CN105789399A - P-type wide band gap oxide and ZnO combined vertical structure luminescent device and manufacturing method thereof - Google Patents
P-type wide band gap oxide and ZnO combined vertical structure luminescent device and manufacturing method thereof Download PDFInfo
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- CN105789399A CN105789399A CN201610286126.9A CN201610286126A CN105789399A CN 105789399 A CN105789399 A CN 105789399A CN 201610286126 A CN201610286126 A CN 201610286126A CN 105789399 A CN105789399 A CN 105789399A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
- H01L33/14—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/005—Processes
- H01L33/0083—Processes for devices with an active region comprising only II-VI compounds
- H01L33/0087—Processes for devices with an active region comprising only II-VI compounds with a substrate not being a II-VI compound
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
- H01L33/26—Materials of the light emitting region
- H01L33/28—Materials of the light emitting region containing only elements of group II and group VI of the periodic system
Abstract
The invention belongs to the semiconductor luminescent device and manufacturing technology field and relates to several kinds of p-type wide band gap oxide and ZnO combined vertical structure luminescent devices and a manufacturing method thereof. Each device is successively formed by a substrate, an n-ZnO luminescent layer epitaxially grown on the substrate, a hole injection layer prepared on the n-ZnO luminescent layer, an upper electrode prepared on the hole injection layer and a lower electrode prepared below the substrate. The device is characterized in that the substrate is an n-type conductive Si single crystal wafer; the hole injection layer is a p-type wide band gap oxide semiconductor films material; a thickness range is 200nm to 2000nm; and a concentration range of a carrier (a hole) is 2*10<17> to 5*10<19>/cm<3>. In the invention, a problem that ZnO material p type doping is difficult can be solved; simultaneously the device adopts a vertical structure and a technology is simple so that an application range of the device can be further expanded.
Description
Technical field
The invention belongs to light emitting semiconductor device and preparing technical field thereof, be specifically related to a kind of based on zno-based
The p-type broad stopband oxide of material and ZnO combination vertical structure light-emitting device and preparation method thereof.
Background technology
GaN material has wider application prospect in solid-state illumination field.The band gap of ZnO and GaN
It is sufficiently close to lattice paprmeter, has close photoelectric characteristic.But, compared with GaN, ZnO has higher
Fusing point and exciton bind energy, exciton gain is higher, epitaxial growth temperature is low, low cost, easily etching and make right
The rear road processing of epitaxial wafer is easier to, and makes preparing of device more convenient etc..Therefore, zno-based luminous tube,
The luminescent devices such as laser instrument are succeeded in developing and are likely replaced or part replacement GaN base photoelectric device, have bigger
Application prospect, particularly ZnO is purple, ultraviolet light photo device more people are paid attention to.
But, owing to unadulterated ZnO material often presents N-shaped conduction (being labeled as n-ZnO), it carries
Stream (electronics) concentration is generally 5 × 1017～2 × 1019/cm3, therefore p-type ZnO material is difficult to preparation.
At present it has been reported that some p-type ZnO material technologies of preparing the most immature, thus prepare ZnO material
P-n junction luminescent device is also had any problem.In order to overcome this difficulty of ZnO-based light-emitting device, the present invention proposes
Other p-type broad stopband oxides several and N-shaped ZnO combination vertical structure light-emitting device and preparation method thereof.
Because being exactly p-type material when having some broad stopband oxide semiconductor material undoped p, just as ZnO not
Being exactly that n-type material is the same during doping, these unadulterated broad stopband its carriers of oxide semiconductor material are (empty
Cave) concentration is up to 2 × 1017～2 × 1018/cm3If carrying out p-type doping (different material institute further
Doping is different), its carrier (hole) concentration can further improve, and can reach 5 × 1017～5 × 1019/cm3,
Such as NiO, CuO material.Visible, so some broad stopband oxide materials are easier to be prepared as high hole
The p-type semiconductor material of conduction, easily combines prepare p-n junction type luminescent device with N-shaped ZnO.
