CN110112267A - Zinc oxide quantum light source and preparation method thereof - Google Patents
Zinc oxide quantum light source and preparation method thereof Download PDFInfo
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- CN110112267A CN110112267A CN201810100060.9A CN201810100060A CN110112267A CN 110112267 A CN110112267 A CN 110112267A CN 201810100060 A CN201810100060 A CN 201810100060A CN 110112267 A CN110112267 A CN 110112267A
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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
- B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/62—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing gallium, indium or thallium
- C09K11/621—Chalcogenides
- C09K11/623—Chalcogenides with zinc or cadmium
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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
- H01L33/04—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 quantum effect structure or superlattice, e.g. tunnel junction
- H01L33/06—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 quantum effect structure or superlattice, e.g. tunnel junction within the light emitting region, e.g. quantum confinement structure or tunnel barrier
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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
- H01L33/285—Materials of the light emitting region containing only elements of group II and group VI of the periodic system characterised by the doping materials
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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
- H01L33/44—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 coatings, e.g. passivation layer or anti-reflective coating
Abstract
The present invention provides a kind of zinc oxide quantum light source, it include: substrate layer, the doped zno layer on the substrate layer and Ag, Au or Al metal nano ball being dispersed on the doped zno layer, wherein, doped chemical in the doped zno layer is that the diameter of one of group-III element or V group element or a variety of and described Ag, Au or Al metal nano ball is 20~50nm.Zinc oxide quantum light source of the invention is coupled using caused complex defect is adulterated with the surface phasmon of metal Nano structure, and the gain and stability of light source are greatly improved.
Description
Technical field
The invention belongs to photonic semiconductors and opto-electronic device preparation technical field, and in particular to a kind of zinc oxide quantum light
Source and preparation method thereof.
Background technique
With the fast development of quantum information technology, the especially considerable hair of quantum calculation in recent years and quantum communications
Exhibition, the solid state quantum light source of high quality are increasingly becoming crucial active device.Most researchs focus primarily upon semiconductor amount at present
Sub- point, semiconductor colour center (point defect), two-dimensional material and frequency lower switch technology, wherein wide bandgap semiconductor (including gold
Hard rock, silicon carbide (SiC), gallium nitride (GaN) and zinc oxide (ZnO)) colour center be considered as a kind of ideal light source, very
Suitable for Solid state quantum information processing.Compared to other several wide bandgap semiconductors, the research based on ZnO colour center control technique
It starts late, just had been reported that successively in recent years.The luminescence of color centers of ZnO covers entire visible region, compared to traditional quantum
Infrared light used in information technology is easier to detect.But as single-photon source, at present to the research of ZnO luminescence of color centers also in
The very preliminary stage；In addition, luminescence of color centers, which has, was up to for more than ten nanoseconds since ZnO has the exciton binding energy of up to 60meV
Coherence time [referring to Polarization spectroscopy of defect-based single photon
Sources in ZnO, ACS Nano 10,1210 (2016)；A single-molecule approach to ZnO
Defect studies:Single photons and single defects, J.Appl.Phys.116,043509
(2014)], there are also low manufacture cost, the advantages such as be readily synthesized and regulate and control, thus it is shown that more powerful application prospect.
Recent research result indicate that the photic of defect in ZnO can be enhanced using the method for introducing surface phasmon
Luminous intensity [referring to: Enhancement of visible-luminescence saturation intensity by
Surface plasmons in Ag/ZnO films, Phys.Rev.Appl.6,044009 (2016)；Selective
Purcell enhancement of defect emission in ZnO thin films, Opt.Lett.37,1538
(2012)；Photon energy conversion via localized surface plasmons in ZnO/Ag/ZnO
Nanostructures, Appl.Surf.Sci.258,5886 (2012)].But in the undoped ZnO film reported at present
Intrinsic point defects there are concentration uncontrollable, result is difficult the disadvantages of repeating, thus surface phasmon effect coupled thereto and
Efficiency is also difficult to control and repeat；In addition, general intrinsic point defects, luminescent lifetime are shorter, it is easy to by quiet around
The disturbance of electric field, to the phenomenon that light-emitting flash and spectral frequency jump occur, i.e., stability is poor, this for quantum light source,
It is a very unfavorable defect.
