3, therefore p-type ZnO material is difficult to prepare.At present it has been reported that some p-types ZnO materials Expect that technology of preparing is all also immature, thus prepare ZnO material p-n junction luminescent device and also have any problem.In order to overcome zno-based photophore This of part is difficult, the present invention propose several other p-type broad stopbands oxides and n-type ZnO combination vertical structure light-emitting devices and Its preparation method.
Because have some broad stopband oxide semiconductor materials undoped with when be exactly p-type material, just as ZnO undoped with when just That n-type material is the same, these undoped with broad stopband oxide semiconductor material its carrier (hole) concentration up to 2 × 1017 ~2 × 1018/cm3If further carry out p-type doping (different material institute dopings is different), its carrier (hole) concentration It can further improve, can be up to 5 × 1017~5 × 1019/cm3, such as NiO, CuO material.It can be seen that such some broad stopband oxide materials Material is easier to be prepared into the conductive p-type semiconductor material of high hole, and easily and p-n junction type photophore is prepared in n-type ZnO combinations Part.
The content of the invention
The purpose of the present invention is exactly to adulterate difficult problem to solve ZnO material p-type, utilizes other p-type broad stopbands oxide P-n junction type luminescent device is prepared in semi-conducting material and n-type ZnO combinations, while in order to simplify device preparation technology, is reduced into This, substrate is prepared into vertical stratification using the conductive Si monocrystal materials of n-type, device.
P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices designed by the present invention is (see accompanying drawing 1 and accompanying drawing Illustrate), successively by substrate 1, on substrate 1 the n-ZnO luminescent layers 2 of epitaxial growth, the hole prepared on n-ZnO luminescent layers 2 Implanted layer 3, the Top electrode 4 prepared on hole injection layer 3, the lower surface of substrate 1 prepare bottom electrode 5 form, its feature exists In:Substrate 1 is that (its carrier (electronics) concentration range is 5 × 10 to the conductive Si single-chips of n-type17~2 × 1019/cm3), hole Implanted layer 3 is p-type broad stopband oxide semiconductor film materials, and thickness range is 200nm~2000nm, and carrier (hole) is dense It is 2 × 10 to spend scope17~5 × 1019/cm3
Further in order to utilize our MOCVD techniques, of the invention and specific proposition hole injection layer 3 is that p-type NiO is thin The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices of membrane material, successively by substrate 1, on substrate 1 extension life Long n-ZnO luminescent layers 2, the hole injection layer 3 prepared on n-ZnO luminescent layers 2, the upper electricity prepared on hole injection layer 3 Pole 4, the bottom electrode 5 prepared in the lower surface of substrate 1 are formed, it is characterised in that:Substrate 1 is the conductive Si single-chips of n-type, and hole is noted It is p-type NiO thin-film materials to enter layer 3.
Also specific p-type broad stopband oxide and the ZnO combination for proposing hole injection layer 3 as p-type CuO thin-film materials of the present invention Vertical structure light-emitting device, successively by substrate 1, on substrate 1 the n-ZnO luminescent layers 2 of epitaxial growth, on n-ZnO luminescent layers 2 The hole injection layer 3 of preparation, the Top electrode 4 prepared on hole injection layer 3, the structure of bottom electrode 5 prepared in the lower surface of substrate 1 Into, it is characterised in that:Substrate 1 is the conductive Si single-chips of n-type, and hole injection layer 3 is p-type CuO thin-film materials.
Further for the p-type Ga prepared using us2O3Technique (the patent No.:ZL201310414275.5), propose again Hole injection layer 3 is p-type Ga2O3The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices of thin-film material, successively by The n-ZnO luminescent layers 2 of substrate 1, on substrate 1 epitaxial growth, the hole injection layer 3 prepared on n-ZnO luminescent layers 2, in sky The Top electrode 4 prepared on cave implanted layer 3, the bottom electrode 5 prepared in the lower surface of substrate 1 are formed, it is characterised in that:Substrate 1 is n-type Conductive Si single-chips, hole injection layer 3 is p-type Ga2O3Thin-film material.
The preparation method of p-type broad stopband of the present invention oxide and ZnO combination vertical structure light-emitting devices, its feature It is:Using MOCVD, (metal has for n-ZnO luminescent layers 2 and p-type broad stopband oxide semiconductor film materials hole injection layer 3 Chemical machine is vapor-deposited) it is prepared by method.