Summary of the invention
The purpose of the present invention is exactly for solving ZnO material p-type doping difficult problem, utilizing other p-type width to prohibit
Band oxide semiconductor material and N-shaped ZnO combination prepare p-n junction type luminescent device, simultaneously in order to simplify
Device preparation technology, reduces cost, and substrate uses the Si monocrystal material of N-shaped conduction, and device is prepared as vertically
Structure.
P-type broad stopband oxide designed by the present invention and ZnO combination vertical structure light-emitting device are (see accompanying drawing
1 and accompanying drawing explanation), successively by substrate 1, the most epitaxially grown n-ZnO luminescent layer 2,
On n-ZnO luminescent layer 2 preparation hole injection layer 3, on hole injection layer 3 preparation upper electrode 4,
Bottom electrode 5 prepared by substrate 1 lower surface is constituted, it is characterised in that: the Si monocrystalline that substrate 1 conducts electricity for N-shaped
(its carrier (electronics) concentration range is 5 × 10 to sheet17～2 × 1019/cm3), hole injection layer 3 is p
Molded breadth forbidden band oxide semiconductor film materials, thickness range is 200nm～2000nm, carrier (hole)
Concentration range is 2 × 1017～5 × 1019/cm3。
Further in order to utilize our MOCVD technique, the present invention the most specifically proposes hole injection layer 3
For p-type broad stopband oxide and the ZnO combination vertical structure light-emitting device of p-type NiO thin-film material, successively
By substrate 1, the most epitaxially grown n-ZnO luminescent layer 2, prepare on n-ZnO luminescent layer 2
Hole injection layer 3, on hole injection layer 3 preparation upper electrode 4, under prepared by substrate 1 lower surface
Electrode 5 is constituted, it is characterised in that: the Si single-chip that substrate 1 conducts electricity for N-shaped, hole injection layer 3 is p
Type NiO thin-film material.
The present invention is the most concrete proposes the p-type broad stopband oxide that hole injection layer 3 is p-type CuO thin-film material
With ZnO combination vertical structure light-emitting device, successively by substrate 1, the most epitaxially grown n-ZnO
Luminescent layer 2, the hole injection layer 3 of preparation, preparation on hole injection layer 3 on n-ZnO luminescent layer 2
Upper electrode 4, the bottom electrode 5 prepared at substrate 1 lower surface are constituted, it is characterised in that: substrate 1 is led for N-shaped
The Si single-chip of electricity, hole injection layer 3 is p-type CuO thin-film material.
Further for p-type Ca utilizing us to prepare2O3Technique (the patent No.: ZL
201310414275.5), proposing again hole injection layer 3 is p-type Ca2O3The p-type broad stopband of thin-film material
Oxide and ZnO combination vertical structure light-emitting device, successively by substrate 1, the most epitaxially grown
N-ZnO luminescent layer 2, on n-ZnO luminescent layer 2 preparation hole injection layer 3, at hole injection layer 3
The upper electrode 4 of upper preparation, the bottom electrode 5 prepared at substrate 1 lower surface are constituted, it is characterised in that: substrate 1
For the Si single-chip of N-shaped conduction, hole injection layer 3 is p-type Ca2O3Thin-film material.
P-type broad stopband oxide of the present invention and the preparation method of ZnO combination vertical structure light-emitting device,
It is characterized in that: n-ZnO luminescent layer 2 and p-type broad stopband oxide semiconductor film materials hole injection layer 3
MOCVD (metal organic chemical vapor deposition) method is all used to be prepared.
