CN103078031A - Nano silver ring local surface plasmon enhanced light emitting diode and preparation method thereof - Google Patents
Nano silver ring local surface plasmon enhanced light emitting diode and preparation method thereof Download PDFInfo
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical group [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 229910004205 SiNX Inorganic materials 0.000 claims abstract description 37
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 32
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000010703 silicon Substances 0.000 claims abstract description 31
- 239000000758 substrate Substances 0.000 claims abstract description 13
- 239000010408 film Substances 0.000 claims description 33
- 239000002077 nanosphere Substances 0.000 claims description 21
- 238000000151 deposition Methods 0.000 claims description 13
- 238000007254 oxidation reaction Methods 0.000 claims description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 10
- 230000003647 oxidation Effects 0.000 claims description 10
- 230000008021 deposition Effects 0.000 claims description 8
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 6
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 5
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 claims description 5
- 229910021529 ammonia Inorganic materials 0.000 claims description 5
- 238000009826 distribution Methods 0.000 claims description 5
- 239000012528 membrane Substances 0.000 claims description 5
- 229910000077 silane Inorganic materials 0.000 claims description 5
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 5
- 239000010409 thin film Substances 0.000 claims description 5
- 239000011324 bead Substances 0.000 claims description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 3
- 238000004140 cleaning Methods 0.000 claims description 3
- 239000003595 mist Substances 0.000 claims description 3
- 230000002093 peripheral effect Effects 0.000 claims description 3
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 claims description 2
- 229910052751 metal Inorganic materials 0.000 abstract description 7
- 239000002184 metal Substances 0.000 abstract description 7
- 230000005693 optoelectronics Effects 0.000 abstract description 3
- 239000000463 material Substances 0.000 abstract description 2
- 239000004793 Polystyrene Substances 0.000 description 16
- 239000010410 layer Substances 0.000 description 14
- 238000000034 method Methods 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 8
- 238000005516 engineering process Methods 0.000 description 5
- 238000004020 luminiscence type Methods 0.000 description 5
- 239000000377 silicon dioxide Substances 0.000 description 4
- 238000011065 in-situ storage Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 230000005684 electric field Effects 0.000 description 2
- 238000005401 electroluminescence Methods 0.000 description 2
- 238000005566 electron beam evaporation Methods 0.000 description 2
- 230000002708 enhancing effect Effects 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 239000002096 quantum dot Substances 0.000 description 2
- UMVBXBACMIOFDO-UHFFFAOYSA-N [N].[Si] Chemical compound [N].[Si] UMVBXBACMIOFDO-UHFFFAOYSA-N 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 239000013528 metallic particle Substances 0.000 description 1
- 238000004377 microelectronic Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000005622 photoelectricity Effects 0.000 description 1
- 238000005424 photoluminescence Methods 0.000 description 1
- 238000000103 photoluminescence spectrum Methods 0.000 description 1
- 238000000623 plasma-assisted chemical vapour deposition Methods 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 239000002094 self assembled monolayer Substances 0.000 description 1
- 239000013545 self-assembled monolayer Substances 0.000 description 1
- 238000001338 self-assembly Methods 0.000 description 1
- 230000003595 spectral effect Effects 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
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Abstract
The invention relates to a nano silver ring local surface plasmon enhanced light emitting diode and a preparation method thereof, which belong to the technical field of nano optoelectronic device materials. The diode comprises a P type silicon substrate, a nano silver ring and an oxygen-doped a-SiNx:O film glowing active layer, wherein the nano silver ring is arranged on the P type silicon substrate, the oxygen-doped a-SiNx:O film glowing active layer is deposited on the nano silver ring and covers the P type silicon substrate, a metal electrode is evaporated on an oxygen-doped a-SiNx:H glowing active layer, and a window is left. According to the light emitting diode and the preparation method, the glowing active layer and the nano metal ring are organically combined, so as to really prepare the silicon substrate local surface plasmon enhanced light emitting diode with a controllable wavelength.
