CN106898543A - Al2O3The method and device of thin film passivation silica-based nanowire - Google Patents
Al2O3The method and device of thin film passivation silica-based nanowire Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02518—Deposited layers
- H01L21/02587—Structure
- H01L21/0259—Microstructure
- H01L21/02603—Nanowires
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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
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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 discloses one kind and utilizes Al2O3The method of thin film passivation silica-based nanowire, one layer of Al is formed on silicon nanowire structure surface2O3Film is coating silica-based nanowire, Al2O3Film layer is used to be passivated nanowire surface defect, and in the range of carrier of its thickness control in silicon substrate can be penetrated, nanowire surface forms Al2O3Still there is the structure of approximate original pattern after film layer, ald can be used, sputtered or waited chemical vapor deposition techniques to sputter Al on silica-based nanowire surface2O3Film layer.Also disclose with Al2O3The device of the nano thread structure of passivation layer.By this Al2O3The method of thin film passivation surface defect state can further boost device luminous efficiency and performance.
Description
Technical field
The invention belongs to field of photoelectric devices, and in particular to using alundum (Al2O3) (Al2O3) thin film passivation nano wire (NW)
The surface defect state of structure is improving the method and device with the structure of device performance.
Background technology
Effective silicon substrate light source is to realize one of silicon based opto-electronicses interconnection problem demanding prompt solution.Traditional silicon is used as one kind
Indirect bandgap material cannot realize effective electroluminescent.Because silicon quantum dot has quantum limitation effect, compared to
Body silicon materials show more preferable luminescent properties, are one of study hotspots of silicon base luminous material in recent years, also serve as solving silicon
One of candidate material of the luminous problem of base.
Found in the research of the silicon quantum dot characteristics of luminescence, the quantum dot light emitting electrical part of introducing has good property
Can, such as excellent sunken luminous effect, faster speed of photoresponse.Therefore, can be introduced by metal ion Assisted Chemical Etching Process can
Reflection of the light in silicon-Air Interface is effectively reduced, so as to improve light extraction efficiency so that silicon quantum dot luminescence enhancement.But at present
Its luminous efficiency and traditional direct band-gap semicondictor material, such as GaAs, indium phosphide, still have necessarily compared to its luminous efficiency
Gap.In order to further improve device performance, it is necessary to material processing technique is entered with device structure design on the basis of existing
Traveling one-step optimization, also many problems associated are worth exploring.
Surface passivation processing technology is a kind of more ripe technique of semiconductor industry development.Passivation technology is prevented from table
Face is polluted, while the more active dangling bonds of passivated surface, improve the reliability and stability of device.In order to adapt to different devices
Part property and use need, and conventional surface passivation material has silica, silicon nitride, Pyrex, phosphorosilicate glass etc..Al2O3
Film has stronger capability of resistance to radiation and anti-sodium ion ability, firmly as a kind of surface passivation material compared to other materials
Degree is big, and good toughness, the protective value to device is preferable.Therefore, Al2O3Film is considered to have raising silica-based nanowire photophore
The potentiality of part performance.
We are prepared for the silicon nanowire array of different length by metal ion Assisted Chemical Etching Process on a silicon substrate, so
One layer of Al grown by technique for atomic layer deposition afterwards2O3Film is with passivated surface defect state.Growth on this basis is prepared for tool
Some silicon quantum dot electroluminescent devices.We have found that deposited Al2O3The luminescent properties of sample are improved after film,
Electroluminescent (EL) intensity is strengthened.This explanation Al2O3There is film obvious passivation to make to surface of silicon nanowires defect state
With it has good application prospect in the silicon base luminescence field of silicon base luminescence, particularly low dimensional structures.
The content of the invention
To solve the above problems, the present invention discloses one kind and utilizes Al2O3The method of thin film passivation silica-based nanowire and have
Al2O3The device of passivation layer, on the basis of, by one layer of Al of upper growth2O3Film is being passivated the defect of nanowire surface
State, further carries device performance, improves the luminous efficiency of device.
The utilization Al of disclosure of the invention2O3The method of thin film passivation silica-based nanowire, is included in nano thread structure surface shape
Into one layer of Al2O3Film is coating silica-based nanowire, Al2O3Film layer is used to be passivated nanowire surface defect, and its thickness control exists
In the range of carrier in silicon substrate can be penetrated.
Further, nanowire surface forms Al2O3There is the structure of approximate original pattern after film layer.
Further, using technique for atomic layer deposition in silica-based nanowire surface depositing Al2O3Film layer.
