CN110212075A - A kind of laminated construction and preparation method thereof enhancing light-emitting film fluorescence radiation intensity - Google Patents

A kind of laminated construction and preparation method thereof enhancing light-emitting film fluorescence radiation intensity Download PDF

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CN110212075A
CN110212075A CN201910393599.2A CN201910393599A CN110212075A CN 110212075 A CN110212075 A CN 110212075A CN 201910393599 A CN201910393599 A CN 201910393599A CN 110212075 A CN110212075 A CN 110212075A
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emitting film
light
metal nano
laminated construction
particle layer
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CN110212075B (en
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闫胤洲
张玉洁
蒋毅坚
杨立学
邢承
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Beijing University of Technology
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Beijing University of Technology
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    • C23C14/06Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
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    • C23C14/00Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
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    • C23C14/00Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
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    • C23C14/00Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
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    • H01L33/50Wavelength conversion elements
    • H01L33/501Wavelength conversion elements characterised by the materials, e.g. binder
    • H01L33/502Wavelength conversion materials

Abstract

The invention discloses a kind of laminated construction and preparation method thereof for enhancing light-emitting film fluorescence radiation intensity, the laminated construction includes single layer dielectric micro-sphere array, light-emitting film and the substrate for stacking gradually connection, further include simultaneously, the first metal nano-particle layer being embedded between the light-emitting film and substrate, and the second metal nano-particle layer being embedded between the light-emitting film and single layer dielectric micro-sphere array.The laminated construction of enhancing light-emitting film fluorescence radiation intensity provided by the present invention combines the collective effect of dielectric microballoon light field regulation and metal surface phasmon coupling effect, the luminous intensity of light-emitting film may make to significantly increase, significantly larger than exclusive use metal nano-particle layer or the reinforcing effect of single layer dielectric micro-sphere array;Its preparation cost is cheap, method is simple, technique is time-consuming short and is not limited by any substrate, the luminescence enhancement suitable for high-quality semiconductor light-emitting film.

Description

A kind of laminated construction and preparation method thereof enhancing light-emitting film fluorescence radiation intensity
Technical field
The invention belongs to luminescent material technical fields, are related to a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity And preparation method thereof.
Background technique
Forbidden bandwidth is big, electronics drift saturated velocity is high and the spies such as dielectric constant is small because having for third generation semiconductor material Point, blue, green, purple light light emitting diode and in terms of have a wide range of applications;Meanwhile semiconductor lighting 21 century most promising one of high-tech sector is also become, but since the luminous intensity of some materials is lower, The obstacle for becoming its practical application, the luminous efficiency for improving material seem especially heavy for the large-scale application of related fields It wants.
Currently, the main method of regulation semiconductor material luminescent properties has the coupling of metal surface phasmon, laser irradiation With doping etc.;Wherein, metal surface phasmon coupling regulation belongs to non-intervention control measures, will not change the intrinsic category of material Property, when metal nano material surface phasmon energy matches with the luminous energy of semiconductor material, it can produce surface Plasmon resonance enhances the luminous intensity of semiconductor material.From nineteen fifty-seven Ritchie (Physical Review, 1957, 106,874-881) propose surface plasmon resonance concept since, this research achievement pushed significantly metal surface etc. from The development of excimer.2005, Ong etc. (Applied Physics Letters, 2005,86,251105) reported ZnO for the first time Band-edge emission enhances 10 times when film upper surface deposition thickness is the Ag film of 89nm, proposes that Ag surface phasmon leads to ZnO Free exciton combined efficiency increases, to realize luminous enhancing.2009, Liu et al. people (Applied Physics Letters, 2009,94,151102) by making Pt nano-pattern and Pt film on ZnO film, realize respectively 12 times and 2 times of band-edge emission enhancing, research find that periodicity Pt atomic energy provides a large amount of scattering medium, greatly improve light extraction Rate;2018, Ye et al. (Optics Letters, 2018,43,2288) discovery utilized Al-AlOxThe nonpolar ZnO of cladding is thin Film makes that ultraviolet emission enhances 84 times and internal quantum improves 8.3 times.Metal surface phasmon is mainly logical It crosses and makes Localized field enhancement with the resonance coupling of semiconductor material, to improve the luminous efficiency of material, but higher for having The internal quantum efficiency and lower high quality semiconductor material monocrystalline of defect luminescence or film, luminescence enhancement effect are not obvious.