Summary of the invention
Therefore, it is an object of the invention to overcome the defect of the above-mentioned prior art, a kind of zinc oxide quantum light source is provided, is wrapped
Include: doped zno layer on substrate layer, the substrate layer and Ag, Au or Al metal being dispersed on the doped zno layer are received
Rice ball, wherein the doped chemical in the doped zno layer is one of group-III element or V group element or a variety of, Yi Jisuo
The diameter for stating Ag, Au or Al metal nano ball is 20~50nm.
Zinc oxide quantum light source according to the present invention, it is preferable that Ag, Au or Al metal nano ball is homogenously dispersed
On the doped zno layer.
Zinc oxide quantum light source according to the present invention, it is preferable that the diameter of Ag, Au or Al metal nano ball is
40nm。
Zinc oxide quantum light source according to the present invention, it is preferable that the doped zno layer is ZnO:Ga film.
Zinc oxide quantum light source according to the present invention, it is preferable that the Ga doping concentration of the ZnO:Ga film is 9 × 1017/
cm3
Zinc oxide quantum light source according to the present invention, it is preferable that effective defect density of the ZnO:Ga film is not higher than 1
×1015/cm3。
Zinc oxide quantum light source according to the present invention, it is preferable that the substrate is made of Si or sapphire.
The present invention also provides a kind of preparation methods of zinc oxide quantum light source, include the following steps:
Step 1: doped zno layer is prepared on substrate；
Step 2: Ag nanosphere suspension is transferred to the surface of the doped zno layer；And
Step 3: Ag nanosphere suspension described in spin coating.
The preparation method of zinc oxide quantum light source according to the present invention further includes the steps that cleaning the doped zno layer.
The present invention is coupled using caused complex defect is adulterated with the surface phasmon of metal Nano structure, and one
The concentration controllability of aspect impurity is relatively good, therefore the concentration of complex defect correspondingly might as well control；On the other hand, it utilizes
When different growing technologies are doped, the dependence of the concentration of the Effective Doping concentration of impurity or even complex defect to growing technology
It is relatively weak, growing technology and equipment are depended on unlike intrinsic point defects；In addition to this, the luminous longevity of the complex defect
It orders long, therefore with after surface phasmon coupling, light-emitting flash and spectral frequency can largely be avoided to jump
The problem of, greatly improve the gain and stability of light source.
Detailed description of the invention
Embodiments of the present invention is further illustrated referring to the drawings, in which:
Fig. 1 is the complex defect schematic diagram in gallium-doped zinc oxide (ZnO:Ga)；
Fig. 2 is to enhance the luminous zinc oxide quantum light of complex defect according to the surface phasmon of first embodiment of the invention
The structure and schematic illustration in source；
Fig. 3 is to be distributed in ZnO:Ga according to the Ag nanosphere of diameter 20nm, 30nm and 40nm of first embodiment of the invention
The scanning electron microscope image of layer surface；
Fig. 4 shows the photoluminescence spectrum and no Ag of the zinc oxide quantum light source comprising different-diameter Ag nanosphere of the invention
The photoluminescence spectrum of the zinc oxide quantum light source of nanosphere modification；
Fig. 5 shows the time-resolved spectrum of the various zinc oxide quantum light sources of Fig. 4；
The surface that 40 nanometer Ag nanospheres of contrast sample and the second embodiment that Fig. 6 modifies for no Ag nanosphere are modified
The confocal optics luminous intensity scan image of phasmon enhancing luminescent sample；
Fig. 7 modifies for no Ag nanosphere contrast sample luminescence generated by light (I) modified and 40 nanometer Ag balls of the embodiment
Phasmon enhance luminous spectrum (II).
Fig. 8 is the hair of the contrast sample of no Ag nanosphere modification and the 40 nanometer Ag nanospheres modification sample of second embodiment
Spectrum at any time with the relationship of wavelength.When without Ag nanosphere, it can be seen that luminous intensity, which changes over time, has occurred light and shade flashing,
And under the modification of 40 nanometer Ag nanospheres, luminous intensity does not change significantly at any time.