Further, using sputter or wait chemical vapor deposition techniques silica-based nanowire surface sputter Al2O3Film layer.
Further, Al2O3The thickness control of film layer is in 2~8nm.
Further, the length of nano wire is 200~450nm.
Further, N-shaped/p-type flat board silicon substrate can also be carved using metal ion Assisted Chemical Etching Process technology
Lose to form silicon nanowire array；Then silicon nanowire array surface after cleaning forms one layer of Al2O3Film is received with coated Si
Rice noodles；Again in surface depositing Al2O3The silicon nanowire array of film sequentially forms intrinsic layer and p-type/n-layer, so as to form n-
I-p/p-i-n device architectures.
Further, may also include after carrying out Dehydroepiandrosterone derivative in nitrogen atmosphere to formation n-i-p devices, then carry out heat and move back
Fire, to form silicon quantum dot, while activating dopant atoms.
Further, may also include respectively with Al2O3The positive back side of the silicon quantum dot device of passivation layer forms metal
Electrode simultaneously carries out Alloying Treatment.
There is Al invention additionally discloses one kind2O3The device of the silicon-based nano cable architecture of passivation layer, including with nanowire-junction
The silicon substrate of structure and the Al positioned at nanowire surface2O3Film layer, Al2O3Carrier of the thickness control of film layer in silicon substrate
In the range of can penetrating.
Further, nanowire surface forms Al2O3Still have after film layer and be similar to original pattern.
Further, the Al on surface2O3Film layer is using technique for atomic layer deposition, sputters or wait chemical vapor deposition skill
Art is formed.
Further, the length of nano wire is 200~450nm, the Al2O3The thickness control of film layer is in 2~8nm.
On this basis, there is Al invention additionally discloses one kind2O3The silicon quantum dot electricity of the silicon-based nano cable architecture of passivation layer
Electroluminescence device, it include by obtained by the above method with Al2O3The silicon substrate of passivation layer.
With Al2O3The preparation and performance test of the silicon quantum dot electroluminescent device of the silicon substrate of passivation layer, key step bag
Include following two fermentation：
First step：To surface depositing Al2O3The preparation of the silicon nanowire array of film and structural characterization；
N-shaped flat board silicon substrate is performed etching using metal ion Assisted Chemical Etching Process technology.Using silver nitrate and hydrogen fluorine
There is chemical reaction and fall part silicon with selective etch in the mixed solution of acid, form silicon nanowires, reaction in substrate surface and silicon
Equation is as follows：
4Ag+(aq)+Si0(s)+6F-(aq)→4Ag(s)+SiF6 2-(aq)
In course of reaction, by the length for controlling etch period to regulate and control nano wire.After the completion of reaction, sample is soaked in
Removing surface impurity in dust technology, then with deionized water rinsing and dry to form the silicon nanowire array of cleaning.
One layer of Al is deposited on silicon nanowire array by technique for atomic layer deposition afterwards2O3Film.Technique for atomic layer deposition
Be by monatomic film layer by layer deposition, therefore deposition Al2O3Uniformity of film is fabulous, and thickness can be controlled in several nanometers
Range scale in.So as to obtain surface depositing Al2O3The silicon of film.
Sample surfaces dangling bonds are characterized by electron spin resonance (ESR) technology, is compared without surface passivation
Treatment and Al2O3The ESR signal intensities of the nano wire sample of passivation, find Al2O3The ESR signals of sample are in g=after passivation
Weaken at 2.005, show Al2O3Nanowire surface defect state can be effectively passivated.
Second step：Silicon quantum dot El element preparation with test.
Nano-wire array is placed in PECVD system, silane (SiH is passed through4) with deposited amorphous silicon (a-Si) layer, then be passed through
Oxygen (O2) in-situ oxidation formation silica (SiO2) layer.So alternately forming a-Si/SiO2Periodicity film knot
Structure, is passed through SiH again afterwards4And borine (the B with 1% dilution proportion in hydrogen2H6) forming the p-type silicon of top layer.
After growth is finished, sample is placed in nitrogen atmosphere and successively carry out dehydrogenation with thermal anneal process to form quantum dot knot
Structure has simultaneously carried out PL tests to sample.
During sample successively then is placed in into thermal evaporation system and magnetic control sputtering system, in bottom and top difference plated aluminum
Electrode and tin indium oxide (ITO) electrode simultaneously carry out Alloying Treatment.