Description
Technical field
Invention relates to a kind of silicon base luminescence diode, and especially a kind of applying nano silver dollar ring local surface phasmon strengthens the silica-based controlled wavelength light-emitting diode of luminous efficiency, also relates to simultaneously its preparation method, belongs to nano photoelectronic devices material technology field.
Background technology
The light emission effciency that improves silica-based light source is to realize at present the integrated bottleneck of monolithic silicon based photoelectricity.Theoretical research shows, the internal quantum efficiency that the local surface phasmon by nano metal improves si-based light-emitting device might become the effective way that addresses this problem.
In recent years, nano metal local surface phasmon is being obtained breakthrough progress aspect the luminous efficiency that strengthens si-based light-emitting device, Korea S Seone-Ju Park group in 2008 has reported that the local surface phasmon that utilizes nano-Ag particles strengthens the silicon quantum dot light-emitting diode, in this structure, the metallic particles layer is placed between luminescent layer and the substrate, coupling between Si quantum dot and local surface plasmon has strengthened radiation recombination probability [1], this research group has arrived similar structure applications in the InGaN/GaN quantum well light-emitting diode again, makes the power output of light-emitting diode improve 32%[2].
Understand according to the applicant, up to the present, research group mainly adopts the luminous efficiency of the silicon base luminescence diode that the local surface phasmon of nano-metal particle strengthens in the world, but the surface phasmon of applying nano silver dollar ring strengthens the silicon base luminescence diode so far there are no report.
Summary of the invention
The object of the invention is to: the local surface phasmon that proposes a kind of at room temperature applying nano silver dollar ring strengthens the silicon base luminescence diode of the controlled wavelength of luminous efficiency, thereby satisfies development in science and technology to the demand of opto-electronic device.Provide simultaneously its preparation method, the method is compatible mutually with current microelectronic technique, thereby can conscientiously be applied to following silicon-based nano optoelectronics device.
In order to reach following purpose, Nano Silver annulus local surface plasmon enhancement type light-emitting diode of the present invention comprises P type silicon base, distribution Nano Silver circle ring array on the described P type silicon base (size and the position of Nano Silver annulus wherein can be controlled, and can be described as in order controlled nano metal annulus); Described Nano Silver circle ring array is covered by the oxygen-doped a-SiNx:O thin-film light emitting active layer of deposition on the P type silicon base; Deposit reserves the electrode of window on the described a-SiNx:H thin-film light emitting active layer.
Nano Silver annulus local surface plasmon enhancement type light-emitting diode of the present invention prepares basic process and may further comprise the steps:
Step 1, construct the Nano Silver annulus
The first step, lay the PS(polystyrene in P type silicon base) the monofilm bead of nanosphere;
Second step, (adopting the technological means such as electron beam evaporation) are being equipped with depositing nano silver film on the P type silicon substrate of PS nanosphere;
The temperature of the 3rd step, control P type silicon substrate is at 50-80 ℃, and the deposition rate of control Nano Silver is the 0.1-0.3 nm/sec, makes nano-Ag particles center on the ring-like peripheral continuous distribution of PS nanosphere;
The 4th goes on foot, the PS nanosphere that is surrounded by Nano Silver around above-mentioned is immersed in the carrene, passes through the successively cleaning of acetone and alcohol again, removes the PS nanosphere, obtains required Nano Silver circle ring array;
Step 2, construct light-emitting active layer---at the Surface disintegration silane of Nano Silver circle ring array and the mist of ammonia, deposit a-SiNx:H film carries out oxidation to the a-SiNx:H film again, obtains the light-emitting active layer that oxygen-doped a-SiNx:O film forms;
Step 3, construct membrane electrode---deposition of electrode on the light-emitting active layer that oxygen-doped a-SiNx:H film forms, and reserve window.
The present invention makes the combination of light-emitting active layer and nano metal annulus, can conscientiously realize the preparation of the light-emitting diode of the controlled wavelength that silica-based local surface phasmon strengthens, and has following remarkable advantage:
1) can obtain the controlled Nano Silver annulus of size by the PS nanosphere of selecting the different-diameter size, for the regulation and control of the absorbing wavelength of local surface phasmon are laid a good foundation;
2) the controllable luminous wavelength of light-emitting active layer provides assurance for the resonance absorption that realizes the local surface phasmon;
3) low temperature preparation, technique is simple, and is compatible, easy to utilize mutually with semi-conductive silicon technology;
4) the in-situ oxidation technique guarantee cleannes of sample surfaces.
