CN102199759B - Gradient hydrogen process grown ZnO-TCO thin film with textured structure and use thereof - Google Patents
Gradient hydrogen process grown ZnO-TCO thin film with textured structure and use thereof Download PDFInfo
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- CN102199759B CN102199759B CN2011101327604A CN201110132760A CN102199759B CN 102199759 B CN102199759 B CN 102199759B CN 2011101327604 A CN2011101327604 A CN 2011101327604A CN 201110132760 A CN201110132760 A CN 201110132760A CN 102199759 B CN102199759 B CN 102199759B
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Abstract
The invention discloses a gradient hydrogen process grown ZnO-TCO thin film with a textured structure, which is prepared by using a glass substrate as a substrate, ZnO:Ga2O3 or ZnO:Al2O3 as a target material and Ar as a sputtering gas, introducing hydrogen in a sputtering process and varying the flow of the hydrogen in a gradient manner in a sputtering coating period and by a magneto-controlled sputter coating technique. The gradient hydrogen process grown ZnO-TCO thin film has the advantages that: compared with ZnO-TCO thin film with the textured structure, which is obtained by using the magneto-controlled sputter coating technique with normal hydrogen flow, the ZnO-TCO thin film with the textured structure, which is grown gradient hydrogen flow process, has higher transmissivity and better electrochemical property, and the textured structure of the thin film is improved obviously; and when the thin film is used in a microcrystalline silicon thin film cell or noncrystalline silicon cell/microcrystalline silicon tandem thin film solar cell, the light scattering effect is improved, the incident light path is increased, the thickness of an active layer is lowered effectively, and the efficiency and stability of a Si-based thin-film solar cell are improved.
Description
[technical field]
The invention belongs to the thin film solar cell field, particularly a kind of gradient hydrogen method growth matte structure ZnO-TCO film and application.
[background technology]
Transparent conductive oxide (transparent conductive oxide-TCO) thin-film material is the important component part of thin film solar cell; Referring to document: A.V.Shah, H.Schade, M.Vanecek; Et al.Progress in Photovoltaics 12 (2004) 113-142, J.M ü ller; B.Rech, J.Springer, et al.Solar Energy77 (2004) 917-930.Using the most widely in the current hull cell, the TCO film is F doping SnO
2Film (SnO
2: F) with Sn doping In
2O
3Film (In
2O
3: Sn).F doping SnO
2Film normally utilizes the preparation of atmospheric pressure cvd (APCVD) technology; Growth temperature higher (～500 ℃), this will limit its further application for the battery material of growing in low temperature depositing and the strong H plasma environment; Referring to document: S.Major; S.Kumar, M.Bhatnagar, et al.Applied Physics Letters 49 (1986) 394-396.Sn doping In
2O
3Film is because the cost of In is higher, and is not easy to obtain coarse surface topography, and performance worsens easily in strong H plasma environment, has also limited its widespread use in thin film solar cell.Than other TCO thin-film materials, it is abundant that ZnO film has source material, nontoxic and the allometry temperature is low (room temperature-300 ℃) and in strong H plasma environment characteristics such as stable performance obtained broad research and application.
Intrinsic ZnO film resistivity is higher, adopts the doping impurity method to improve its electric property usually, and main alloying element has B, Al, Ga, In and F etc.Be applied to TCO film in the silicon-film solar-cell except excellent photoelectric performance, suitable suede structure (being rough textured surface) is used for the sunken light of thin film solar cell has importance.Grain-size has good scattering process to the light of comparable wavelength.Research shows that the application of suede structure TCO film can improve the scattering of light effect, increases the incident light path; It plays decisive influence for the efficient and the stability (SW effect) that improve the Si base thin film solar battery effectively to reduce active layer thickness (being intrinsic layer i-layer); Referring to document: J.M ü ller, B.Rech, J.Springer; Etal.TCO and light trapping in silicon thin film solar cells, Solar Energy 77 (2004) 917-930.The grain-size of the main and film of suede structure, factors such as grain shape and roughness are relevant.