Specific embodiment
In short, the present invention improves the radiation recombination of luminescence of color centers in ZnO by being introduced into metal surface phasmon
Quantum efficiency.The result of study of inventor early period shows that (such as the vacancy Zn-displacement Ga uses V to the complex defect in ZnOZn-GaZn
Indicate) be can be by realizing accurately controlling to defect density and defect distribution to the regulation of growth conditions, in this base
On plinth, the controllable preparation of single-photon source photonic device may be implemented.In addition, before accurately control complex defect (colour center) concentration
Put, in order to improve the light emission luminance and optical stability of ZnO colour center, introduce metal surface phasmon be it is a kind of have very much it is latent
The technological means of power.It, can be by the coupling of metal surface phasmon by constructing suitable metal (Ag, Au or Al)/interface ZnO
Multiplex section is adjusted near luminescence of color centers peak；Due to the participation of a large amount of free electrons in metal surface, surface phasmon can be provided
Very big Photon state density.According to fermic golden rule, the transition probability of electronics and the size of Photon state density are directly proportional, because
The brightness of this defect luminescence can improve a lot；In addition, due to the strong coupling of ZnO colour center and the formation of metal surface phasmon
Conjunction substantially reduces its coupling probability between unstable electronic state present in ZnO, therefore the flashing of luminescence of color centers
Phenomenon is significantly improved, and the stability of luminescent device is further improved.
In order to make the purpose of the present invention, technical solution and advantage are more clearly understood, and are passed through below in conjunction with attached drawing specific real
Applying example, the present invention is described in more detail.It should be appreciated that the specific embodiments described herein are merely illustrative of the present invention,
It is not intended to limit the present invention.
First embodiment
The present embodiment provides a kind of zinc oxide quantum light sources of surface phasmon enhancing, referring to Fig. 1 and Fig. 2.Fig. 1 is to mix
Complex defect schematic diagram in gallium zinc oxide (ZnO:Ga), it can be seen that in ZnO:Ga, defect includes the vacancy Zn and displacement
Ga.Fig. 2 shows the structures and principle of the luminous zinc oxide quantum light source of the surface phasmon of embodiment enhancing complex defect
Schematic diagram.Zinc oxide quantum light source include: silicon (Si) substrate, Si substrate ZnO:Ga layer and be dispersed in ZnO:Ga layers
On Ag nanosphere, wherein silicon substrate with a thickness of 0.5mm, ZnO:Ga layers with a thickness of 400nm, Ga doping concentration is 9 ×
1017/cm3, the diameter of Ag nanosphere is 40nm.Referring to Fig. 3, (a) of Fig. 3, (b) and (c) be respectively diameter 20nm, 30nm and
The Ag nanosphere of 40nm is distributed in the scanning electron microscope image of ZnO:Ga layer surface, it can be seen that the dispersion of Ag nanosphere is arranged in
On ZnO:Ga layers of surface.
In the zinc oxide quantum light source of the embodiment, ZnO:Ga layers of VZn-GaZnComplex defect shines and Ag nanosphere
Surface phasmon coupling, so that the luminescence enhancement of zinc oxide quantum light source.In this embodiment, incident light and emergent light
In the ipsilateral of ZnO:Ga film.In addition, according to other embodiments of the invention, it is preferable that the diameter of Ag nanosphere be 20nm~
Any size between 50nm.In order to embody effect of the invention, the present inventor also by the Ag nanosphere comprising different-diameter and
The photoluminescence spectrum of zinc oxide quantum light source not comprising Ag nanosphere is compared, and referring to fig. 4, Fig. 4 shows packet of the invention
The zinc oxide quantum light that the photoluminescence spectrum of the zinc oxide quantum light source of the nanosphere of Ag containing different-diameter is modified with no Ag nanosphere
The photoluminescence spectrum in source.As can be seen that zinc oxide quantum light source of the invention is compared to the zinc oxide quantum light that no nanosphere is modified
The output light intensity in source improves 2-5 times, and the Ag nanosphere of diameter 40nm is better than the Ag nanosphere of diameter 30nm, and is better than
The Ag nanosphere of diameter 20nm.
