CN111613706B - Silicon-based red light emission enhanced heterojunction diode and preparation method thereof - Google Patents
Silicon-based red light emission enhanced heterojunction diode and preparation method thereof Download PDFInfo
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- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims abstract description 18
- 239000010703 silicon Substances 0.000 title claims abstract description 18
- 238000002360 preparation method Methods 0.000 title claims abstract description 7
- 239000000758 substrate Substances 0.000 claims abstract description 46
- 239000002131 composite material Substances 0.000 claims abstract description 8
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- 229910001316 Ag alloy Inorganic materials 0.000 claims abstract description 6
- PQTCMBYFWMFIGM-UHFFFAOYSA-N gold silver Chemical compound [Ag].[Au] PQTCMBYFWMFIGM-UHFFFAOYSA-N 0.000 claims abstract description 6
- 238000004528 spin coating Methods 0.000 claims abstract description 6
- 239000002073 nanorod Substances 0.000 claims abstract description 5
- 238000004140 cleaning Methods 0.000 claims description 14
- 238000000137 annealing Methods 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 8
- 239000013078 crystal Substances 0.000 claims description 2
- 238000007747 plating Methods 0.000 claims description 2
- 239000004065 semiconductor Substances 0.000 abstract description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 12
- 239000010931 gold Substances 0.000 description 9
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- 239000000203 mixture Substances 0.000 description 7
- 239000002086 nanomaterial Substances 0.000 description 7
- 229910052757 nitrogen Inorganic materials 0.000 description 6
- 229910021642 ultra pure water Inorganic materials 0.000 description 6
- 239000012498 ultrapure water Substances 0.000 description 6
- 238000001035 drying Methods 0.000 description 5
- 230000003287 optical effect Effects 0.000 description 5
- 238000011160 research Methods 0.000 description 5
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- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
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- 238000001291 vacuum drying Methods 0.000 description 1
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
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- H01L33/002—Devices characterised by their operation having heterojunctions or graded gap
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- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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Abstract
The invention discloses a gold-silver alloy nanorod induced silicon-based red light emission enhanced heterojunction diode and a preparation method thereof, wherein the red light emission diode consists of 4 parts: (a) a Ni/Au electrode vapor-deposited on the p-Si substrate; (b) a p-Si substrate; (c) conductive glass (ITO) covering the n-ZnO Ga micron line; (d) and spin-coating the n-ZnO of the gold-silver alloy nanorod (AuAgNRs) into the Ga microwire. The invention adopts Ga-doped ZnO micron line with higher carrier concentration, spin-coats AuAgNRs on the surface of the Ga-doped ZnO micron line, and constructs a heterojunction (AuAgNRs @ n-ZnO: Ga/p-Si) light-emitting diode with a composite structure by taking p-Si as a substrate. Compared with an n-ZnO Ga bare wire heterojunction (n-ZnO Ga/p-Si) light-emitting diode, under forward bias, the red light emission is obviously enhanced, and the application of a silicon-based semiconductor in the field of light-emitting diodes is promoted.
Description
Technical Field
The invention relates to the technical field of semiconductor photoelectronic devices, in particular to a gold-silver alloy nanostructure induced silicon-based red light emission enhanced heterojunction diode and a preparation method thereof.
Background
High-purity silicon is an important semiconductor material and is widely applied to the fields of solar cells, diodes, triodes, field effect transistors, integrated circuits and the like. Because the silicon element has huge reserve in the earth crust and is only second to the oxygen element, the silicon-based light-emitting diode has great potential application value. ZnO is used as a direct band gap semiconductor and has higher exciton binding energy (60eV) at normal temperature, and meanwhile, the ZnO micro-nano structure prepared by the CVD method has good crystallinity and a quadrilateral or hexagonal section structure, and the natural optical resonant cavity enables the ZnO micro-nano structure to be used for preparing a micro light-emitting device. Although many research groups research and improve heterojunction light-emitting diodes constructed by n-ZnO/p-Si, Si is an indirect bandgap semiconductor, and an insulating oxide thin film is easily formed on the surface of the semiconductor, so that the prepared light-emitting diodes have low efficiency. In basic science and application technology, especially in research of micro-luminescent devices, research of micro-nano luminescent devices and modulation of luminescent intensity and luminescent wavelength thereof are one of research hotspots. In recent years, with the development of micro-nano material synthesis technology, controllable synthesis of noble metal nanostructures such as gold and silver is realized, and the noble metal nanostructures have been used in the fields of photoelectrons, energy sources, biomedicine and the like due to good plasmon optical effect and especially local field enhancement characteristic. The gold-silver alloy nanorod (AuAgNRs) not only has adjustable optical characteristics, but also has high chemical stability and thermal stability. According to the invention, the heterojunction diode with the AuAgNRs @ n-ZnO: Ga/p-Si composite structure is constructed in a surface spin coating manner, and the improvement of the luminous intensity of the Si-based heterojunction light-emitting diode is realized.