Van de Walle etc.; Referring to document: Chris G.Van de Walle.Hydrogen as a Cause of Doping in Zinc Oxide; Physical Review Letters 85 (2000) 1012-1015; First principle calculating based on density functional theory shows that H can be used as shallow donor's effect, H in the ZnO material
+Be to be in the most stable and lowest energy state in the fermi level position.Afterwards; Hization ZnO film growth and characteristic have obtained broad research, and Liang-Yih Chen etc. are referring to document: Liang-Yih Chen; Wen-Hwa Chen; Jia-Jun Wang, et al.Hydrogen-doped high conductivity ZnO films deposited by radio-frequency magnetron sputtering, Applied Physics Letters 85 (2004) 5628-5630; Utilize radiofrequency magnetron sputtering technology to study the photoelectric characteristic of H doping ZnO-TCO film, lowest resistivity～2 * 10
-4Ω cm, electronic mobility reaches～40cm
2/ Vs, carrier concentration reaches～and 6 * 10
20/ cm
-3Feed an amount of H in the Ar gas sputter atmosphere
2Gas can effectively reduce the resistivity of film; And along with H
2The increase of flow, (002) interplanar distance increases, and carrier concentration increases in the film, and this phenomenon is attributable to H shallow donor effect in the ZnO film; In addition, H
2The increase visible-range transmitance of flow increases.The follow-up H of ZnO film handles also has material impact to film performance, and Baik etc. are referring to document: S.J.Baik; J.H.Jang; C.H.Lee,, et al.Highly textured and conductive undoped ZnO film using hydrogen post-treatment; Applied Physics Letters 70 (1997) 3516-3518 have studied H
2Anneal and ultraviolet lighting are to the ZnO film Effect on Performance, and experiment finds that film resiativity is from～1 * 10
-2Ω cm drops to～and 2 * 10
-3Ω cm; Kohiki etc.; Referring to document: Shigemi Kohiki; Mikihiko Nishitani; Takahiro Wada, et al.Enhanced conductivity of zinc oxide thin films by ion implantation of hydrogen atoms, Applied Physics Letters 64 (1994) 2876-2878.After experiment showed that the ZnO film intermediate ion injects H, film resiativity was from～1 * 10
7Ω cm drops to～and 1.8 * 10
-3Ω cm.
Over the past two years, Hization doped ZnO-TCO growth for Thin Film and characteristic research caused the concern of researcher.S.J.Tark etc.; Referring to document: S.J.Tark; Y.W.Ok, M.G.Kang, et al.Effect of a hydrogen ratio in electrical and optical properties of hydrogenated Al-doped ZnO films; Journal of Electroceram23 (2009) 548-553 utilizes radiofrequency magnetron sputtering technology to study the microtexture and the photoelectric properties of Hization Al doping ZnO-TCO film.Experiment shows, than the ZnO:Al film of direct growth, suitable H
2/ Ar throughput ratio (R=2%) helps to improve the electric property of film, and resistivity reaches～and 4.98 * 10
-4Ω cm.Yet, along with H
2/ Ar throughput ratio increases, and film resiativity increases, and electronic mobility descends, and simultaneously, the film grain-size reduces, and the film stress increases.In addition; This study group utilizes wet etching technique to prepare suede structure Hization Al doping ZnO-TCO film, and is applied to μ c-Si hull cell and has obtained 7.78% efficient, referring to document: Sung Ju Tark; Min Gu Kang; Sungeun Park, et al.Development of surface-textured hydrogenated ZnO:Al thin-films for μ c-Si solar cells, Current Applied Physics 9 (2009) 1318-1322.Young Ran Park etc.; Referring to document: Young Ran Park; Juho Kim and Young Sung Kim.Growth and characteristics of hydrogenated In-doped ZnO thin films by pulsed DC magnetron sputtering, Applied Surface Science 256 (2009) 1589-1594 utilize the pulse direct current magnetron sputtering technique Hization Al doping ZnO-TCO film of having grown; Wherein underlayer temperature is 500 ℃; Experimental result shows that the introducing of H is less relatively to the electric property influence, and bigger variation takes place the surface topography of film.W.F.Liu etc., referring to document: W.F.Liu, G.T.Du, Y.F.Sun, et al.Effects of hydrogen flux on the properties of Al-doped ZnO films sputtered in Ar+H
2Ambient at low temperature; Applied Surface Science253 (2007) 2999-3003, Weifeng Liu; Guotong Du; Yanfeng Sun, et al.Al-doped ZnO thin films deposited by reactive frequency magnetron sputtermg:H
2-induced property changes, Thin Solid Films 515 (2007) 3057-3060 utilize radiofrequency magnetron sputtering technology to study the microtexture and the photoelectric properties of Hization Al doping ZnO-TCO film.In sputtering atmosphere, feed H
2When airshed is 1.0sccm, obtain lower film resiativity～4.15 * 10
-4Ω cm is along with H
2Flow is increased to the 1.6sccm process from 0sccm, and ZnO film (002) peak diffraction intensity is dull to be reduced.