In recent years, dielectric it is micro-/micro-nano structure because becoming in the ultraviolet high transmittance near infrared band realizes semiconductor material A kind of effective way of material/luminescent device all band luminescence enhancement;Wherein, optical dielectric microballoon is because having high quality factor With minimum mode volume, light field can be limited in specific region, improve intracavitary Photon state density, thus effectively enhancing light with Full spectral luminescence enhancing is realized in the interaction of substance.1961, Garrett (Physical Review, 1961,124, 1807) Whispering-gallery-mode of discovery dielectric microballoon excitation can effectively enhance luminous;2017, Yan et al. (Optics Express, 2017,25,6000) substrate and film thickness pair are had studied by dielectric micro-sphere array/luminescent film/substrate sandwich structure The influence of the luminescence enhancement of ZnO, 11.25 times of band-edge emission is realized by covering micro-sphere array on ZnO film to be enhanced, and Disclosing it enhances mechanism.
Dielectric microballoon has enhanced the luminous mechanism luminous with the enhancing of metal surface plasmon resonance of semiconductor material not Together, microballoon enhancing semiconductor material shines mainly improves the spontaneous radiation radiation efficiency of material using light field regulating effect, belongs to Enhance in full spectral luminescence, will not relate to electronics transfer.Therefore, by combining metal surface phasmon effect and dielectric micro- The advantage of spherical cavity light field regulating and controlling effect, on high-quality semiconductor light-emitting film surface, building dielectric microballoon/metal nanoparticle is multiple Closing structure is the effective way realizing semiconductor material luminous efficiency and being further obviously improved.
Summary of the invention
The present invention compensates for the shortcomings of the prior art, provides a kind of lamination for enhancing light-emitting film fluorescence radiation intensity Structure and preparation method thereof is applicable to the semiconductor light emitting film grown on any substrate, industrially has important push away Wide value.
To achieve the above object, the invention adopts the following technical scheme:
A kind of laminated construction enhancing light-emitting film fluorescence radiation intensity, the laminated construction includes stacking gradually connection Single layer dielectric micro-sphere array, light-emitting film and substrate, the difference is that, it further include being embedded in the light-emitting film and lining The first metal nano-particle layer between bottom, and the second gold medal being embedded between the light-emitting film and single layer dielectric micro-sphere array Metal nano-particle layer.
In the above-mentioned technical solutions, the microsphere diameter of the single layer dielectric micro-sphere array is 1.5-7.3 μm.
Preferably, in the above-mentioned technical solutions, the single layer dielectric micro-sphere array is single layer silicon dioxide microsphere array.
Further, in the above-mentioned technical solutions, first metal nano-particle layer and second metal nano Granulosa is respectively one of gold, silver, aluminium and platinum nanoparticle layer.
Further, in the above-mentioned technical solutions, first metal nano-particle layer and second metal nano The thickness of granulosa distinguishes 15-20nm and 10-15nm.
Still further, in the above-mentioned technical solutions, first metal nano-particle layer is the Jenner with a thickness of 16nm Rice grain layer, wherein the partial size of gold nano grain is 15-17.5nm, spacing 2.5-3.6nm.
Still further, in the above-mentioned technical solutions, second metal nano-particle layer is to receive with a thickness of the aluminium of 10nm Rice grain layer, wherein the partial size of aluminum nanoparticles is 9.5-10.6nm, spacing 1.6-2.4nm.
Also further, in the above-mentioned technical solutions, the light-emitting film is zinc-oxide film, carborundum films, nitridation One of gallium film and aluminium nitride film, the light-emitting film with a thickness of 200-450nm.
Also further, in the above-mentioned technical solutions, the substrate is signle crystal alumina, mono-crystal gallium nitride and monocrystalline silicon lining One of bottom.