Specifically comprise the following steps that
1) MOCVD method is used, particularly with Chinese patent 02100436.6 He
ZnO film special growth MOCVD device described in ZL200410011164.0 and work thereof
Skill grows unadulterated n-ZnO luminescent layer 2 on the Si single crystalline substrate sheet 1 that N-shaped conducts electricity,
Its thickness is 300～800nm, and its carrier (electronics) concentration is 5 × 1017～2 × 1019/cm3；
2) MOCVD method is used again, particularly with 02100436.6 and ZL200410011164.0
Described ZnO film special growth MOCVD device grows p on n-ZnO luminescent layer 2
(these p-type broad stopbands aoxidize molded breadth forbidden band oxide semiconductor film materials hole injection layer 3
Thing semiconductor film material can be unadulterated p-type material, it is also possible to be the p-type of doping
Material, different material institute dopant material is different.), its thickness is 300～2000nm, carries
Flowing sub-concentration is 5 × 1017～2 × 1019/cm3；
3) then thermal evaporation is used in subregion (the 10 of area～30%) at hole injection layer 3 upper surface
Platform or the upper electrode 4 of electron beam evaporation platform evaporation metal preparation, do not have the region of the upper electrode 4 of preparation
For output optical zone；
4) finally the Si single-chip substrate 1 that N-shaped conducts electricity is thinned to 60～150 microns, then at substrate
1 lower surface thermal evaporation station or electron beam evaporation platform evaporation metal prepare bottom electrode 5, finally exist
Nitrogen gas protection under, upper/lower electrode alloy together anneal, annealing temperature can at 300～450 DEG C,
Annealing time is 2～5 minutes, thus prepares p-type broad stopband of the present invention oxide
With ZnO combination vertical structure light-emitting device.
Upper and lower electrode material can close with Au, Al, Ni-Au, Ti-Au, Zn-Au or Pt-Au etc.
One in gold copper-base alloy, its thickness is 100～600 nanometers.
The invention have the advantages that:
P-type broad stopband oxide prepared by the present invention and ZnO combination vertical structure light-emitting device, owing to using
Undoped p is exactly the broad stopband oxide material of p-type electric-conducting, or we have prepared more ripe p-type width and have prohibited
Band oxide material prepares hole injection layer 3, can solve ZnO material p-type doping difficult problem, simultaneously
Device uses vertical stratification, and technique is simple, can expand the range of application of device further.
Accompanying drawing explanation
Fig. 1: p-type broad stopband oxide and ZnO combination vertical structure light-emitting device architecture schematic diagram.
In figure, parts 1 are substrate, and 2 is n-ZnO luminescent layer, and 3 is hole injection layer, and 4 is upper electrode, 5
For bottom electrode.
The broad stopband oxide of Fig. 2: p-type NiO thin-film material and ZnO combination vertical structure light-emitting device electricity
Stream is with voltage change curve.
Fig. 3: for p-type broad stopband oxide and the ZnO combination vertical structure light-emitting of p-type NiO thin-film material
Device electrical pumping luminescent spectrum.
Fig. 4: for p-type broad stopband oxide and the ZnO combination vertical structure light-emitting of p-type CuO thin-film material
Device electrical pumping luminescent spectrum.
Fig. 5: for p-type Ca2O3P-type broad stopband oxide and the ZnO combination vertical structure of thin-film material are sent out
Optical device electrical pumping luminescent spectrum.
Detailed description of the invention
Specific embodiment and the implementing process of the present invention is described in detail below in conjunction with technical scheme and accompanying drawing.