In sum, the investigator thinks that H plays shallow donor's effect in the ZnO film material, can effectively improve the electricity and the optical property of film; Magnetron sputtering technique growing high-quality ZnO-TCO film and characteristic research thereof are the hot subjects of current scientific effort, and suitable coarse suede structure can strengthen the scattering of light effect of ZnO film effectively.
In addition, in the magnetron sputtering membrane process, introduce H both at home and abroad
2Mainly be constant rate, the ZnO film of growth still needs further to improve film performance.In film growth techniques, guarantee the material photoelectric properties and have the important topic that good suede structure is research.The present invention utilizes magnetron sputtering technique, ZnO:Ga
2O
3Perhaps ZnO:Al
2O
3Ceramic target is as starting material, and Ar gas is introduced H in the sputter procedure simultaneously as sputter gas
2Gas proposes in the experimentation through modulation gradient H
2Gas flowrate method is led Ga or Al doping matte structure ZnO-TCO film with high permeability thereby prepare high electricity.Above-mentioned technical characterictic is different from the method that current other magnetron sputterings obtain ZnO film.
[summary of the invention]
The objective of the invention is to above-mentioned technical Analysis; A kind of gradient hydrogen method growth matte structure ZnO-TCO film is provided; Solve conventional sputtering technology growing ZnO thin-film optics and electric property is poor, the high shortcoming of underlayer temperature, obtain the ZnO-TCO film of high permeability, low-resistivity, suede structure.This matte structure ZnO-TCO film is applied to thin film solar cell, can improve the scattering of light effect, increases the incident light path, effectively reduces active layer thickness, improves the efficient and the stability of Si base thin film solar battery.
Technical scheme of the present invention:
A kind of gradient hydrogen method growth matte structure ZnO-TCO film is a substrate with the glass substrate, is 99.995% ZnO:Ga with purity
2O
3Or ZnO:Al
2O
3Ceramic target is as the target raw material, and sputter gas is an Ar gas, introduce in the sputter procedure hydrogen and sputter coating in the cycle hydrogen flowing quantity change in gradient, utilize magnetron sputtering technology to prepare matte structure ZnO-TCO film.
Said sputter coating in the cycle hydrogen flowing quantity change in gradient and comprise preliminary stage and later stage, the hydrogen flowing quantity of preliminary stage is for to be 1.0-5.0sccm than low discharge, the plated film cycle times of preliminary stage accounts for the 25%-50% of total plated film cycle times; The hydrogen flowing quantity of later stage is that normal discharge is 5.0-10.0sccm, and the plated film cycle times of later stage accounts for the 75%-50% of total plated film cycle times.
Said ZnO:Ga
2O
3Or ZnO:Al
2O
3Target component Ga in the ceramic target
2O
3And Al
2O
3Weight percent be 0.5-2.0%.
Said matte structure ZnO-TCO film thickness is 700-2500nm, and the suede structure roughness RMS value is 30-150nm.
Said glass substrate temperature is a room temperature-350 ℃.
The sputtering pressure of said sputter gas Ar gas is 2.0-6.0mTorr.
Said sputtering power density is 0.2-2.0W/cm
2
The flow of introducing hydrogen in the said sputter procedure is 0sccm to 20sccm.
A kind of application of said gradient hydrogen method growth matte structure ZnO-TCO film is applied to amorphous silicon membrane or non-crystalline silicon/microcrystalline silicon solar cell.