Fig. 5 shows the time-resolved spectrum of the various zinc oxide quantum light sources of Fig. 4.It is obtained from interpretation of result, due to Ag nanometers
Colour center-surface phasmon coupling caused by the modification of ball, with the increase of Ag nanometers of bulb diameters, photon radiation longevity
Life is reduced to the 0.1ns of 40 nanometer Ag nanospheres from the 3.77ns of no Ag nanosphere, and the quantum efficiency of defect radiation recombination obtains
It is greatly improved.
The preparation of the zinc oxide quantum light source of the embodiment includes the following steps:
Step 1: the ZnO film adulterated on a si substrate by MBE epitaxial growth with a thickness of the Ga of 400nm, wherein Ga
Doping concentration be 9 × 1017/cm3；
Step 2: by the surface treatment of n-butyl acetate, acetone and isopropanol, the ZnO with clean surface is obtained:
Ga film；
Step 3: 10 microlitres of 0.05g/mol, the Ag nanosphere suspension that diameter is 20~40nm are shifted using pipettor
To ZnO:Ga film surface；
Step 4: with 200-1000 revolutions per seconds of speed spin coating Ag nanosphere suspension, so that Ag nanosphere dispersion row
Cloth is on ZnO:Ga film surface.
According to other embodiments of the invention, Ag nanosphere is replaced using Au or Al nanosphere, or thin using ZnO:Ga
Film replaces with ZnO:Al film, and other conditions are constant, is also able to achieve the zinc oxide quantum of surface phasmon enhancing of the invention
Light source.
Second embodiment
The embodiment provides a kind of ZnO defect report based on the enhancing of Ag nanosphere/ZnO:Ga structure surface phasmon
Photon source, structural schematic diagram is similar with first embodiment, and the main distinction is that the effective defect for needing to control ZnO:Ga is dense
Degree, to guarantee that each Ag nanosphere covering is not more than single VZn-GaZnComplex defect, to realize single-photon source.The embodiment
ZnO defect single-photon source include: Sapphire Substrate, the ZnO:Ga film on Sapphire Substrate and be dispersed in ZnO:Ga film
On Ag nanosphere, wherein ZnO:Ga film with a thickness of 400nm, effective defect density be not higher than 1 × 1015/cm3, to protect
It demonstrate,proves each Ag nanosphere covering and is not more than single VZn-GaZnComplex defect, the diameter of Ag nanosphere are 40nm.ZnO:Ga film
Effective defect density and Ga doping concentration, preparation condition (including growth temperature, foreign atom line size and annealing temperature
Deng) etc. many factors it is related, need to coordinate each correlative factor to carry out organic regulation to effective defect density.
Referring to Fig. 6, Fig. 6 repairs for 40 nanometer Ag balls of contrast sample (I) and the second embodiment that no Ag nanosphere is modified
The confocal optics luminous intensity scan image of surface phasmon enhancing luminescent sample (II) of decorations.Identical test condition
Under, the luminous intensity of contrast sample (I) is 2x103(note: characterizing luminous intensity with nondimensional relative intensity), 40 nanometer Ags
The luminous intensity of surface phasmon enhancing luminescent sample (II) of ball modification is 6.98 × 104.As can be seen that surface etc. from
Under the mechanism of excimer enhancing, luminous around Ag has apparent enhancing, forms significantly luminous " hot spot ".
Fig. 7 is the luminous spectrum for the individual defect chosen in sample shown in fig. 6, with modifying in the Fig. 7 without Ag nanosphere
Sample I compare, the luminous peak intensity of the surface phasmon enhancing luminescent sample II of 40 nanometer Ag balls in Fig. 7 modification has 5-
6 times of enhancing.
Fig. 8 is peak position-strength versus time profile diagram that individual defect shines.It obviously observes, in no Ag nanosphere
In the case of (left figure), due to the Random Coupling of defect and the unstable electronic environment of surrounding, luminous intensity is in wavelength at any time
Reveal irregular flashing.And in the case where there is Ag (right figure), due to the coupling of defect and surface phasmon, shine
Scintillation is substantially reduced.
