CN103413869A - Preparation method of textured ZnO-TCO film and application of textured ZnO-TCO film - Google Patents

Preparation method of textured ZnO-TCO film and application of textured ZnO-TCO film Download PDF

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CN103413869A
CN103413869A CN2013102943176A CN201310294317A CN103413869A CN 103413869 A CN103413869 A CN 103413869A CN 2013102943176 A CN2013102943176 A CN 2013102943176A CN 201310294317 A CN201310294317 A CN 201310294317A CN 103413869 A CN103413869 A CN 103413869A
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陈新亮
张晓丹
赵颖
赵慧旭
杨旭
倪牮
张德坤
魏长春
张建军
耿新华
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Nankai University
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02E10/00—Energy generation through renewable energy sources
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    • Y02E10/548—Amorphous silicon PV cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

The invention relates to a preparation method of a textured ZnO-TCO film and application of the textured ZnO-TCO film. The textured ZnO-TCO film is structurally characterized by glass/low-doped textured ZnO:B/ultrathin ITO film/high-conductivity transparent ZnO:B film. The preparation method of the textured ZnO-TCO film comprises the following steps that: a textured low-content boron-doped ZnO transparent conductive film is grown on a glass substrate through using metal organic chemical vapor deposition (MOCVD) technology; 2) the ultrathin Sn-doped In2O3 film is grown through using thermal evaporation technology; and 3) small grain-sized high-conductivity and highly-transparent ZnO:B film is grown on the film. According to the invention, the ZnO film is obtained through using the metal organic chemical vapor deposition (MOCVD) technology, and therefore, the concentration of free carriers can be decreased under a lower-B-doped condition, and electron mobility of the film can be improved; and the ultrathin ITO film is grown through using the thermal evaporation technology, and therefore, the growth orientation of the ZnO film can be promoted, and crystallization can be also promoted; and if the textured ZnO-TCO film is applied to a pin-type Si-base layered film solar cell, high photoelectric conversion efficiency can be realized.