Description of drawings
The present invention is further illustrated below in conjunction with accompanying drawing.
Fig. 1 (a), Fig. 1 (b), Fig. 1 (c) and Fig. 1 (d) are respectively each technical process schematic diagrames of one embodiment of the invention.
Fig. 2 is the sample cross-section structural representation that Fig. 1 embodiment makes.
Fig. 3 is the AFM picture after Fig. 1 embodiment Nano Silver annulus is made.
Embodiment
Embodiment one
The Nano Silver annulus local surface plasmon enhancement type light-emitting diode of the present embodiment adopts the preparation of technical process shown in Fig. 1 (a), Fig. 1 (b), Fig. 1 (c) and Fig. 1 (d).
Step 1, construct the Nano Silver annulus
The first step, shown in Fig. 1 (a), adopt self-assembly method to lay the monofilm bead of the PS nanosphere of ordered arrangement in P+ type silicon base; Nanosphere is available from Duke company, and concentration is 10wt.%, and the size of nanosphere changes to 170 nanometers from 300 nanometers, and standard deviation is less than 10%.Concrete operations are, first the PS nanosphere are self-assembled into monofilm at liquid level, film are transferred on the substrate natural volatile dry in air again.
Second step, shown in Fig. 1 (b), adopt electron beam evaporation equipment, be equipped with hydatogenesis nano silver film on the P+ type silicon substrate of PS nanosphere, the THICKNESS CONTROL of film is in the 80-150 nanometer.
The temperature of the 3rd step, control P+ type silicon substrate is at 50-80 ℃, and the deposition rate of control Nano Silver is the 0.1-0.3 nm/sec, makes nano-Ag particles center on the ring-like peripheral continuous distribution of PS nanosphere.
The 4th step, shown in Fig. 1 (c), the PS nanosphere that is surrounded by Nano Silver around above-mentioned is immersed in the carrene, pass through again the successively cleaning of acetone and alcohol, and by ultrasonic wave, remove the PS nanosphere, obtains required orderly controlled Nano Silver circle ring array.The diameter of Nano Silver annulus can be by choosing the diameter change of PS nanosphere.
Step 2, construct light-emitting active layer---shown in Fig. 1 (d), adopt the PECVD method to decompose the mist of silane and ammonia on the surface of controlled in order Nano Silver circle ring array, deposit a-SiNx:H film, again the a-SiNx:H film is carried out oxidation, obtain the light-emitting active layer that oxygen-doped a-SiNx:O film forms.This step can be 200710020068.6 Chinese patent literature referring to application number, wherein be oxidized to in-situ plasma oxidation, perhaps thermal oxidation.
Control ammonia/silane (NH
3/ SiH
4) flow-rate ratio, can make the oxygen-doped a-SiNx:H film of different nitrogen components, thereby obtain the a-SiNx:H film of different emission wavelengths.By changing gas NH
3/ SiH
4Flow-rate ratio R, be increased to 8 from 0.5, reach and change in the a-SiNx:H film N component and be increased to 0.89 from 0.33, the emission wavelength of controlled made membrane changes to 650 nanometers from 425 nanometers.
More specifically, this step by computer control mass flowmenter switch, is decomposed SiH in reative cell in the plasma reinforced chemical vapor deposition system
4And NH
3Deposit a-SiNx: H film, and then to a-SiNx: the H layer carries out the pure oxygen plasma oxidation and obtains oxygen-doped silicon nitride a-SiNx: O, by 80 to the 100 seconds time controlling oxygen-doped silicon nitride deposition, a-SiNx at substrate preparation different-thickness: the H film, a-SiNx: the excursion of H film thickness is controlled at 80 and is advisable to 100nm.The power of plasma oxidation is 50 watts, and oxidization time is 30 minutes to 60 minutes.Adopt the He-Cd laser laser spectrum analyser of 325 nm to carry out the measurement of photoluminescence spectrum, determine a-SiNx: the content ratio of Si and N in the membrane component of the photoluminescence wavelength λ of H film and correspondence thereof.