Another aspect of the present invention provides a kind of preparation method of laminated construction for enhancing light-emitting film fluorescence radiation intensity, Successively the following steps are included:
S1, the first metal nano-particle layer is sputtered on the substrate of clean dried;
S2, light-emitting film is prepared in first metal nano-particle layer upper surface;
S3, the second metal nano-particle layer is sputtered in the light-emitting film upper surface;
S4, configuration dielectric microballoon suspension, and dielectric microballoon suspension is passed through into natural sedimentation in the second metal nano Stratum granulosum upper surface is self-assembly of the single layer dielectric micro-sphere array in close paving state.
In detail, above-mentioned preparation method further includes the pretreatment of substrate, is specifically included: substrate is dipped in acetone first, Then ultrasonic cleaning 2-3 time, each 5-10min is impregnated and is surpassed with ethyl alcohol with the chemistry spot such as organic matter for removing substrate surface Sound cleans for several times, further to remove pollutant and acetone remained on surface, deionized water repeated flushing substrate is finally used, in room Middle benefit gas is dry.
In the above-mentioned technical solutions, in step S4, the natural sedimentation self assembling process of the single layer dielectric micro-sphere array Specifically: by dropper by the suspended drop-coated of dielectric microballoon in the second inclined metal nano-particle layer upper surface, list Layer dielectric micro-sphere array is self-assembly of under liquid tension effect by the evaporation of solvent in dielectric microballoon suspension.
Preferably, in the above-mentioned technical solutions, in step S4, the solvent of the dielectric microballoon suspension is volatile molten One of agent, specially deionized water, ethyl alcohol and isopropanol.
Still further, in the above-mentioned technical solutions, in step S4, the tilt angle of second metal nano-particle layer For 5-10 degree.
In detail, in actual fabrication process, in step s 4, it can place it in and to be 5-10 ° with inclination angle and incline On the closed box of sloping platform, the close paving battle array of single layer is preferably formed to reduce in the case that outside air flowing prepares micro-sphere array Column.
Further, in the above-mentioned technical solutions, first metal nano-particle layer and second metal nano The preparation method of stratum granulosum is vacuum ion sputtering method.
Further, in the above-mentioned technical solutions, the preparation method of the light-emitting film is molecular beam epitaxy, magnetic control One of sputtering method and pulsed laser deposition.
Compared with prior art, the present invention has the advantage that
(1) the present invention provides a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity, the structure preparation costs It is cheap, method is simple, technique is time-consuming short and is not limited by any substrate, the hair suitable for high-quality semiconductor light-emitting film Light enhancing;
(2) preparation method of a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity provided by the present invention, root It is asked according to the difference of practical application, adjusts the technological parameter of metal nano-particle layer, it is special to may make that surface plasmon resonance absorbs Property in the ultraviolet extensive region to visible light be continuously adjusted;
(3) the single layer dielectric microballoon battle array in the laminated construction of enhancing light-emitting film fluorescence radiation intensity provided by the present invention Column in air stablize by physicochemical properties, can enhance the luminous intensity of light-emitting film steadily in the long term;
(4) laminated construction of enhancing light-emitting film fluorescence radiation intensity provided by the present invention combines dielectric microballoon light field The collective effect of regulation and metal surface phasmon coupling effect, may make the luminous intensity of light-emitting film to significantly increase, far Much higher than the reinforcing effect that metal nano-particle layer or single layer dielectric micro-sphere array is used alone.