Comprise the following steps that:
1) MOCVD methods, the ZnO described in particularly with Chinese patent 02100436.6 and ZL200410011164.0 are used The special growth MOCVD device of film and its technique on the conductive Si single crystalline substrates piece 1 of n-type growth undoped with n-ZnO light Layer 2, its thickness is 300~800nm, and its carrier (electronics) concentration is 5 × 1017~2 × 1019/cm3
2) MOCVD methods are used again, it is particularly special with the ZnO film described in 02100436.6 and ZL200410011164.0 P-type broad stopband oxide semiconductor film materials hole injection layer 3 is grown on n-ZnO luminescent layers 2 with growth MOCVD device (these p-type broad stopband oxide semiconductor film materials can be undoped with p-type material or doping p-type Material, different materials institute dopant material are different.), its thickness is 300~2000nm, and carrier concentration is 5 × 1017~2 × 1019/cm3
3) thermal evaporation station or electron beam and then in the subregion of the upper surface of hole injection layer 3 (10~30% of area) are used Evaporator evaporation metal prepares Top electrode 4, and the region for not preparing Top electrode 4 is output optical zone;
4) the conductive Si single-chips substrate 1 of n-type is finally thinned to 60~150 microns, then steamed in the lower surface of substrate 1 with heat Hair platform or electron beam evaporation platform evaporation metal prepare bottom electrode 5, and finally under nitrogen gas protection, alloy moves back upper/lower electrode together Fire, annealing temperature can be at 300~450 DEG C, and annealing time is 2~5 minutes, so as to which the wide taboo of p-type of the present invention be prepared Band oxide and ZnO combination vertical structure light-emitting devices.
Upper and lower electrode material can use one kind in the alloy materials such as Au, Al, Ni-Au, Ti-Au, Zn-Au or Pt-Au, its Thickness is 100~600 nanometers.
The invention has the advantages that:
P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices prepared by the present invention, due to using undoped with just It is the broad stopband oxide material of p-type electric-conducting, or we have prepared more ripe p-type broad stopband oxide material and have prepared hole Implanted layer 3, can solve ZnO material p-type doping difficult problem, while device uses vertical stratification, technique is simple, can be further Expand the application of device.
Brief description of the drawings
Fig. 1:P-type broad stopband oxide and ZnO combination vertical structure light-emitting device architecture schematic diagrames.
Part 1 is substrate in figure, and 2 be n-ZnO luminescent layers, and 3 be hole injection layer, and 4 be Top electrode, and 5 be bottom electrode.
Fig. 2:The broad stopband oxide and ZnO combination vertical structure light-emitting device currents of p-type NiO thin-film materials become with voltage Change curve.
Fig. 3:P-type broad stopband oxide and ZnO combination vertical structure light-emitting device electrical pumpings for p-type NiO thin-film materials Luminescent spectrum.
Fig. 4:P-type broad stopband oxide and ZnO combination vertical structure light-emitting device electrical pumpings for p-type CuO thin-film materials Luminescent spectrum.
Fig. 5:For p-type Ga2O3The p-type broad stopband oxide and ZnO combination vertical structure light-emitting device electrical pumpings of thin-film material Luminescent spectrum.
Embodiment
Describe the specific embodiment and implementing process of the present invention in detail below in conjunction with technical scheme and accompanying drawing.
Embodiment 1:
The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices of p-type NiO thin-film materials.This luminescent device Structure is shown in accompanying drawing 1, and its preparation process is, special using the ZnO film described in 02100436.6 and ZL200410011164.0 patents With growth MOCVD device and technique the conductive Si single-chips of n-type (can directly be commercially available, its carrier concentration is 2 × 1018/cm3) on substrate 1 growth undoped with n-ZnO luminescent layers 2, its thickness be 500nm, and carrier concentration is 2 × 1018/cm3; Then again using the special growth MOCVD device of the ZnO film described in 02100436.6 and ZL200410011164.0 patents in n- ZnO luminescent layers 2 above then grow undoped with p-type NiO thin-film materials hole injection layer 3, organic nickel source of growth is first Base dicyclopentadienyl nickel (NiMCP2), source bottle temperature are 50 DEG C, and growth temperature is 600 DEG C, working gas argon gas and oxygen mixed gas, Reaction chamber pressure is 80Pa, and growth time 1 hour, film thickness 500nm, carrier (hole) concentration is 5 × 1017/cm3.So Use mask platemaking technology afterwards, deposited by electron beam evaporation platform the upper part region of p-type NiO thin-film materials hole injection layer 3 (area 15%) alloy Ni-Au is deposited and prepares Top electrode 4, the region for not preparing Top electrode 4 is output optical zone;Finally Si substrates 1 are thinned Bottom electrode 5 is prepared with thermal evaporation station evaporation metal Al to 100 microns, then in the lower surface of substrate 1, is finally protected in nitrogen gas Under, upper/lower electrode together anneal by alloy, and annealing temperature is at 420 DEG C.The thickness of Top electrode 4 and bottom electrode 5 is 150nm, during annealing Between be 3 minutes.