EL tests and current-voltage (I-V) test have been carried out to sample after forming device architecture.We have found that Al2O3Passivation
The PL intensity and EL intensity of sample are all remarkably reinforced afterwards, and I-V tests show Al2O3The rectification characteristic of sample improves after passivation,
Injected current density becomes big under identical bias, it was demonstrated that Al2O3Passivation can significantly improve the luminescent properties of device.
The present invention in silicon-based nano cable architecture by growing one layer of Al2O3Film to be passivated the defect state of nanowire surface,
Have the advantages that：
(1) by Al2O3Surface passivation technique significantly improves the performance of the device having, the silicon quantum especially having
Point electroluminescent device, while Al2O3Film serves protective effect to device again to the cladding of device, being capable of preferably anti-spoke
Penetrate, antipollution, so as to improve the service life of device.This silicon base luminescence to studying silicon base luminescence, particularly low dimensional structures, it is right
Finally realize that effective silicon substrate light source all has highly important directive significance.
(2) device fabrication process is relatively easy.Metal ion Assisted Chemical Etching Process technology be applied to large-scale production, wait from
Daughter enhancing chemical vapour deposition technique, technique for atomic layer deposition, the development of high annealing technology are more ripe.
(3) parameters of device can Effective Regulation.For example, can be by controlling etch period Effective Regulation nanometer
Line length, can be by controlling sedimentation time Effective Regulation silicon quantum dot size and Al2O3Film thickness.
(4) additionally, using Al2O3The method of thin film passivation nano thread structure is applicable not only to electroluminescent device, can be with
Suitable for the solar cell with nano thread structure, its short circuit current and open-circuit voltage are improved, so as to lift its conversion efficiency.
Brief description of the drawings
Fig. 1：Silicon quantum dot EL device structure schematic diagram.
Fig. 2：Silicon quantum dot electroluminescent device reflectance spectrum.
Fig. 3：The electron spin resonance spectroscopy of silicon nanowires.
Fig. 4：Silicon quantum dot electroluminescent device I-V characteristic curve.
Fig. 5：Silicon quantum dot device luminescence generated by light (PL) spectrum.
Fig. 6：Silicon quantum dot device electroluminescent (EL) spectrum.
Specific embodiment
As shown in figure 1, disclosing the structure chart of the silicon quantum dot electroluminescent device having in embodiment, the structure includes
N-type silicon substrate (n-Si) with silicon, the Al on cladding nano-wire array surface2O3Film layer, the intrinsic layer with silicon quantum dot
Tin indium oxide (ITO) electrode that (Si Q.D.MLs), p-type silicon layer and metallization are formed, i.e., a kind of silicon quantum dot n- having
I-p luminescent devices.Wherein, Al2O3In the range of carrier of the thickness control of film layer in silicon substrate can be penetrated, and nanometer
Line surface forms Al2O3Still there is the structure for being similar to original pattern after film layer.
A kind of preparation method of silicon quantum dot electroluminescent device is also disclosed in embodiment, is comprised the following steps：
S1, prepare silicon nanowire array
N-type silicon chip (the Ω cm of resistivity 1.7~3.2) first to 1cm × 1cm carries out RCA standard cleanings, utilizes afterwards
Metal ion Assisted Chemical Etching Process method is performed etching to silicon chip, and etching solution used is according to the AgNO of 0.2mol/L3Solution:Hydrogen
Fluoric acid:Deionized water=1:2.5:The mixed solution of 6.5 proportions, etch period is chosen 3 minutes, 5 minutes, 8 points respectively
Clock, the different nanowire length of correspondence is respectively 200nm, 310nm, 450nm.Reaction equation is：
4Ag+(aq)+Si0(s)+6F-(aq)→4Ag(s)+SiF6 2-(aq)
After etching is finished, silicon chip is placed in dilute nitric acid solution 20 minutes to remove the Ag on surface, then floated with deionized water
Wash 5 times foreign ions to remove surface.The silicon nanowire array of cleaning is obtained after being dried.
S2, in silicon nanowire array surface depositing Al2O3Film
Obtained silicon nanowire array is placed in the atomic layer deposition system of Oxford companies production and grows a layer thickness
It is the Al of 6nm2O3Film is coating silicon nanowires.
Due to technique for atomic layer deposition be by monatomic film layer by layer deposition, therefore deposition Al2O3Uniformity of film pole
Get well, and thickness can be controlled in several nanometers of range scale.