Description

Preparation method and the application thereof of a kind of matte structure ZnO-TCO film
Technical field
The present invention relates to the solar cell transparent conductive oxide film, particularly preparation method and the application thereof of a kind of matte structure ZnO-TCO film.
Background technology
The optical bandwidth of amorphous silicon hydride (a-Si:H) is 1.7 eV left and right, its absorption coefficient is higher in the shortwave direction, and the optical bandwidth of microcrystalline hydrogenated silicon (μ c-Si:H) is about 1.1 eV, its absorption coefficient is higher in the long wave direction, and can absorb the near-infrared Long wavelength region, absorbing wavelength can extend to 1100nm, and this just makes solar spectrum can obtain more good utilisation.In addition, than amorphous silicon thin-film materials, microcrystalline silicon film material structure order degree is high, and therefore, the microcrystalline silicon film battery has good device stability, without obvious decay.As can be seen here, microcrystalline silicon solar cell can utilize the near infrared light zone of solar spectrum preferably, and novel amorphous silicon/microcrystal silicon (a-Si:H/ μ c-Si:H) laminated film solar battery will be expanded the solar spectrum range of application, whole stability test and the efficiency of improving ,Referring to: J. Meier, S. Dubail, R. Platz, etc. Sol. Energy Mater. Sol. Cells 49 (1997) 35; Arvind Shah, J. Meier, E. Vallat-Sauvain, etc, Thin Solid Films 403-404 (2002) 179.
Crystallite dimension has good scattering process to the light of the wavelength of can comparing.Research shows, the application of suede structure (textured structure) transparent conductive oxide ━ TCO film can the enhanced light scattering effect, improve and fall into light effect, it plays conclusive impact to efficiency and the stability (SW effect) that improves the Si base thin film solar battery ,Referring to: A. V. Shah, H. Schade, M. Vanecek, etc, Progress in Photovoltaics, 12 (2004) 113.The crystallite dimension of the main and film of suede structure, the factors such as grain shape and roughness are relevant.
MOCVD(metal organic chemical vapor deposition ━ MOCVD, i.e. metal-organic chemical vapor deposition equipment) but the technology direct growth goes out the ZnO film of suede structure ,Referring to: X.L. Chen, X.H. Geng, J.M. Xue, etc. J. Cryst. Growth, 296 (2006) 43; Chen Xinliang, Xue Junming, Sun Jian etc., the semiconductor journal, 2007,28(7): 1072; W.W. Wenas, A. Yamada, K. Takahashi, etc, J. Appl. Phys. 70 (1991) 7119; S. Fa, U. Kroll, C. Bucher, etc, Sol. Energy Mater. Sol. Cells 86 (2005) 385; S. Fa, L. Feitknecht, R. Schluchter, etc, Sol. Energy Mater. Sol. Cells 90 (2006) 2960.Thin film growth process is the thermal decomposition process without particle bombardment, depositing temperature low (~ 423 K); Can realize high-speed, large tracts of land and ZnO film growth uniformly, meet the industrialized development requirement.The surface topography of typical MOCVD-ZnO film, crystal grain presents " pyramid-like " shape, corresponding (110) peak preferred orientation in the XRD diffraction spectra, characteristic grain size ~ 300-500 nm, mean roughness σ rms =40-80 nm, resistivity ρ~ 1.5-3 * 10 -3Ω cm.
Suede structure BZO film do before microcrystalline hydrogenated silicon (μ c-Si:H) battery of electrode can provide high short-circuit current density ( J Sc ), but sharp-pointed " pyramid-like " shape make the fill factor, curve factor (FF) of solar cell and open circuit voltage ( V Oc ) relatively low ,Referring to: M. Python, E. Vallat-Sauvain, J. Bailat, etc, J. Non-Cryst. Solids, 354 (2008) 2258; K.C. Lai, C.C. Liu, C.H. Lu, etc, Sol. Energy Mater. Sol. Cells 94 (2010) 397.Be mainly because the contact interface of itself and battery material is too precipitous, multiple hole or defects i.e.cracks structure easily occur when dopant deposition layer p-Si:H and active layer i-Si:H material, have a strong impact on migration and the collection of charge carrier.In order on the BZO film at matte, to obtain the high efficiency silicon-based thin film solar cell, will be optimized BZO film surface characteristic, make its existing stronger sunken luminous energy power, good BZO/p-Si interface is arranged again.According to the literature, the researcher has attempted many methods, and as plasma surface treatment, growing film on coarse glass substrate, introduce amorphous silicon material as resilient coating, multi-layer film structure, nanometer embossing etc. ,Referring to: M. Boccard, P. Cuony, M. Despeisse, etc, Sol. Energy Mater. Sol. Cells 95 (2011) 195; H. Aswin, K. Taweewat, A.Y. Ihsanul, etc, Appl. Phys. Express 3 (2010) 051102; J. Steinhauser, J.F. Boucher, E. Omnes, etc, Thin Solid Films 520 (2011) 1218; K. Soderstrom, G. Bugnon, F.J. Haug, etc, Sol. Energy Mater. Sol. Cells 101 (2012) 193; M. Boccard, C. Battaglia, S. Hanni, etc, 2012 Nano Lett. 12 1344; D. Messerschmidt, S. Nicolay, L. Ding, etc, 2013 J. Appl. Phys. 113 024908.
Summarize describedly, exploitation has the ZnO-TCO film that applicable Si base thin film solar battery applies becomes emphasis and the future thrust in current research work.
Summary of the invention
The objective of the invention is to solve the low electron mobility of normal transparent conductive film and surface texture is sharp-pointed and light scattering characteristic a little less than, thereby impact improves the problem of Si hull cell performance, a kind of growing ZnO-TCO thin film with suede structure and application process thereof are provided, adopt the MOCVD technology to prepare large crystallite dimension and little crystallite dimension ZnO:B film, the ZnO film obtained has suede structure, in low B doping situation, effectively reduced the sub-concentration of free subflow simultaneously, and can improve the thin film electronic mobility, reduced the absorption near infrared region.