Embodiment 2:
The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices of p-type CuO thin-film materials.This luminescent device Structure is shown in accompanying drawing 1, and its preparation process is, special using the ZnO film described in 02100436.6 and ZL200410011164.0 patents With growth MOCVD device and technique, in n-Si single-chips substrate 1, (its carrier concentration is 2 × 1018/cm3) on growth undoped with N-ZnO luminescent layers 2, its thickness is 500nm, and carrier concentration is 2 × 1018/cm3;Then 02100436.6 He is used again The special growth MOCVD device of ZnO film described in ZL200410011164.0 patents then grows on n-ZnO luminescent layers 2 Undoped with p-type CuO thin-film materials hole injection layer 3, the organic copper sources of growth are 2,2,6,6- tetramethyl -3,5- heptadione (TMHD) (Htmhd=2,2,6,6 ,-tetramethyl-3,5-heptandione), source bottle temperature is 90 DEG C, and growth temperature is 600 DEG C, working gas argon gas and oxygen mixed gas, reaction chamber pressure is 200Pa, growth time 1 hour, film thickness 400nm, carrier (hole) concentration are 6 × 1017/cm3.Then mask platemaking technology is used, deposited by electron beam evaporation platform is in p-type CuO The upper part region of thin-film material hole injection layer 3 (15% of area) evaporation Au prepares Top electrode 4, does not prepare Top electrode 4 Region be output optical zone;Si substrates 1 are finally thinned to 100 microns, then in the lower surface of substrate 1 thermal evaporation station evaporation metal Al Bottom electrode 5 is prepared, finally under nitrogen gas protection, upper/lower electrode together anneal by alloy, and annealing temperature is 420 DEG C.Top electrode 4 Thickness with bottom electrode 5 is 150nm, and annealing time is 3 minutes.
Embodiment 3:
P-type Ga2O3The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices of thin-film material.This photophore Part structure is shown in accompanying drawing 1, and its preparation process is, using the ZnO film described in 02100436.6 and ZL200410011164.0 patents (its carrier concentration is 2 × 10 in n-Si single-chips substrate 1 for special growth MOCVD device and technique18/cm3) on grow and do not mix Miscellaneous n-ZnO luminescent layers 2, its thickness are 500nm, and carrier concentration is 2 × 1018/cm3;Then ZL is used again 201310414275.5 the p-type Ga described in patent2O3Then the p-type of magnesium is mixed in growth to preparation technology on n-ZnO luminescent layers 2 Ga2O3Thin-film material hole injection layer 3, doped source are two luxuriant magnesium, and source bottle temperature is 25 DEG C, and growth temperature is 600 DEG C, work gas Body argon gas and oxygen mixed gas, reaction chamber pressure are 120Pa, growth time 1 hour, film thickness 500nm, carrier (hole) concentration is 7.5 × 1017/cm3.Then mask platemaking technology is used, deposited by electron beam evaporation platform is in p-type Ga2O3Thin-film material is empty The upper part region of cave implanted layer 3 (15% of area) evaporation Au prepares Top electrode 4, and the region for not preparing Top electrode 4 is Light area;Si substrates 1 are finally thinned to 100 microns, then bottom electrode is prepared with thermal evaporation station evaporation metal Al in the lower surface of substrate 1 5, finally under nitrogen gas protection, upper/lower electrode together anneal by alloy, and annealing temperature is 430 DEG C.Top electrode 4 and bottom electrode 5 Thickness be 150nm, annealing time is 3 minutes.