Certainly, in addition to atomic deposition technique (ALD), can also be by skills such as existing sputtering or chemical vapor depositions (CVD)
Art forms Al2O3Film layer, such as using the sputtering equipment sputtering Al of Applied Materials2O3Film, using Centrotherm's
PECVD depositing Als2O3Film.Wherein, cause that atom or molecule depart from target under sputtering usually high-energy, and sunk on substrate
The technique that product forms film.It is that formed uniformity of film is fabulous with CVD advantages relative to sputtering, thickness can be controlled
In several nanometer ranges.Preferred ALD schemes in embodiment, and the supplement with CVD as our technological means will be sputtered.
It is worth noting that, Al in the prior art2O3Film layer is generally used for being passivated Si, SiO2、SiNxDeng surface, therefore
Also by often referred to as Al2O3Passivation layer, its thickness typically affects only the effect of surface passivation；And Al in the present invention2O3Film layer
Thickness need simultaneously meet three conditions：
First, Al2O3The thickness of film layer can not be too thin, to be enough to be passivated the more active suspension in nano-wire array surface
Key, reduces interface state defects, so as to reduce surface recombination, improves the reliability and stability of device；
Secondly, Al2O3Film layer can not be blocked up, blocked up to hinder penetrating for minority carrier, therefore its thickness must be able to protect
Card minority carrier passes through Al2O3Layer simultaneously reaches silicon quantum dot layer.
Again, Al2O3The thickness of film layer will preferably control to coat silicon nanowires, and keep nanometer linear array as much as possible
Original pattern is arranged, to prevent the preferable optical property of nano-wire array to be destroyed, such as reflection preventing ability.
Empirical tests, Al2O3The thickness control of film layer can simultaneously meet above-mentioned condition in 2~8nm, ensure that son is worn less
Thoroughly and on the premise of holding surface pattern, energy preferably passivated surface defect, so as to improve the luminous efficiency of device.
S3, prepare n-i-p device architectures
Nano-wire array is placed in PECVD system to grow Si/SiO2Periodicity film, its process is as follows：
First it is passed through the SiH that flow is 5sccm4To deposit a-Si layers, the time is 20 seconds；The O that flow is 20sccm is passed through again2
In-situ oxidation is carried out to form SiO2Layer, the time is 90 seconds.So alternately a-Si/SiO2Layer growth, grew altogether for 9 week
Phase.
The last SiH for being passed through 5sccm again4And the B with 1% dilution proportion in hydrogen of 50sccm2H6, to form top
The p-type silicon of layer, material is thus formed n-i-p device architectures.
S4, formation silicon quantum dot
Si/SiO is grown in PECVD2After periodic multilayer film and top layer p-type silicon, in order in i layers of (i.e. Si/SiO2
Layer) silicon quantum dot is formed, while activating dopant atoms, we have successively carried out 450 DEG C of Dehydroepiandrosterone derivatives in nitrogen atmosphere to sample
One hour and 1000 DEG C of thermal annealings one hour.
S5, prepare metal electrode
Afterwards, respectively by thermal evaporation system and magnetic control sputtering system the bottom and top of sample plate aluminium electrode and
ITO electrode, and 450 DEG C of alloyings are carried out 30 minutes to form good Ohmic contact.
So, with Al2O3The silicon quantum dot electroluminescent device of passivation layer is just prepared and completed.
In manufacturing process, to silicon quantum dot electroluminescent device characterize.
It should be noted that the present embodiment is by taking n-i-p devices as an example, specifically a kind of silicon quantum dot electroluminescent cell
Part, but, similarly the present invention can also be implemented to p-i-n, p-n, n-p device, and also be not limited only to quantum dot device, can also be fitted
There is the luminescent device of nano thread structure for other.
As shown in Fig. 2 measuring the reflectance spectrum of sample by Shimadzu UV-3600 spectrometers.We have found that in Al2O3It is blunt
The reflectance spectrum of sample is having substantially reduction compared with long-wave band (＞ 1100nm) after change, illustrates Al2O3Film has more preferably compared with long-wave band
Anti-reflective effect, this is conducive to the lifting of device performance.
As shown in figure 3, by electron spin resonance (ESR) technology to Al2O3The surface dangling bonds of the nano wire sample of passivation
Characterize, spinning electron resonance (ESR) test of sample shows, compared to the sample not being passivated, Al2O3The ESR letters of sample after passivation
Substantially weaken number at g=2.005, this explanation Al2O3Film has effectively been passivated surface of silicon nanowires defect state really.