Detailed description of the invention
Fig. 1 is a kind of structure for the laminated construction for enhancing light-emitting film fluorescence radiation intensity provided by the embodiment of the present invention Schematic diagram;
Fig. 2 is that the embodiment of the present invention 1 is splashed by ion sputtering instrument in the case where vacuum degree is 8Pa, electric current is 10mA on substrate Penetrate the stereoscan photograph of the preparation-obtained gold nano grain layer of 30s;
Fig. 3 be the embodiment of the present invention 1 on gold nano grain layer by pulse laser deposition instrument be prepared with a thickness of The stereoscan photograph of the zinc oxide luminescent film of 300nm;
Fig. 4 be the embodiment of the present invention 1 on zinc oxide luminescent film by ion sputtering instrument vacuum degree be 8Pa, electric current For the stereoscan photograph for sputtering the preparation-obtained aluminum nanoparticles layer of 32s under 8mA;
Fig. 5 is the preparation method schematic diagram that single layer dielectric micro-sphere array is prepared in the embodiment of the present invention;
Fig. 6 is the laser copolymerization for the single layer dielectric micro-sphere array pattern that diameter prepared in the embodiment of the present invention 1 is 5 μm Burnt flying-spot microscope photo;
Fig. 7 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 1 Change the normalization luminescent spectrum comparison diagram of zinc film;
Fig. 8 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 2 Change the normalization luminescent spectrum comparison diagram of zinc film;
Fig. 9 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 3 Change the normalization luminescent spectrum comparison diagram of zinc film;
Figure 10 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 4 Change the normalization luminescent spectrum comparison diagram of zinc film;
Figure 11 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 5 Change the normalization luminescent spectrum comparison diagram of zinc film;
Figure 12 is the laminated construction and pure oxygen of enhancing light-emitting film fluorescence radiation intensity prepared in the embodiment of the present invention 6 Change the normalization luminescent spectrum comparison diagram of zinc film;
Figure 13 is that the laminated construction of enhancing light-emitting film fluorescence radiation intensity prepared in comparative example 1 of the present invention (is free of Single layer dielectric micro-sphere array) with the normalization luminescent spectrum comparison diagram of pure zinc oxide film;
Figure 14 is that the laminated construction of enhancing light-emitting film fluorescence radiation intensity prepared in comparative example 2 of the present invention (is free of First metal nano-particle layer and the second metal nano-particle layer) with the normalization luminescent spectrum comparison diagram of pure zinc oxide film;
In figure:
A, dielectric micro-sphere array, B, the second metal nano-particle layer, C, light-emitting film, D, the first metal nano-particle layer, E, substrate;
1, dielectric microballoon suspension, 2, rubber head dropper, 3, suspended drop, the 4, second metal nano-particle layer, 5, shine it is thin Film, the 6, first metal nano-particle layer, 7, substrate, 8, the tilting table that inclination angle is 5-10 °, 9, suspension drop infiltration lamination knot Structure surface, 10, be formed by single layer dielectric micro-sphere array after the solvent evaporation in suspension drop;
A, enhance the normalization luminescent spectrum figure of the laminated construction of light-emitting film fluorescence radiation intensity, b, pure zinc oxide film Normalize luminescent spectrum figure, c, the laminated construction (be free of single layer dielectric micro-sphere array) for enhancing light-emitting film fluorescence radiation intensity Luminescent spectrum figure is normalized, d, the laminated construction for enhancing light-emitting film fluorescence radiation intensity (are free of the first metal nano-particle layer With the second metal nano-particle layer) normalization luminescent spectrum figure.
Specific embodiment
With reference to the accompanying drawings and examples, specific embodiments of the present invention will be described in further detail.
Following embodiment is merely to illustrate the present invention, the protection scope being not intended to limit the invention.
Experimental method used in following embodiment is conventional method unless otherwise specified.
Material used in following embodiment, reagent etc., are commercially available unless otherwise specified.