To tentatively prepare the p-type broad stopband oxides of p-type NiO thin-film materials and ZnO combination vertical structure light-emittings device, The p-type broad stopband oxide and ZnO combination vertical structure light-emitting devices and p-type Ga of p-type CuO thin-film materials2O3The p of thin-film material The electric current of molded breadth forbidden band oxide and ZnO combination vertical structure light-emitting devices is tested with voltage change characteristic, wherein p-type The p-type broad stopband oxide and ZnO combination vertical structure light-emitting device currents of NiO thin-film materials are with voltage change characteristic such as Fig. 2 Shown, this characteristic of other two kinds of devices is also more or less the same, and three kinds of device currents are almost identical with voltage change curve shape, P-n junction diode characteristic is all presented, does not draw one by one here.The electrical pumping characteristics of luminescence of three kinds of devices is also tested, Its electrical pumping luminescent spectrum respectively as shown in Fig. 3,4,5, although due to being preliminary experiment, the crystal mass of epitaxial thin film material Differ larger, experimental result is also undesirable, and the luminescent spectrum difference of three kinds of devices is larger, but all realizes the electricity of ZnO material Injection is luminous, and it is feasible to have sufficed to show that its technology path.If further the epitaxy technique of optimization Material growth improves Crystal mass, while optimised devices structure and preparation technology, the characteristics of luminescence of device can make moderate progress, and further realize ZnO materials The electronic injection laser transmitting of material is also possible.

Claims (3)

  1. A kind of 1. p-type Ga2O3With ZnO combination vertical structure light-emitting devices, successively by substrate (1), in substrate (1) Epitaxial growth N-ZnO luminescent layers (2), prepared on n-ZnO luminescent layers (2) hole injection layer (3), prepared on hole injection layer (3) Top electrode (4), the bottom electrode (5) for preparing below in substrate (1) forms, it is characterised in that:Substrate (1) is the conductive Si of n-type Single-chip, its carrier electrons concentration range are 5 × 1017~2 × 1019/cm3, hole injection layer (3) is the p-type Ga for mixing magnesium2O3 Semiconductor film material, thickness range are 200nm~2000nm, and carrier hole concentration range is 2 × 1017~5 × 1019/ cm3;And the luminescent device is prepared by following steps,
    1) on the conductive Si single crystalline substrates piece (1) of n-type growth undoped with n-ZnO luminescent layers (2), its thickness is 300~ 800nm, carrier concentration are 5 × 1017~2 × 1019/cm3
    2) the p-type Ga of magnesium is mixed in growth on n-ZnO luminescent layers (2)2O3Semiconductor film material hole injection layer (3), its thickness are 300~2000nm, carrier concentration are 5 × 1017~2 × 1019/cm3
    3) the subregion evaporation metal in hole injection layer (3) upper surface prepares Top electrode (4), does not prepare Top electrode (4) Region be output optical zone;
    4) the conductive Si substrates (1) of n-type are thinned to 60~150 microns, then evaporation metal prepares bottom electrode below in substrate (1) (5), finally under nitrogen gas protection, upper and lower electrode metal annealing, annealing temperature is 300~450 DEG C, annealing time is 2~ 5 minutes, so as to which p-type Ga be prepared2O3With ZnO combination vertical structure light-emitting devices.
  2. A kind of 2. p-type Ga as claimed in claim 12O3With ZnO combination vertical structure light-emitting devices, it is characterised in that:It is upper and lower Electrode material is Au, Al, Ni-Au, Ti-Au, Zn-Au or Pt-Au, and thickness is 100~600 nanometers.
  3. A kind of 3. p-type Ga as claimed in claim 12O3With ZnO combination vertical structure light-emitting devices, it is characterised in that:Using MOCVD techniques prepare n-ZnO luminescent layers (2) and hole injection layer (3);Top electrode is prepared using evaporator or electron beam evaporation platform And bottom electrode (5) (4).
CN201610286126.9A 2016-05-03 2016-05-03 P-type broad stopband oxide and ZnO combination vertical structure light-emitting devices and preparation method thereof Expired - Fee Related CN105789399B (en)

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CN111668354B (en) 2019-03-08 2021-08-17 华南师范大学 InGaN-based LED epitaxial wafer and preparation method thereof
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