Embodiment 1:
The p-type broad stopband oxide of p-type NiO thin-film material and ZnO combination vertical structure light-emitting device.This
Planting emitting device structure and see accompanying drawing 1, its preparation process is, uses 02100436.6 He
ZnO film special growth MOCVD device described in ZL200410011164.0 patent and technique are at N-shaped
(can directly be commercially available, its carrier concentration is 2 × 10 to the Si single-chip of conduction18/cm3) substrate 1
Upper growth unadulterated n-ZnO luminescent layer 2, its thickness is 500nm, and carrier concentration is 2 × 1018/cm3；
Use the special growth of ZnO film described in 02100436.6 and ZL200410011164.0 patent the most again
MOCVD device then grows unadulterated p-type NiO thin-film material hole on n-ZnO luminescent layer 2
Implanted layer 3, organic nickel source of growth is methyl dicyclopentadienyl nickel (NiMCP2), and source bottle temperature is 50 ° of С, raw
Long temperature is 600 ° of С, working gas argon and oxygen mixed gas, and reative cell pressure is 80Pa, growth
1 hour time, film thickness 500nm, carrier (hole) concentration is 5 × 1017/cm3.Then use
Mask plate technology, deposited by electron beam evaporation platform is in p-type NiO thin-film material hole injection layer 3 upper part region
Electrode 4 in the alloy Ni-Au preparation of (the 15% of area) evaporation, does not has the region of the upper electrode 4 of preparation for going out
Light district；Finally Si substrate 1 is thinned to 100 microns, then at substrate 1 lower surface thermal evaporation station gold evaporation
Belonging to Al and prepare bottom electrode 5, finally under nitrogen gas is protected, upper/lower electrode alloy together is annealed, annealing temperature
Degree is at 420 DEG C.The thickness of upper electrode 4 and bottom electrode 5 is 150nm, and annealing time is 3 minutes.
Embodiment 2:
The p-type broad stopband oxide of p-type CuO thin-film material and ZnO combination vertical structure light-emitting device.This
Planting emitting device structure and see accompanying drawing 1, its preparation process is, uses 02100436.6 He
ZnO film special growth MOCVD device described in ZL200410011164.0 patent and technique are at n-Si
(its carrier concentration is 2 × 10 to single-chip substrate 118/cm3) the unadulterated n-ZnO luminescent layer 2 of upper growth,
Its thickness is 500nm, and carrier concentration is 2 × 1018/cm3；Use 02100436.6 He the most again
ZnO film special growth MOCVD device described in ZL200410011164.0 patent is luminous at n-ZnO
Layer 2 then grows unadulterated p-type CuO thin-film material hole injection layer 3, the organic copper of growth above
Source be DPM dpm,dipivalomethane (TMHD) (Htmhd=2,2,6,6 ,-tetramethyl-3,
5-heptandione), source bottle temperature is 90 ° of С, and growth temperature is 600 ° of С, working gas argon and oxygen
Oxygen mixture, reative cell pressure is 200Pa, growth time 1 hour, film thickness 400nm, current-carrying
Son (hole) concentration is 6 × 1017/cm3.Then using mask plate technology, deposited by electron beam evaporation platform is in p-type
Electrode 4 in the evaporation Au preparation of CuO thin-film material hole injection layer 3 upper part region (the 15% of area),
The region not having the upper electrode 4 of preparation is output optical zone；Finally Si substrate 1 is thinned to 100 microns, then at lining
The end 1 lower surface thermal evaporation station evaporation metal Al prepares bottom electrode 5, finally under nitrogen gas is protected, on
Bottom electrode alloy together is annealed, and annealing temperature is 420 DEG C.The thickness of upper electrode 4 and bottom electrode 5 is 150nm,
Annealing time is 3 minutes.
Embodiment 3:
P-type Ca2O3The p-type broad stopband oxide of thin-film material and ZnO combination vertical structure light-emitting device.