Advantage of the present invention and effect: the matte structure ZnO-TCO film that utilizes under the normal hydrogen airshed magnetron sputtering technology to obtain; The present invention utilizes the matte structure ZnO-TCO film of gradient hydrogen flowing quantity method growth to have transmitance preferably; And keep electrology characteristic preferably, the suede structure of film is obtained obvious improvement simultaneously.This ZnO-TCO film is applied to microcrystalline silicon film battery or amorphous silicon/microcrystalline silicon tandem thin film solar cell, can improve the scattering of light effect, increases the incident light path, effectively reduces active layer thickness, improves the efficient and the stability of Si base thin film solar battery.
[description of drawings]
The matte structure ZnO film structural representation of Fig. 1 for obtaining under the magnetron sputtering technique normal hydrogen airshed situation.
Fig. 2 this matte structure ZnO film structural representation for obtaining under the magnetron sputtering technique gradient hydrogen flowing quantity situation.
This matte structure ZnO film that Fig. 3 obtains for gradient hydrogen flowing quantity method is applied to the structural representation of pin type a-Si:H thin film solar cell.
This matte structure ZnO film that Fig. 4 obtains for gradient hydrogen flowing quantity method is applied to the structural representation of pin type a-Si:H/ μ c-Si:H laminated film solar battery.
[embodiment]
Embodiment 1:
1, utilizing magnetron sputtering technique, is 99.995% ZnO:Ga with purity
2O
3Ceramic target is as the target raw material, dopant component Ga in the ceramic target
2O
3Weight percent be 1.0%, sputter gas is an Ar gas, the matte structure ZnO of on glass substrate, growing-TCO film, underlayer temperature are 125 ℃, background vacuum pressure is 8 * 10
-5Pa, sputtering pressure are 4.3mTorr, and sputtering power density is 1.0W/cm
2, film thickness is 1200nm.This membrane structure is: the Ga doping ZnO-TCO film of glass/graded hydrogen flowing quantity for growing under " low hydrogen flowing quantity+normal hydrogen airshed " condition; Amounting to coating times is 20 cycles; Wherein low hydrogen flowing quantity 2sccm is 5 cycles, and normal hydrogen airshed 6.0sccm is 15 cycles.
Fig. 2 is this matte structure ZnO film structural representation; Compare with the matte structure ZnO film structure that under normal hydrogen airshed situation, obtains shown in Figure 1; Sputter coating in the cycle hydrogen flowing quantity change the film that makes in gradient and have high-quality suede structure; Be that thickness is less, the suede degree is bigger, and have the high and high electricity of high permeability and lead.
2, this matte structure ZnO film is applied to pin type a-Si/ μ c-Si laminated film solar battery, Fig. 4 is an a-Si/ μ c-Si thin film solar cell battery structure synoptic diagram.Be coated with textured ZnO-TCO film on the glass substrate, grow in succession pin a-Si film and pin μ c-Si film, totally 6 layers of Si film then are coated with the ZnO/Al film, and above-mentioned characteristic constitutes the solar cell device.This matte structure ZnO film make silicon-film solar-cell raise the efficiency and stable aspect improve obviously.
Embodiment 2:
Utilizing magnetron sputtering technique, is 99.995% ZnO:Al with purity
2O
3Ceramic target is as the target raw material, dopant component Al in the ceramic target
2O
3Weight percent be 1.0%, sputter gas is an Ar gas, growth ZnO-TCO film on glass substrate, underlayer temperature is 250 ℃, background vacuum pressure is 8 * 10
-5Pa, sputtering pressure are 4.0mTorr, and sputtering power density is 0.8W/cm
2, film thickness is 1500nm.This membrane structure is: the Al doping matte structure ZnO-TCO film of glass/graded hydrogen flowing quantity for growing under " low hydrogen flowing quantity+normal hydrogen airshed " condition; Amounting to coating times is 20 cycles; Wherein low hydrogen flowing quantity 1sccm is 5 cycles, and normal oxygen flow 4.5sccm is 15 cycles.
2, above-mentioned matte structure ZnO-TCO film is applied to pin type a-Si thin film solar cell.As shown in Figure 3, be coated with this textured ZnO membrane on the glass substrate, the p that grows thereafter, i, three layers of a-Si film of n are coated with the ZnO/Al laminated film at last, and above-mentioned characteristic constitutes the solar cell device.This matte structure ZnO film make thin film solar cell raise the efficiency and stable aspect improve obviously.