Technical scheme of the present invention:
The preparation method of a kind of matte structure ZnO-TCO film, the architectural feature of described matte structure ZnO-TCO film are the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and preparation process is as follows:
1) take glass is substrate, take diethyl zinc (DEZn) and the water (H of purity as 99.995% 2O) be raw material, take the borine B of hydrogen diluted concentration as 1.0% 2H 6As impurity gas, utilize the MOCVD technology, growth glass/low-doped type matte structure ZnO: the B transparent conductive film, film thickness is 1000-1800nm, utilizes the technological parameter of MOCVD technology: the base substrate temperature is 135-165 ℃, B 2H 6Dopant gas flow is the 0.1-1.0% of diethyl zinc flow, and reaction pressure is 1.0 Torr, and growth rate is 20-100 nm/min;
2) take the In-Sn alloy of purity as 99.99% is raw material, and in the In-Sn alloy, the weight percent content of Sn doping is 6.0-10.0%, take the O of purity as 99.99% 2Gas is as reacting gas, utilizes thermal evaporation techniques at the glass of above-mentioned acquisition/low-doped type matte structure ZnO: grow ultra-thin Sn doping film (In on the B transparent conductive film 2O 3: Sn, i.e. ITO), film thickness is 2-15nm, utilizes the technological parameter of thermal evaporation techniques: underlayer temperature is 235-350 ℃, and vaporization voltage is 5V, and evaporation current is 200A, and evaporation rate is 0.01nm/s, O 2Dividing potential drop is 1.5-2.5 * 10 -1Pa;
3) take purity is 99.995% diethyl zinc (DEZn) and water (H 2O) be raw material, the hydrogen diluted concentration is 1.0% borine B 2H 6As impurity gas, utilize the MOCVD technology at above-mentioned glass/low-doped type matte structure ZnO: the ultra-thin ito thin film of B/ OnThe high electricity of the little crystallite dimension of growing is led the ZnO:B transparent conductive film, film thickness 50-300nm, and utilize the technological parameter of MOCVD technology: underlayer temperature is 135-165 ℃, B 2H 6Dopant gas flow is 1.0% of diethyl zinc flow, and reaction pressure is 1.0 Torr, and growth rate is 20-100 nm/min.
The application of a kind of prepared matte structure ZnO-TCO film, for pin type Si base laminated film solar battery.
Advantage of the present invention and effect: the MOCVD technology can be regulated and be obtained large crystallite dimension and little crystallite dimension ZnO:B film, the ZnO film obtained has suede structure, in low B doping situation, effectively reduced the sub-concentration of free subflow simultaneously, and can improve the thin film electronic mobility, reduced the absorption near infrared region.In addition, thermal evaporation techniques can be grown and be controlled ultra-thin ito thin film, and the growth orientation that it can promote ZnO film, improve interfacial characteristics, promotes crystallization etc.Therefore, in conjunction with the suede structure feature of ZnO film and the interface modification of ultra-thin ito thin film (making surface be tending towards soft adaptation film growth), expectation obtains the optical scattering of visible light and near infrared region, improve the growth of follow-up Si base film, reduce crackle and the defect of active layer, realize high light electricity transformation efficiency.
Basic thought of the present invention is in conjunction with the MOCVD technology growth, to regulate the advantage of large crystallite dimension and little crystallite dimension ZnO:B film feature and thermal evaporation techniques growing high-quality ito thin film, realize the NEW TYPE OF COMPOSITE glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and be applied to the Si base thin film solar battery.At first, utilize the MOCVD technology on glass substrate, to prepare the large crystallite dimension matte structure ZnO of low B doping: B transparent conductive film, film thickness 1000-1800nm; Secondly, glass/low-doped type matte structure ZnO: on the B Membranous Foundations, by thermal evaporation techniques grow ultra-thin ito thin film, film thickness 2-15nm; Finally, at glass/low-doped type matte structure ZnO: utilize the high electricity of MOCVD technology growth to lead little crystallite dimension ZnO:B film on the ultra-thin ito thin film of B/ basis.NEW TYPE OF COMPOSITE glass/ultra-thin the ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and be applied to the Si base thin film solar battery.
Typical case's sandwich type matte structure ZnO film resistivity 7.22 * 10 -4Ω cm, square resistance 7.2 Ω, carrier concentration 1.96 * 10 20Ω cm, electron mobility 44.1cm 2V -1s -1, visible light and near infrared region mean transmissivity 80%.The matte structure ZnO film that this kind technology obtains has improved visible-range and near infrared region spectrum sees through that (λ=380-1100nm), and having strengthened the incident scattering of light can be applicable to pin type Si base thin film solar battery.
[accompanying drawing explanation]
Fig. 1 is glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B membrane structure schematic diagram.
Fig. 2 is ESEM (SEM) image of this glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film.