Step 3, construct membrane electrode---deposition of electrode on the light-emitting active layer that oxygen-doped a-SiNx:H film forms, and reserve window.
The strongest absorbing wavelength of above local surface phasmon is mainly recently selected by the diameter of adjusting argent annulus and the thickness of ring, the emission wavelength of oxygen-doped silicon nitride film is then recently realized by regulation and control silicon nitrogen component, when the emission wavelength of the strongest absorbing wavelength of local surface phasmon and oxygen-doped silicon nitride film approaches when resonance absorption occurs, the enhancing luminescent effect of local surface phasmon is the most remarkable.The local surface phasmon enhancing absorbing wavelength that experiment showed, the Nano Silver annulus can be adjusted variation between minimum value 300 nanometers and maximum 800 nanometers.Top and bottom at the present embodiment sample add electric field, the I-V characteristic of test sample, and test with photomultiplier, the electroluminescence spectrogram that sends from window proves, can obtain the emission wavelength from 425 nm to 650nm, thereby become silica-based controlled wavelength light-emitting diode shown in Figure 2, on P+ type silicon base, obtain the Nano Silver circle ring array take the PS bead as mask; The Nano Silver circle ring array is formed light-emitting active layer by the oxygen-doped a-SiNx:O film of deposition on the P type silicon base and covers; Evaporated metal electrode on the a-SiNx:H light-emitting active layer, and reserve window.Top and bottom at sample add electric field, and the I-V characteristic of test sample can record the electroluminescence spectrogram that sends from window with photomultiplier.
AFM photo after the Nano Silver annulus is made as shown in Figure 3, the evaporation Nano Silver obtains the Nano Silver circle ring array take self-assembled monolayer PS nanosphere as template on silicon chip, deposited amorphous SiNx:H film and obtain oxygen-doped a-SiNx:H film as active layer in conjunction with the technology of in-situ plasma oxidation on the silicon base with Nano Silver circle ring array.Detection shows, the oxygen-doped SiNx:O film of amorphous at room temperature has the stronger luminescence generated by light from the blue light to the red spectral band.
In addition to the implementation, the present invention can also have other execution modes.All employings are equal to the technical scheme of replacement or equivalent transformation formation, all drop on the protection range of requirement of the present invention.
[1]
B.‐H.?Kim,?C.‐H.?Cho,?J.‐S.?Mun,?M.‐K.?Kwon,?T.‐Y.?Park,?J.?S.?Kim,?C.?C.?Byeon,?J.
Lee,?and?S.‐J.?Park,?Adv.?Mater.?20,?3100?(2008)?
[2]
M.‐K.?Kwon,?J.‐Y.?Kim,?B.‐H.?Kim,?I.‐K.?Park,?C.‐Y.?Cho,?C.?C.?Byeon,?and?S.‐J.?Park,
Adv.?Mater.?20,?1253?(2008)
Claims (6)
1. a Nano Silver annulus local surface plasmon enhancement type light-emitting diode comprises P type silicon base, it is characterized in that: distribution Nano Silver circle ring array on the described P type silicon base; Described Nano Silver circle ring array is covered by the oxygen-doped a-SiNx:O thin-film light emitting active layer of deposition on the P type silicon base; Deposit reserves the electrode of window on the described a-SiNx:H thin-film light emitting active layer.
2. Nano Silver annulus local surface plasmon enhancement type light-emitting diode according to claim 1, it is characterized in that: the thickness of described a-SiNx:O film is the 80-150 nanometer.