The embodiment of the invention provides a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity, specifically such as Fig. 1 institute Show, single layer dielectric micro-sphere array, the second metal nano-particle layer, light-emitting film, the first metal including stacking gradually connection are received Rice grain layer and substrate;Preparation method includes:
(1) substrate clean and drying pre-processes;
(2) vacuum ion sputtering instrument is used, suitable metal target is selected, sample chamber pressure and sputtering current is adjusted, is serving as a contrast Bottom surface sputters the first metal nano-particle layer;
(3) using molecular beam epitaxy, magnetron sputtering method or pulsed laser deposition in the first metal nano-particle layer Surface prepares light-emitting film, for example, preparing the specific steps of light-emitting film zinc oxide luminescent film using pulsed laser deposition It is as follows: the sample that sputtering has the first metal nano-particle layer being placed on the silicon heater in settling chamber first, utilizes machinery After deposition room pressure is evacuated to 2.0Pa by pump, molecular pump pumping high vacuum is opened, reaches 10 to vacuum degree-4When Pa or so, closes and divide Son pump, is then passed through a certain amount of oxygen into settling chamber, opens silicon heater, and adjusting silicon plate electric current rises temperature slowly To preset temperature, then by the laser beam line focus lens focus of KrF excimer laser on zinc oxide ceramic target, so that Plasma plume brightness uniform fold sample, can start deposition film, by silicon heater in settling chamber after finally growing Temperature is slowly adjusted to room temperature, takes out zinc-oxide film, and specifically, deposition indoor oxygen pressure is 45Pa, silicon heater temperature Degree is 400 DEG C.KrF excimer laser parameter is energy 300mJ, frequency 3Hz, umber of pulse 2500, obtained zinc oxide films Film thickness is 300nm;
(4) vacuum ion sputtering instrument is used, suitable metal target is selected, sample chamber pressure and sputtering current is adjusted, is sending out Optical thin film surface sputters the second metal nano-particle layer;
(5) dielectric microballoon suspension is configured, and dielectric microballoon suspension is passed through into natural sedimentation in the second metal nano Stratum granulosum upper surface is self-assembly of the single layer dielectric micro-sphere array in close paving state, and specific steps are as shown in Figure 5, comprising: first First configure dielectric microballoon suspension 1;Then configured suspension 1 is used into 2 drawing section of dropper after the ultrasonic several seconds in Ultrasound Instrument Divide suspension 1, and by 3 the second metal nano-particle layer of drop coating surface of suspended drop in dropper 2, then places it in inclination angle and be In the closed box of 5-10 ° of tilting table 8, brought influence, suspension are prepared to reduce outside air flowing to micro-sphere array Drop 3 gradually forms the close paving array of single layer with solvent volatilization, wherein the solvent of dielectric microballoon suspension is easy volatile solvent, such as Deionized water, ethyl alcohol or isopropanol, concentration 104-106μL-1;The diameter of dielectric microballoon used is 1.5-7.3 μm.
Embodiment 1
Alumina single crystal substrate is cleaned up, after being spontaneously dried in room temperature, is put on ion sputtering instrument sample table, target Material is gold target, intracavitary pressure is adjusted to 8Pa, sputtering current is set as 10mA, and sputtering time is set as 30s, so that gold nano For grain uniform deposition in alumina substrate, nano particle diameter is about 16nm, and the scanning electron microscope of the gold nano grain of preparation is aobvious Micro- figure is as shown in Figure 2.
It will prepare on the silicon heater that the sample containing gold nano grain is put into pulse laser deposition instrument settling chamber, Molecular pump pumping high vacuum is opened after settling chamber's air pressure is evacuated to 2.0Pa using mechanical pump, reaches 10 to vacuum degree-4When Pa or so, Close molecular pump;Then a certain amount of oxygen is passed through into settling chamber, adjusting silicon plate electric current makes temperature be raised slowly to 400 DEG C Afterwards, KrF excimer laser is focused on zinc oxide ceramic target, the distance between target and sample are 5cm, so that plasma Body feathers brightness uniform fold sample starts deposition film.Wherein, energy of lasers 300mJ, frequency 3Hz, umber of pulse are 2500, growth is about the zinc-oxide film of 300nm thickness.Silicon heater temperature is slowly adjusted to room temperature after growth, is taken The zinc-oxide film of zinc-oxide film out, preparation is as shown in Figure 3.
The zinc-oxide film that the sputtering prepared has gold nano grain is put on ion sputtering instrument sample table, target replacement For aluminium target, intracavitary pressure is adjusted to 8Pa, and sputtering current is set as 8mA, sputters the aluminum nanoparticles of 32s in sample surfaces, preparation The scanning electron microscope micrograph of aluminum nanoparticles is as shown in Fig. 4.