Fig. 3 is that the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B membrane structure is applied to pin type Si base laminated film solar battery structure chart.
Fig. 4 is the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film and conventional glass/suede structure SnO 2: the F film is applied to the electric current of pin type Si base laminated film solar battery -voltage (J-V)Curve.
[embodiment]
Embodiment 1:
The preparation method of a kind of matte structure ZnO-TCO film, the architectural feature of described matte structure ZnO-TCO film are the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and as shown in Figure 1, preparation process is as follows:
1) take glass is substrate, take diethyl zinc (DEZn) and the water (H of purity as 99.995% 2O) be raw material, take the borine B of hydrogen diluted concentration as 1.0% 2H 6As impurity gas, utilize the MOCVD technology, growth glass/low-doped type matte structure ZnO: the B transparent conductive film, film thickness is 1200nm, utilizes the technological parameter of MOCVD technology: the base substrate temperature is 150 ℃, B 2H 6Dopant gas flow is 0.3% of DEZn flow, and reaction pressure is 1.0 Torr, and growth rate is 50 nm/min;
2) take the In-Sn alloy of purity as 99.99% is raw material, and in the In-Sn alloy, the weight percent content of Sn doping is 10.0%, take the O of purity as 99.99% 2Gas is as reacting gas, utilizes thermal evaporation techniques at the glass of above-mentioned acquisition/low-doped type matte structure ZnO: grow ultra-thin Sn doping film (In on the B transparent conductive film 2O 3: Sn, i.e. ITO), film thickness is 3nm, utilizes the technological parameter of thermal evaporation techniques: underlayer temperature is 250 ℃, and vaporization voltage is 5V, and evaporation current is 200A, and evaporation rate is 0.01nm/s, O 2Dividing potential drop is 2.0 * 10 -1Pa;
3) take purity is 99.995% diethyl zinc (DEZn) and water (H 2O) be raw material, the hydrogen diluted concentration is 1.0% borine B 2H 6As impurity gas, utilize the MOCVD technology at above-mentioned glass/low-doped type matte structure ZnO: the ultra-thin ito thin film of B/ OnThe high electricity of the little crystallite dimension of growing is led the ZnO:B transparent conductive film, film thickness 200nm, and utilize the technological parameter of MOCVD technology: underlayer temperature is 150 ℃, B 2H 6Dopant gas flow is 1.0% of DEZn flow, and reaction pressure is 1.0 Torr, and growth rate is 50 nm/min.
Fig. 2 is ESEM (SEM) image of this glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, in figure, show: film surface presents " cauliflower " shape structure, the ZnO crystal of the little crystallite dimension of preparation on large crystallite dimension.
This glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film is used for to pin type silicon-based thin film solar cell, solar battery structure as shown in Figure 3, is amorphous silicon (a-Si:H)/crystallite SiGe (μ c-SiGe:H) stacked solar cell, cascade solar cell.With with traditional glass/SnO 2: F suede structure film is compared as front electrode solar cell, battery short circuit current density and the battery efficiency of this pin type silicon-based thin film solar cell improve respectively 17.4% and 10.6%, glass/ultra-thin the ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film as suede structure before the efficiency of solar cell of electrode reach 9.04%, as shown in Figure 4.
Embodiment 2:
The preparation method of a kind of matte structure ZnO-TCO film, the architectural feature of described matte structure ZnO-TCO film are the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and as shown in Figure 1, preparation process is as follows:
1) take glass is substrate, take diethyl zinc (DEZn) and the water (H of purity as 99.995% 2O) be raw material, take the borine B of hydrogen diluted concentration as 1.0% 2H 6As impurity gas, utilize the MOCVD technology, growth glass/low-doped type matte structure ZnO: the B transparent conductive film, film thickness is 1800nm, utilizes the technological parameter of MOCVD technology: the base substrate temperature is 150 ℃, B 2H 6Dopant gas flow is 0.5% of DEZn flow, and reaction pressure is 1.0 Torr, and growth rate is 50 nm/min;
2) take the In-Sn alloy of purity as 99.99% is raw material, and in the In-Sn alloy, the weight percent content of Sn doping is 10.0%, take the O of purity as 99.99% 2Gas is as reacting gas, utilizes thermal evaporation techniques at the glass of above-mentioned acquisition/low-doped type matte structure ZnO: grow ultra-thin Sn doping film (In on the B transparent conductive film 2O 3: Sn, i.e. ITO), film thickness is 5nm, utilizes the technological parameter of thermal evaporation techniques: underlayer temperature is 250 ℃, and vaporization voltage is 5V, and evaporation current is 200A, and evaporation rate is 0.01nm/s, O 2Dividing potential drop is 2.5 * 10 -1Pa;
3) take purity is 99.995% diethyl zinc (DEZn) and water (H 2O) be raw material, the hydrogen diluted concentration is 1.0% borine B 2H 6As impurity gas, utilize the MOCVD technology at above-mentioned glass/low-doped type matte structure ZnO: the ultra-thin ito thin film of B/ OnThe high electricity of the little crystallite dimension of growing is led the ZnO:B transparent conductive film, film thickness 150nm, and utilize the technological parameter of MOCVD technology: underlayer temperature is 150 ℃, B 2H 6Dopant gas flow is 1.0% of DEZn flow, and reaction pressure is 1.0 Torr, and growth rate is 50 nm/min.
This glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film is for pin type silicon-based thin film solar cell, identical with embodiment 1.