Claims (7)
1. gradient hydrogen method growth matte structure ZnO-TCO film, it is characterized in that: being substrate with the glass substrate, is 99.995% ZnO:Ga with purity
2O
3Or ZnO:Al
2O
3Ceramic target is as the target raw material; Sputter gas is an Ar gas; Introduce in the sputter procedure hydrogen and sputter coating in the cycle hydrogen flowing quantity change in gradient, utilize magnetron sputtering technology to prepare matte structure ZnO-TCO film, said sputter coating in the cycle hydrogen flowing quantity change in gradient and comprise preliminary stage and later stage; The hydrogen flowing quantity of preliminary stage is for to be 1.0-5.0sccm than low discharge, and the plated film cycle times of preliminary stage accounts for the 25%-50% of total plated film cycle times; The hydrogen flowing quantity of later stage is that normal discharge is 5.0-10.0sccm, and the plated film cycle times of later stage accounts for the 75%-50% of total plated film cycle times.
2. according to the said gradient hydrogen of claim 1 method growth matte structure ZnO-TCO film, it is characterized in that: said ZnO:Ga
2O
3Or ZnO:Al
2O
3Target component Ga in the ceramic target
2O
3And Al
2O
3Weight percent be 0.5-2.0%.
3. according to the said gradient hydrogen of claim 1 method growth matte structure ZnO-TCO film, it is characterized in that: said matte structure ZnO-TCO film thickness is 700-2500nm, and the suede structure roughness RMS value is 30-150nm.
4. according to the said gradient hydrogen of claim 1 method growth matte structure ZnO-TCO film, it is characterized in that: said glass substrate temperature is a room temperature-350 ℃.
5. according to the said gradient hydrogen of claim 1 method growth matte structure ZnO-TCO film, it is characterized in that: the sputtering pressure of said sputter gas Ar gas is 2.0-6.0mTorr.
6. according to the said gradient hydrogen of claim 1 method growth matte structure ZnO-TCO film, it is characterized in that: said sputtering power density is 0.2-2.0W/cm
2
7. the application of gradient hydrogen method growth matte structure ZnO-TCO film according to claim 1 is characterized in that: be applied to amorphous silicon membrane or non-crystalline silicon/microcrystalline silicon solar cell.
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| CN103137778A (en) * | 2011-11-25 | 2013-06-05 | 吉富新能源科技(上海)有限公司 | High-efficiency double-knot thin film solar cell technique for internal light secondary scattering |
| CN106024932B (en) * | 2016-06-16 | 2017-10-31 | 浙江大学 | Amorphous silicon/microcrystalline silicon tandem solar cell based on nano-pore periodic array |
| US10103282B2 (en) | 2016-09-16 | 2018-10-16 | Nano And Advanced Materials Institute Limited | Direct texture transparent conductive oxide served as electrode or intermediate layer for photovoltaic and display applications |
| CN106784112A (en) * | 2016-12-23 | 2017-05-31 | 中山大学 | A kind of silicon substrate zinc sulfide heterojunction solar cell and preparation method thereof |
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| CN101572279A (en) * | 2009-06-10 | 2009-11-04 | 南开大学 | High mobility textured structure IMO/ZnO composite film grown by sputtering method and application thereof to solar cell |
| CN101985740A (en) * | 2009-07-29 | 2011-03-16 | 中国科学院福建物质结构研究所 | Method for annealing aluminum-doped zinc oxide transparent conductive thin film |
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| JP2010241638A (en) * | 2009-04-06 | 2010-10-28 | Riichi Murakami | Thin film laminate with metal nanoparticle layer interposed |
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| CN101572279A (en) * | 2009-06-10 | 2009-11-04 | 南开大学 | High mobility textured structure IMO/ZnO composite film grown by sputtering method and application thereof to solar cell |
| CN101985740A (en) * | 2009-07-29 | 2011-03-16 | 中国科学院福建物质结构研究所 | Method for annealing aluminum-doped zinc oxide transparent conductive thin film |
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| JP特开2010-241638A 2010.10.28 |
| 朱锋等.绒面ZnO透明导电薄膜.《人工晶体学报》.2004,第33卷(第3期),第419-421页及第427页. * |
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