The transparent dielectric microballoon that diameter is 5 μm is mixed with deionized water, forms microballoon suspension as shown in Figure 5, it is small Ball concentration is 4 × 104μL-1;The dropper shown in Fig. 5 draws part microballoon suspension, drips the metal nano for being 5 ° at inclination angle On grain sandwich structure, sample surfaces are infiltrated;At room temperature, it after the deionized water evaporation of sample surfaces, obtains as attached The laminated construction of enhancing light-emitting film fluorescence radiation intensity shown in FIG. 1, dielectric micro-sphere array pattern are as shown in Figure 6.
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 160 times of luminous intensity b, as a result as shown in Figure 7.
Embodiment 2
The preparation process of the embodiment of the present invention is similar to Example 1, the difference is that, aluminum nanoparticles are prepared in sputtering When, sputtering time 24s;In addition, when configuring dielectric microballoon suspension, by diameter be 1.5 μm transparent dielectric microballoon with Ethyl alcohol mixing, concentration of small ball are 1 × 106μL-1
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 101 times of luminous intensity b, as a result as shown in Figure 8.
Embodiment 3
The preparation process of the embodiment of the present invention is similar to Example 1, the difference is that, selected substrate is monocrystalline silicon Substrate;When sputtering prepares aluminum nanoparticles, sputtering time 28s;In addition, when configuring dielectric microballoon suspension, it will be straight Diameter is that 3.9 μm of transparent dielectric microballoon is mixed with ethyl alcohol, and concentration of small ball is 6 × 105μL-1
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 97 times of luminous intensity b, as a result as shown in Figure 9.
Embodiment 4
The preparation process of the embodiment of the present invention is similar to Example 1, the difference is that, selected substrate is monocrystalline nitrogen Change gallium substrate;When sputtering prepares aluminum nanoparticles, sputtering time 32s;In addition, when configuring dielectric microballoon suspension, The transparent dielectric microballoon that diameter is 5 μm is mixed with isopropanol, concentration of small ball is 5 × 105μL-1
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 160 times of luminous intensity b, the results are shown in Figure 10.
Embodiment 5
The preparation process of the embodiment of the present invention is similar to Example 1, the difference is that, selected substrate is monocrystalline two Silicon oxide substrate;When sputtering prepares aluminum nanoparticles, sputtering time 36s;In addition, in configuration dielectric microballoon suspension When, the transparent dielectric microballoon that diameter is 6.5 μm is mixed with ethyl alcohol, concentration of small ball is 2 × 104μL-1
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 146 times of luminous intensity b, as a result as shown in figure 11.
Embodiment 6
The preparation process of the embodiment of the present invention is similar to Example 1, the difference is that, aluminum nanoparticles are prepared in sputtering When, sputtering time 40s;In addition, when configuring dielectric microballoon suspension, by diameter be 7.3 μm transparent dielectric microballoon with Isopropanol mixing, concentration of small ball are 1 × 104μL-1
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength a is pure zinc oxide film hair 135 times of luminous intensity b, as a result as shown in figure 12.
Comparative example 1
The preparation process of comparative example of the present invention is similar to Example 1, the difference is that, in the second metal nano-particle layer On do not prepare single layer dielectric micro-sphere array.
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength c is pure zinc oxide film hair 36.5 times of luminous intensity b, as a result as shown in figure 13.
Comparative example 2
The preparation process of comparative example of the present invention is similar to Example 1, the difference is that, without being embedded in light-emitting film and The first metal nano-particle layer between substrate and be embedded between the light-emitting film and single layer dielectric micro-sphere array second Metal nano-particle layer.
The film is excited using 325nm uv excitation light, gained 376nm wavelength luminescence strength d is pure zinc oxide film hair 4.4 times of luminous intensity b, as a result as shown in figure 14.
Finally, being not intended to limit the scope of the present invention the above is only preferred embodiment of the invention.It is all this Within the spirit and principle of invention, any modification, equivalent replacement, improvement and so on should be included in protection model of the invention Within enclosing.

Claims (10)

1. a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity, the laminated construction includes the list for stacking gradually connection Layer dielectric micro-sphere array, light-emitting film and substrate, which is characterized in that further include being embedded between the light-emitting film and substrate The first metal nano-particle layer, and the second metal nano being embedded between the light-emitting film and single layer dielectric micro-sphere array Stratum granulosum.