Claims (2)

1. the preparation method of matte structure ZnO-TCO film, it is characterized in that: the architectural feature of described matte structure ZnO-TCO film is the glass/ultra-thin ito thin film of low-doped type matte structure ZnO: B//highly conductive, transparent ZnO:B film, and preparation process is as follows:
1) take glass is substrate, and diethyl zinc and the water of purity as 99.995% of take is raw material, take the borine B of hydrogen diluted concentration as 1.0% 2H 6As impurity gas, utilize the MOCVD technology, growth glass/low-doped type matte structure ZnO: the B transparent conductive film, film thickness is 1000-1800nm, utilizes the technological parameter of MOCVD technology: the base substrate temperature is 135-165 ℃, B 2H 6Dopant gas flow is the 0.1-1.0% of diethyl zinc flow, and reaction pressure is 1.0 Torr, and growth rate is 20-100 nm/min;
2) take the In-Sn alloy of purity as 99.99% is raw material, and in the In-Sn alloy, the weight percent content of Sn doping is 6.0-10.0%, take the O of purity as 99.99% 2Gas is as reacting gas, utilize thermal evaporation techniques at the glass of above-mentioned acquisition/low-doped type matte structure ZnO: grow ultra-thin Sn doping film on the B transparent conductive film, film thickness is 2-15nm, utilize the technological parameter of thermal evaporation techniques: underlayer temperature is 235-350 ℃, vaporization voltage is 5V, evaporation current is 200A, and evaporation rate is 0.01nm/s, O 2Dividing potential drop is 1.5-2.5 * 10 -1Pa;
3) take purity is raw material as 99.995% diethyl zinc and water, and the hydrogen diluted concentration is 1.0% borine B 2H 6As impurity gas, utilize the MOCVD technology at above-mentioned glass/low-doped type matte structure ZnO: the ultra-thin ito thin film of B/ OnThe high electricity of the little crystallite dimension of growing is led the ZnO:B transparent conductive film, film thickness 50-300nm, and utilize the technological parameter of MOCVD technology: underlayer temperature is 135-165 ℃, B 2H 6Dopant gas flow is 1.0% of diethyl zinc flow, and reaction pressure is 1.0 Torr, and growth rate is 20-100 nm/min.
2. the application of the prepared matte structure ZnO of a claim 1-TCO film, is characterized in that: for pin type Si base laminated film solar battery.
CN2013102943176A 2013-07-15 2013-07-15 Preparation method of textured ZnO-TCO film and application of textured ZnO-TCO film Pending CN103413869A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN106373992A (en) * 2016-09-19 2017-02-01 陕西理工学院 Boron-doped zinc oxide laminated sphere/p-type PET-ITO heterojunction and preparation method and application thereof
CN108235789A (en) * 2015-09-09 2018-06-29 无限股份有限公司 Thin film solar cell and its manufacturing method

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CN102176471A (en) * 2011-03-11 2011-09-07 南开大学 Textured structural ZnO:B (BZO)/ZnO:Ga/H (HGZO) composite thin film and application
CN102945865A (en) * 2012-11-23 2013-02-27 南开大学 Conductive back reflection electrode based on pyramid texture degree morphology ZnO layer

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CN102176471A (en) * 2011-03-11 2011-09-07 南开大学 Textured structural ZnO:B (BZO)/ZnO:Ga/H (HGZO) composite thin film and application
CN102945865A (en) * 2012-11-23 2013-02-27 南开大学 Conductive back reflection electrode based on pyramid texture degree morphology ZnO layer

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Publication number Priority date Publication date Assignee Title
CN108235789A (en) * 2015-09-09 2018-06-29 无限股份有限公司 Thin film solar cell and its manufacturing method
CN106373992A (en) * 2016-09-19 2017-02-01 陕西理工学院 Boron-doped zinc oxide laminated sphere/p-type PET-ITO heterojunction and preparation method and application thereof
CN106373992B (en) * 2016-09-19 2019-03-12 陕西理工学院 A kind of boron doping zinc oxide lamella ball/p-type PET-ITO hetero-junctions and its preparation method and application

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Application publication date: 20131127