This emitting device structure is shown in accompanying drawing 1, and its preparation process is, uses 02100436.6 He
ZnO film special growth MOCVD device described in ZL200410011164.0 patent and technique are at n-Si
(its carrier concentration is 2 × 10 to single-chip substrate 118/cm3) the unadulterated n-ZnO luminescent layer 2 of upper growth,
Its thickness is 500nm, and carrier concentration is 2 × 1018/cm3；Use ZL 201310414275.5 the most again
P-type Ca described in patent2O3Preparation technology then grows the p-type mixing magnesium on n-ZnO luminescent layer 2
Ca2O3Thin-film material hole injection layer 3, doped source is two cyclopentadienyl magnesium, and source bottle temperature is 25 ° of С, growth temperature
Being 600 ° of С, working gas argon and oxygen mixed gas, reative cell pressure is 120Pa, growth time 1
Hour, film thickness 500nm, carrier (hole) concentration is 7.5 × 1017/cm3.Then mask is used
Platemaking technology, deposited by electron beam evaporation platform is in p-type Ca2O3(face, thin-film material hole injection layer 3 upper part region
Long-pending 15%) it is deposited with electrode 4 in Au preparation, the region not having the upper electrode 4 of preparation is output optical zone；Finally will
Si substrate 1 is thinned to 100 microns, then prepares lower electricity at substrate 1 lower surface thermal evaporation station evaporation metal Al
Pole 5, finally under nitrogen gas is protected, upper/lower electrode alloy together is annealed, and annealing temperature is 430 DEG C.On
The thickness of electrode 4 and bottom electrode 5 is 150nm, and annealing time is 3 minutes.
P-type broad stopband oxide and ZnO combination vertical structure to the preliminary p-type NiO thin-film material prepared
Luminescent device, the p-type broad stopband oxide of p-type CuO thin-film material and ZnO combination vertical structure light-emitting device
Part and p-type Ca2O3The p-type broad stopband oxide of thin-film material and ZnO combination vertical structure light-emitting device
Electric current is tested with change in voltage characteristic, wherein the p-type broad stopband oxide of p-type NiO thin-film material
With ZnO combination vertical structure light-emitting device current with change in voltage characteristic as in figure 2 it is shown, other two kinds of devices
This characteristic be also more or less the same, three kinds of device current are almost identical with voltage change curve shape, all present
P-n junction diode characteristic, draws the most one by one.It is also carried out surveying to the electrical pumping characteristics of luminescence of three kinds of devices
Examination, its electrical pumping luminescent spectrum is respectively as shown in Fig. 3,4,5, although owing to being preliminary experiment, extension
The crystal mass difference of thin-film material is relatively big, and experimental result is the most undesirable, and the luminescent spectrum difference of three kinds of devices is relatively
Greatly, but all achieve the electrical pumping luminescence of ZnO material, sufficed to show that its technology path is feasible.
If the epitaxy technique optimizing Material growth further improves crystal mass, simultaneously optimised devices structure and preparation work
Skill, the characteristics of luminescence of device can make moderate progress, and the electronic injection laser transmitting realizing ZnO material further is also
Possible.
Claims (7)
1. p-type broad stopband oxide and a ZnO combination vertical structure light-emitting device, successively by substrate (1),
At the n-ZnO luminescent layer (2) of substrate (1) Epitaxial growth, on n-ZnO luminescent layer (2)
The hole injection layer (3) of preparation, at the upper electrode (4) of the upper preparation of hole injection layer (3), at lining
The bottom electrode (5) that the end (1) prepares below is constituted, it is characterised in that: substrate (1) is N-shaped conduction
Si single-chip, its carrier (electronics) concentration range is 5 × 1017～2 × 1019/cm3, hole
Implanted layer (3) is p-type broad stopband oxide semiconductor film materials, and thickness range is
200nm～2000nm, carrier (hole) concentration range is 2 × 1017～5 × 1019/cm3。
The p-type broad stopband oxide of a kind of p-type NiO thin-film material the most as claimed in claim 1 and ZnO
Combination vertical structure light-emitting device, it is characterised in that: hole injection layer (3) is p-type NiO thin film
Material.
The p-type broad stopband oxide of a kind of p-type CuO thin-film material the most as claimed in claim 1 and ZnO
Combination vertical structure light-emitting device, it is characterised in that: hole injection layer (3) is p-type CuO thin film
Material.
4. a kind of p-type Ca as claimed in claim 12O3The p-type broad stopband oxide of thin-film material and ZnO
Combination vertical structure light-emitting device, it is characterised in that: hole injection layer (3) is p-type Ca2O3Thin
Membrane material.