As shown in figure 4, I-V (current-voltage) tests show, Al2O3The rectification characteristic of sample is obviously improved after passivation, blunt
The commutating ratio of sample differs nearly 4 orders of magnitude after change.Under identical bias, Al2O3The injected current density of sample has been after passivation
Increase.
As shown in figure 5, PL tests show in Al2O3Silicon quantum dot luminescent properties are improved after passivation.Wherein, etch period choosing
Take 3 minutes, 5 minutes, the luminescent properties increase rate corresponding to the sample corresponding to 8 minutes rose successively, especially etch 8 points
Clock, improves clearly.
By the result of contrast experiment, it has been found that etch period 8 minutes (correspondence nanowire length about 450nm), Al2O3
Thickness has best luminescent properties for the quantum dot device of 6nm.And the sample Al2O3 passivation effect slightly shorter for etch period
Without 8 minutes obvious of etching.Because the slightly shorter sample defects state of etch period is less, Al2O3 passivation effects were without 8 minutes
Substantially.Therefore the sample tests that etch period is 8 minutes are only gived in Fig. 6.
As shown in fig. 6, the EL tests of the silicon quantum dot device for passing through show, Injection Current IinAfter=100mA, for etching
Time is 8 minutes samples of (correspondence nanowire length about 450nm), in Al2O3(Al2O3 thickness is 6nm), EL intensity after passivation
All it is significantly improved in whole test wave band, luminous intensity a maximum of about of enhances 7 times.Because etch period is more long, surface defect
State is more, Al2O3Passivation effect is more obvious, therefore etch period is the best sample luminescence enhancement effect of 8 minutes.This is further
Illustrate Al2O3Thin film passivation technology can effectively be passivated surface of silicon nanowires defect state, injected current density be improved, so that substantially
Improve device performance.
What deserves to be explained is, although only having enumerated the embodiment of the silicon quantum dot electroluminescent device having in embodiment,
But this utilization Al2O3The method of thin film passivation nano thread structure is applicable not only to electroluminescent device, can be applicable to have
The solar cell of nano thread structure, either common p-type battery, SE batteries or efficient PERC batteries etc., pass through
Al2O3Surface passivation reduces surface defect state, its short circuit current and open-circuit voltage is improved, so as to lift the conversion of solar cell
Efficiency.
The preferred embodiments of the present invention are the foregoing is only, is not intended to limit the invention, for the skill of this area
For art personnel, the present invention can have various modifications and variations.It is all within the spirit and principles in the present invention, made any repair
Change, equivalent, improvement etc., should be included within the scope of the present invention.
Claims (10)
1. a kind of Al2O3The method of thin film passivation silica-based nanowire, it is characterised in that form one in silica-based nanowire body structure surface
Layer Al2O3Film is coating silica-based nanowire, Al2O3Film layer is used to be passivated nanowire surface defect, and its thickness control is in silicon substrate
In carrier can penetrate in the range of.
2. the method for claim 1, it is characterised in that nanowire surface forms Al2O3Still have after film layer approximate former
There is the structure of pattern.
3. the method for claim 1, it is characterised in that deposited on silica-based nanowire surface using technique for atomic layer deposition
Al2O3Film layer.
4. the method for claim 1, it is characterised in that using sputtering or wait chemical vapor deposition techniques in silicon-based nano
Line surface sputters Al2O3Film layer.
5. the method for claim 1, it is characterised in that the length of the nano wire is 200~450nm.
6. the method for claim 1, it is characterised in that the Al2O3The thickness control of film layer is in 2~8nm.
7. it is a kind of that there is Al2O3The device of the silicon-based nano cable architecture of passivation layer, it is characterised in that including with nano thread structure
Silicon substrate and the Al positioned at nano thread structure surface2O3Film layer, Al2O3Current-carrying of the thickness control of film layer in silicon substrate
In the range of son can be penetrated.
8. device as claimed in claim 7, it is characterised in that nanowire surface forms Al2O3Have after film layer approximate original
The structure of pattern.
9. device as claimed in claim 7, it is characterised in that the Al on surface2O3Film layer be using technique for atomic layer deposition,
Sputter or wait chemical vapor deposition techniques to be formed.
10. device as claimed in claim 7, it is characterised in that the length of the nano wire is 200~450nm, the Al2O3
The thickness control of film layer is in 2~8nm.
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| CN113206181A (en) * | 2021-05-06 | 2021-08-03 | 南京大学 | Radial junction silicon quantum dot electroluminescent device and preparation method thereof |
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