Disclosure of Invention
The invention aims to provide a silicon-based red light emission enhanced heterojunction diode and a preparation method thereof. The AuAgNRs are spin-coated on the surface of an n-ZnO-Ga micron line with excellent crystallization quality, and a heterojunction light-emitting diode is constructed by taking p-Si as a substrate. By using AuAgNRs plasmon resonance, the red light emission of the Si-based diode is enhanced. Due to the red light and infrared window effect of atmosphere and biological tissues, the red light emission enhanced diode can be applied to the light source for manufacturing micro devices of biomedicine, detection and the like.
In order to achieve the purpose, the preparation method of the silicon-based red light emission enhanced heterojunction diode comprises the following steps:
(1) annealing the p-Si substrate, cleaning the p-Si substrate, and keeping the p-Si substrate flat and clean;
(2) plating Ni/Au electrodes on the cleaned p-Si substrate;
(3) spin-coating the prepared AuAgNRs on an n-ZnO-Ga micron line;
(4) cleaning the ITO, and keeping the ITO flat and clean;
(5) and (3) placing the AuAgNRs @ n-ZnO and Ga composite structure micrometer line obtained in the step (3) on the p-Si substrate obtained in the step (2), and covering the ITO cleaned in the step (4) on the structure micrometer line to construct the silicon-based red light emission enhanced heterojunction diode.
The annealing and cleaning method of the p-Si substrate in the step (1) comprises the following steps: and (3) placing the p-Si substrate in a high-temperature tube furnace, keeping the Ar gas atmosphere, and annealing at the temperature of 600-650 ℃ for 20 min. The p-Si substrate was then removed from the high temperature tube furnace and rapidly cooled with a nitrogen gun. And then putting the mixture into trichloroethylene, putting the mixture into an ultrasonic cleaning instrument for cleaning for 20min, and respectively putting the mixture into acetone, ethanol and ultrapure water for cleaning for 20min by the same method after cleaning. Finally, the cleaned substrate was blow-dried with a nitrogen gun. Wherein the size of the p-Si substrate is 2cm by 2 cm.
Preparing the p-Si substrate Ni/Au electrode in the step (2): covering a part of the p-Si substrate with a mask plate, and evaporating Ni/Au electrodes on the exposed part by using an electron beam evaporation instrument, wherein the thickness of the electrodes is 20-40 nm. The obtained electrode is in ohmic contact with a p-Si substrate and is used as an anode of a heterojunction.
And (3) preparing the AuAgNRs by spin coating on an n-ZnO-Ga micron wire: centrifugally cleaning the synthesized AuAgNRs with ultrapure water, taking a ZnO-Ga micron wire with good crystallization quality, dripping the cleaned AuAgNRs on the micron wire, and drying.
The method for cleaning ITO in the step (4) comprises the following steps: and putting the ITO into a glass beaker, respectively cleaning with trichloroethylene, acetone, ethanol and ultrapure water, and then blow-drying with a nitrogen gun.
The method for constructing the red light emission enhancement heterojunction in the step (5) comprises the following steps: under an optical microscope, the composite structure microwire is placed on a p-Si substrate, so that the microwire is fully contacted with the substrate, and then the ITO is placed on the microwire. The ITO is used as a cathode, and meanwhile, the device is well contacted. The Ni/Au electrode is not contacted with the micron line and the conductive glass. Electrons are transferred from ITO to n-ZnO Ga micron lines, holes are transferred from Ni/Au electrodes to the p-Si substrate, and the electrons and the holes are compounded and emit light in the contact area of the n-ZnO Ga micron lines and the p-Si substrate to form a heterojunction structure.