5. a kind of p-type broad stopband oxide described in claim 1 and ZnO combination vertical structure light-emitting device system
Preparation Method, its step is as follows:
1) Si single crystalline substrate sheet (1) the unadulterated n-ZnO luminescent layer (2) of upper growth of N-shaped conduction,
Its thickness is 300～800nm, and carrier concentration is 5X1017～2 × 1019/cm3；
2) in n-ZnO luminescent layer (2) upper growth oxide semiconductor film materials hole, p-type broad stopband
Implanted layer (3), its thickness is 300～2000nm, and carrier concentration is
5X1017～2 × 1019/cm3；
3) at the upper electrode (4) of subregion evaporation metal preparation of hole injection layer (3) upper surface, do not have
The region having the upper electrode (4) of preparation is output optical zone；
4) the Si substrate (1) that N-shaped conducts electricity is thinned to 60～150 microns, then under substrate (1)
Face evaporation metal prepares bottom electrode (5), finally under nitrogen gas is protected, and upper and lower electrode
Alloy is annealed, and annealing temperature is 300～450 DEG C, and annealing time is 2～5 minutes, from
And prepare p-type broad stopband oxide and ZnO combination vertical structure light-emitting device.
6. a kind of p-type broad stopband oxide as claimed in claim 5 and ZnO combination vertical structure light-emitting device
Preparation method, it is characterised in that: upper and lower electrode material is Au, Al, Ni-Au, Ti-Au, Zn-Au
Or Pt-Au, thickness is 100～600 nanometers.
7. a kind of p-type broad stopband oxide as claimed in claim 5 and ZnO combination vertical structure light-emitting device
Preparation method, it is characterised in that: use MOCVD technique to prepare n-ZnO luminescent layer (2) and sky
Cave implanted layer (3)；Use evaporator or the upper electrode (4) of electron beam evaporation platform preparation and bottom electrode (5).
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109509843A (en) * | 2017-09-15 | 2019-03-22 | 财团法人工业技术研究院 | Light emitting element and transparent electrode thereof |
| CN111668354A (en) * | 2019-03-08 | 2020-09-15 | 华南师范大学 | InGaN-based LED epitaxial wafer and preparation method thereof |
| CN112038455A (en) * | 2020-08-27 | 2020-12-04 | 厦门士兰明镓化合物半导体有限公司 | Ultraviolet light emitting diode and manufacturing method thereof |
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| CN103268911A (en) * | 2013-04-22 | 2013-08-28 | 浙江大学 | p-NiO/n-ZnO heterojunction light-emitting device and preparation method thereof |
| CN103280498A (en) * | 2013-04-22 | 2013-09-04 | 常州大学 | Preparation method of pointed-cone-shaped zinc oxide/nickel oxide heterojunction diodes |
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| CN103268911A (en) * | 2013-04-22 | 2013-08-28 | 浙江大学 | p-NiO/n-ZnO heterojunction light-emitting device and preparation method thereof |
| CN103280498A (en) * | 2013-04-22 | 2013-09-04 | 常州大学 | Preparation method of pointed-cone-shaped zinc oxide/nickel oxide heterojunction diodes |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109509843A (en) * | 2017-09-15 | 2019-03-22 | 财团法人工业技术研究院 | Light emitting element and transparent electrode thereof |
| CN111668354A (en) * | 2019-03-08 | 2020-09-15 | 华南师范大学 | InGaN-based LED epitaxial wafer and preparation method thereof |
| CN111668354B (en) * | 2019-03-08 | 2021-08-17 | 华南师范大学 | InGaN-based LED epitaxial wafer and preparation method thereof |
| CN112038455A (en) * | 2020-08-27 | 2020-12-04 | 厦门士兰明镓化合物半导体有限公司 | Ultraviolet light emitting diode and manufacturing method thereof |
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