The preparation method of the ZnO defect single-photon source of the embodiment includes the following steps:
Step 1: pass through metallochemistry vapor deposition (MOVPE) ZnO that growth thickness is 400nm on a sapphire substrate:
Effective defect density of Ga film, ZnO:Ga film is not higher than 1 × 1015/cm3, to guarantee in the Ag nanosphere prepared on it
Each covering be not more than single VZn-GaZnComplex defect；
Step 2: by the surface treatment of n-butyl acetate, acetone and isopropanol, the ZnO with clean surface is obtained:
Ga film；
Step 3: using pipettor, by 0.05g/mol, Ag nanosphere suspension that diameter is 40nm, to be transferred to ZnO:Ga thin
Film surface；And
Step 4: using the method for spin coating, under 200-1000 revolutions per seconds of revolving speed, the dispersion of Ag nanosphere is arranged in
ZnO:Ga film surface, to guarantee that discrete Ag nanosphere covers single complex defect or other types point defect.
According to other embodiments of the invention, Ag nanosphere is replaced using Au nanosphere or Al nanosphere, or used
ZnO:Ga film replaces with ZnO:Al film, and other conditions are constant, is also able to achieve the ZnO of surface phasmon enhancing of the invention
Defect single-photon source, in addition, the diameter of Ag nanosphere is preferably 20nm~50nm.
According to other embodiments of the invention, the doped chemical of ZnO film can using group-III element Al, Ga, In or
One or more of V group element N, P, As, Ab, in addition, ZnO thin film doped thickness is not limited to 400nm.
In zinc oxide quantum light source of the invention, incident light and emergent light are in ZnO thin film doped ipsilateral (i.e. positive hair
Light), therefore the thickness of substrate is not also limited.
According to other embodiments of the invention, the pattern of metal material Al, Au and Ag is not particularly limited, depending on device architecture
Depending on.Due to the coupling of metal and doped zno layer, surface phasmon introduces the bigger optics density of states, according to Fermi's Huang
The brightness of defect quantum light source is greatly improved in golden rule.Additionally, due to the coupling of disfigurement model and surface phasmon
Effect considerably reduces electronic environment bring adverse effect, so that the stability of quantum light source be greatly improved.
Although the present invention has been described by means of preferred embodiments, the present invention is not limited to described here
Embodiment, without departing from the present invention further include made various changes and variation.
Claims (9)
1. a kind of zinc oxide quantum light source, comprising: doped zno layer on substrate layer, the substrate layer and be dispersed in described mix
Ag, Au or Al metal nano ball on miscellaneous ZnO layer, wherein the doped chemical in the doped zno layer is group-III element or V
One of race's element or the diameter of a variety of and described Ag, Au or Al metal nano ball are 20~50nm.
2. zinc oxide quantum light source according to claim 1, wherein Ag, Au or Al metal nano ball equably dissipates
It is distributed on the doped zno layer.
3. zinc oxide quantum light source according to claim 1, wherein the diameter of Ag, Au or Al metal nano ball is
40nm。
4. zinc oxide quantum light source according to any one of claim 1-3, wherein the doped zno layer is ZnO:Ga
Film.
5. zinc oxide quantum light source according to claim 4, wherein the Ga doping concentration of the ZnO:Ga film be 9 ×
1017/ cm3。
6. zinc oxide quantum light source according to claim 4, wherein effective defect density of the ZnO:Ga film is not high
In 1 × 1015/cm3。
7. zinc oxide quantum light source according to claim 1, wherein the substrate layer is made of Si or sapphire.
8. the preparation method of zinc oxide quantum light source described in any one of -7 according to claim 1, includes the following steps:
Step 1: doped zno layer is prepared on substrate layer；
Step 2: Ag nanosphere suspension is transferred to the surface of the doped zno layer；And
Step 3: Ag nanosphere suspension described in spin coating.
9. preparation method according to claim 8 further includes the steps that cleaning the doped zno layer.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111262133A (en) * | 2020-01-16 | 2020-06-09 | 北京理工大学 | Method for improving single-layer two-dimensional semiconductor light-emitting brightness |
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