2. a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 1, which is characterized in that institute The microsphere diameter for stating single layer dielectric micro-sphere array is 1.5-7.3 μm;Preferably, the single layer dielectric micro-sphere array is single layer dioxy SiClx micro-sphere array.
3. a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 1 or 2, feature exist In,
First metal nano-particle layer and second metal nano-particle layer are respectively gold, silver, aluminium and Pt nanoparticle One of layer;
And/or first metal nano-particle layer and second metal nano-particle layer thickness difference 15-20nm and 10-15nm。
4. a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 3, which is characterized in that
First metal nano-particle layer is the gold nano grain layer with a thickness of 16nm, wherein the partial size of gold nano grain is 15-17.5nm, spacing 2.5-3.6nm;
And/or second metal nano-particle layer is the aluminum nanoparticles layer with a thickness of 10nm, wherein aluminum nanoparticles Partial size is 9.5-10.6nm, spacing 1.6-2.4nm.
5. a kind of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 1-4, special Sign is,
The light-emitting film is one of zinc-oxide film, carborundum films, gallium nitride film and aluminium nitride film, the hair Optical thin film with a thickness of 200-450nm;
And/or the substrate is one of signle crystal alumina, mono-crystal gallium nitride and monocrystalline substrate.
6. it is a kind of enhance light-emitting film fluorescence radiation intensity laminated construction preparation method, which is characterized in that successively include with Lower step:
S1, the first metal nano-particle layer is sputtered on the substrate of clean dried;
S2, light-emitting film is prepared in first metal nano-particle layer upper surface;
S3, the second metal nano-particle layer is sputtered in the light-emitting film upper surface;
S4, configuration dielectric microballoon suspension, and dielectric microballoon suspension is passed through into natural sedimentation in the second metal nanoparticle Layer upper surface is self-assembly of the single layer dielectric micro-sphere array in close paving state.
7. a kind of preparation method of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 6, It is characterized in that, in step S4, the natural sedimentation self assembling process of the single layer dielectric micro-sphere array specifically: will by dropper The suspended drop-coated of dielectric microballoon passes through in the second inclined metal nano-particle layer upper surface, single layer dielectric micro-sphere array The evaporation of solvent is self-assembly of under liquid tension effect in dielectric microballoon suspension;
Preferably, the solvent of the dielectric microballoon suspension is easy volatile solvent, specially in deionized water, ethyl alcohol and isopropanol One kind.
8. a kind of preparation method of laminated construction for enhancing light-emitting film fluorescence radiation intensity according to claim 7, It is characterized in that, in step S4, the tilt angle of second metal nano-particle layer is 5-10 degree.
9. according to a kind of described in any item preparations for the laminated construction for enhancing light-emitting film fluorescence radiation intensity of claim 6-8 Method, which is characterized in that the preparation method of first metal nano-particle layer and second metal nano-particle layer is true Empty ion sputtering process.
10. according to a kind of described in any item systems for the laminated construction for enhancing light-emitting film fluorescence radiation intensity of claim 6-8 Preparation Method, which is characterized in that the preparation method of the light-emitting film is that molecular beam epitaxy, magnetron sputtering method and pulse laser are heavy One of area method.
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CN110993754A (en) * 2019-12-04 2020-04-10 南京邮电大学 LED tube core with bionic metal nano island-shaped structure and preparation method thereof
CN111239088A (en) * 2020-01-17 2020-06-05 中山大学 Micro-nano composite structure with fluorescence enhancement and optical amplification effects and preparation method thereof
CN111755579A (en) * 2020-06-15 2020-10-09 西安电子科技大学 Zinc oxide based light emitting diode and manufacturing method thereof
CN113725341A (en) * 2021-08-23 2021-11-30 广东工业大学 Method for improving quantum dot light intensity

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CN110993754A (en) * 2019-12-04 2020-04-10 南京邮电大学 LED tube core with bionic metal nano island-shaped structure and preparation method thereof
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