The invention has the beneficial effects that: by constructing the AuAgNRs @ n-ZnO: Ga/p-Si heterojunction structure, when forward bias is applied, an obvious red light enhancement phenomenon appears. The invention greatly improves the problem of weak luminous intensity of the Si-based light-emitting diode in a plasmon resonance mode.
Drawings
FIG. 1 is a schematic representation of a silicon-based red-emitting enhanced heterojunction diode of the present invention, (a) a Ni/Au electrode vapor-deposited on a p-Si substrate; (b) a p-Si substrate; (c) ITO conductive glass; (d) the AuAgNRs @ n-ZnO and Ga composite structure micron line.
FIG. 2 is a graph showing the rectifying characteristics of a silicon-based red light emission enhancement heterojunction diode according to the present invention.
FIG. 3 is a comparison of luminescence photographs of an n-ZnO: Ga/p-Si heterojunction (a) of the present invention and an AuAgNRs @ n-ZnO: Ga/p-Si heterojunction (b).
FIG. 4 shows the emission spectra of the n-ZnO: Ga/p-Si heterojunction and AuAgNRs @ n-ZnO: Ga/p-Si heterojunction of the present invention at the same current.
Detailed Description
The invention is further illustrated by the following examples.
In the silicon-based red light emission enhanced heterojunction diode, the adopted metal nano structure is AuAgNRs; the substrate is p-Si, the thickness of the substrate is 365-385 mu m, the size is 2cm x 2cm, the resistivity is 0.001-0.005 omega cm, and the crystal orientation is<100>Direction; the thickness of the electrode on the p-Si substrate is 20-40 nm; the electron concentration of the n-ZnO-Ga micron line is 1017～1019/cm3Electron mobility of 5-100 cm2V.s; the dimensions of the ITO used were 1.5cm by 2 cm.
Example 1:
the first step is as follows: and (3) placing the p-Si substrate in a high-temperature tube furnace for thermal annealing, wherein the annealing time is 20min, and the annealing temperature is 600 ℃. After annealing, the substrate was taken out of the tube furnace and immediately cooled with a nitrogen gun. And ultrasonically cleaning the mixture for 20min by respectively using trichloroethylene, acetone, ethanol and ultrapure water, drying the mixture by using a nitrogen gun after cleaning, keeping the mixture flat and dry, and then putting the mixture into a drying cabinet for later use.
The second step is that: covering a part of the cleaned p-Si substrate by a mask plate, placing the p-Si substrate into an electron beam evaporation instrument, evaporating a Ni/Au electrode on the exposed part to form an electrode with the thickness of 35nm, testing the conductive characteristic between the electrode and the p-Si substrate, and determining whether the p-Si substrate is in ohmic contact.
The third step: the prepared AuAgNRs sample is centrifugally cleaned once by a centrifuge and dispersed in ultrapure water. And taking a hexagonal n-ZnO-Ga micron wire to ensure the good crystallization quality, putting the hexagonal n-ZnO-Ga micron wire on a clean glass slide, putting the glass slide under an optical microscope, taking a drop of a cleaned AuAgNRs sample to be dropped on the micron wire, putting the micron wire into a vacuum drying box, vacuumizing and drying the micron wire for one hour at the temperature of 60 ℃, and taking the micron wire out for later use.
The fourth step: taking an ITO (indium tin oxide), cutting the ITO into 1.5cm by 2cm, wiping the surface cullet with a dust-free cloth, putting the ITO into a clean beaker, ultrasonically cleaning the ITO with trichloroethylene, acetone, ethanol and ultrapure water for 20min respectively, then blow-drying the ITO with a nitrogen gun, and putting the cleaned ITO into a drying cabinet for later use.
The fifth step: and (3) taking a piece of the treated p-Si substrate, placing the p-Si substrate under a microscope, taking a hexagonal micron line spin-coated with AuAgNRs by using tweezers, and placing the hexagonal micron line in the part of the p-Si substrate, which is not coated with the Ni/Au electrode by evaporation, so as to ensure the p-Si substrate to be in full contact. And pressing a piece of processed ITO on the micron line of the composite structure to ensure good contact between the micron line and the ITO and between the micron line and the p-Si substrate, so as to construct the silicon-based red light emission enhanced heterojunction diode.