3. the preparation method of a Nano Silver annulus local surface plasmon enhancement type light-emitting diode is characterized in that may further comprise the steps:
Step 1, construct the Nano Silver annulus
The first step, lay the monofilm bead of PS nanosphere in P type silicon base;
Second step, be equipped with on the P type silicon substrate of PS nanosphere depositing nano silver film;
The temperature of the 3rd step, control P type silicon substrate is at 50-80 ℃, and the deposition rate of control Nano Silver is the 0.1-0.3 nm/sec, makes nano-Ag particles center on the ring-like peripheral continuous distribution of PS nanosphere;
The 4th goes on foot, the PS nanosphere that is surrounded by Nano Silver around above-mentioned is immersed in the carrene, passes through the successively cleaning of acetone and alcohol again, removes the PS nanosphere, obtains required Nano Silver circle ring array;
Step 2, construct light-emitting active layer---at the Surface disintegration silane of Nano Silver circle ring array and the mist of ammonia, deposit a-SiNx:H film carries out oxidation to the a-SiNx:H film again, obtains oxygen-doped a-SiNx:O thin-film light emitting active layer;
Step 3, construct membrane electrode---deposition of electrode on the light-emitting active layer that oxygen-doped a-SiNx:H film forms, and reserve window.
4. the preparation method of described Nano Silver annulus local surface plasmon enhancement type light-emitting diode according to claim 3, it is characterized in that: in the described step 2, the flow-rate ratio of ammonia/silane is 0.5 to 8.
5. the preparation method of described Nano Silver annulus local surface plasmon enhancement type light-emitting diode according to claim 4 is characterized in that: in the described step 2, decompose first SiH
4And NH
3Deposit a-SiNx: the H film, and then to a-SiNx: the H layer carries out the pure oxygen plasma oxidation, obtains oxygen-doped a-SiNx: the O film.
6. the preparation method of described Nano Silver annulus local surface plasmon enhancement type light-emitting diode according to claim 5, it is characterized in that: the deposition time of the oxygen-doped silicon nitride film of control was at 80 to 100 seconds in the described step 2.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108831981A (en) * | 2018-06-19 | 2018-11-16 | 南京邮电大学 | A kind of light emitting diode |
| CN110444641A (en) * | 2019-08-13 | 2019-11-12 | 黄山博蓝特半导体科技有限公司 | A kind of graphical compound substrate of high brightness and preparation method thereof |
| CN111146338A (en) * | 2019-11-18 | 2020-05-12 | 华南师范大学 | Ferroelectric diode memory and preparation method thereof |
| CN113437164A (en) * | 2021-06-15 | 2021-09-24 | 南京理工大学泰州科技学院 | Photoconductive all-silicon solar blind ultraviolet detector and manufacturing method thereof |
| CN117937227A (en) * | 2024-03-20 | 2024-04-26 | 量晶显示(浙江)科技有限公司 | Light emitting structure, pixel unit and display device |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108831981A (en) * | 2018-06-19 | 2018-11-16 | 南京邮电大学 | A kind of light emitting diode |
| CN110444641A (en) * | 2019-08-13 | 2019-11-12 | 黄山博蓝特半导体科技有限公司 | A kind of graphical compound substrate of high brightness and preparation method thereof |
| CN111146338A (en) * | 2019-11-18 | 2020-05-12 | 华南师范大学 | Ferroelectric diode memory and preparation method thereof |
| CN111146338B (en) * | 2019-11-18 | 2022-12-06 | 华南师范大学 | Ferroelectric diode memory and preparation method thereof |
| CN113437164A (en) * | 2021-06-15 | 2021-09-24 | 南京理工大学泰州科技学院 | Photoconductive all-silicon solar blind ultraviolet detector and manufacturing method thereof |
| CN113437164B (en) * | 2021-06-15 | 2023-02-17 | 南京理工大学泰州科技学院 | Photoconductive all-silicon solar blind ultraviolet detector and manufacturing method thereof |
| CN117937227A (en) * | 2024-03-20 | 2024-04-26 | 量晶显示(浙江)科技有限公司 | Light emitting structure, pixel unit and display device |
| CN117937227B (en) * | 2024-03-20 | 2024-05-24 | 量晶显示(浙江)科技有限公司 | Light emitting structure, pixel unit and display device |
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Application publication date: 20130501 |