And a sixth step: and repeating the first, second, fourth and fifth steps to prepare an n-ZnO: Ga/p-Si heterojunction light-emitting diode without spin coating AuAgNRs as a control group, and comparing the n-ZnO: Ga/p-Si heterojunction light-emitting diode with the AuAgNRs @ n-ZnO: Ga/p-Si heterojunction light-emitting diode prepared in the fifth step.
The seventh step: and measuring the rectification properties of the heterojunction light-emitting diodes prepared in the fifth step and the sixth step, shooting a luminescence video, measuring a luminescence spectrum, and comparing the luminescence photo with the luminescence spectrum, as shown in fig. 2, 3 and 4. With the increase of the injection current, the luminous intensity of the two heterojunction diodes is improved, but the luminous intensity of the AuAgNRs @ n-ZnO: Ga/p-Si heterojunction light-emitting diode of the spin-coated AuAgNRs is obviously stronger than that of a control group.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (4)
1. A preparation method of a silicon-based red light emission enhanced heterojunction diode comprises a p-Si substrate, a Ni/Au electrode evaporated on the p-Si substrate, n-ZnO Ga microwire fixed on the p-Si substrate, and conductive glass covering the n-ZnO Ga microwire; the surface of the n-ZnO Ga micron line is coated with gold-silver alloy nanorods in a spin mode, and the method is characterized by comprising the following steps:
step 1: annealing the p-Si substrate, cleaning the p-Si substrate, and keeping the p-Si substrate flat and clean;
step 2: plating Ni/Au electrodes on the cleaned p-Si substrate;
and step 3: spin coating prepared gold-silver alloy nano rods on an n-ZnO-Ga micron line;
and 4, step 4: cleaning the ITO, and keeping the ITO flat and clean;
and 5: and (3) placing the AuAgNRs @ n-ZnO and Ga composite structure micrometer line obtained in the step (3) on the p-Si substrate obtained in the step (2), and covering the ITO cleaned in the step (4) on the AuAgNRs @ n-ZnO and Ga composite structure micrometer line to construct the silicon-based red light emission enhanced heterojunction diode.
2. The method of claim 1, wherein the p-Si substrate has a thickness of 365-385 μm, a resistivity of 0.001-0.005 Ω -cm, and a crystal orientation of <100> orientation.
3. The method for preparing a silicon-based red light emission enhanced heterojunction diode according to claim 1, wherein the thickness of the Ni/Au electrode is 20-40 nm.
4. The method of claim 1, wherein the electron concentration of the n-ZnO Ga micron line is 1017～1019/cm3Electron mobility of 5-100 cm2/V·s。
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105280761A (en) * | 2014-07-11 | 2016-01-27 | 三星电子株式会社 | Semiconductor light emitting device and manufacturing method thereof |
| CN110137315A (en) * | 2019-04-25 | 2019-08-16 | 南京航空航天大学 | Single ZnO:Ga micro wire hetero-junctions substantial point source device and preparation method |
| CN110828620A (en) * | 2019-10-16 | 2020-02-21 | 南京航空航天大学 | Single ZnO micron line heterojunction-based near-infrared light-emitting diode and preparation method thereof |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105280761A (en) * | 2014-07-11 | 2016-01-27 | 三星电子株式会社 | Semiconductor light emitting device and manufacturing method thereof |
| CN110137315A (en) * | 2019-04-25 | 2019-08-16 | 南京航空航天大学 | Single ZnO:Ga micro wire hetero-junctions substantial point source device and preparation method |
| CN110828620A (en) * | 2019-10-16 | 2020-02-21 | 南京航空航天大学 | Single ZnO micron line heterojunction-based near-infrared light-emitting diode and preparation method thereof |
Non-Patent Citations (1)
| Title |
|---|
| 《Optoelectronic properties of p-n and p-i-n heterojunction devices prepared by electrodeposition of n-ZnO on p-Si》;A.E.Rakhshani;《JOURNAL OF APPLIED PHYSICS》;20101103;第108卷(第2010期);第2-5页、图2，10 * |
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