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Optimization of Processing and Modeling Issues for Thin Film Solar Cell Devices Including Concepts for the Development of Polycrystalline Multijunctions

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Optimization of Processing and Modeling Issues for Thin Film Solar Cell Devices Including Concepts for the Development of Polycrystalline Multijunctions August 2000 • NREL/SR-520-28783 Optimization of Processing and Modeling Issues for Thin Film Solar Cell Devices Including Concepts for the Development of Polycrystalline Multijunctions Annual Report 24 August 1998—23 August 1999 R.W. Birkmire, J.E. Phillips, W.N. Shafarman, E. Eser, S.S. Hegedus, B.E. McCandless Institute of Energy Conversion Newark, Delaware National Renewable Energy Laboratory 1617 Cole Boulevard Golden, Colorado 80401-3393 NREL is a U.S. Department of Energy Laboratory Operated by Midwest Research Institute ••• Battelle ••• Bechtel Contract No. DE-AC36-99-GO10337 August 2000 • NREL/SR-520-28783 Optimization of Processing and Modeling Issues for Thin Film Solar Cell Devices Including Concepts for the Development of Polycrystalline Multijunctions Annual Report 24 August 1998—23 August 1999 R.W. Birkmire, J.E. Phillips, W.N. Shafarman, E. Eser, S.S. Hegedus, B.E. McCandless Institute of Energy Conversion Newark, Delaware NREL Technical Monitor: B. von Roedern Prepared under Subcontract No. ZAK-8-17619-33 National Renewable Energy Laboratory 1617 Cole Boulevard Golden, Colorado 80401-3393 NREL is a U.S. Department of Energy Laboratory Operated by Midwest Research Institute ••• Battelle ••• Bechtel Contract No. DE-AC36-99-GO10337 NOTICE This report was prepared as an account of work sponsored by an agency of the United States government. Neither the United States government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States government or any agency thereof. Available electronically at http://www.doe.gov/bridge Available for a processing fee to U.S. Department of Energy and its contractors, in paper, from: U.S. Department of Energy Office of Scientific and Technical Information P.O. Box 62 Oak Ridge, TN 37831-0062 phone: 865.576.8401 fax: 865.576.5728 email: [email protected] Available for sale to the public, in paper, from: U.S. Department of Commerce National Technical Information Service 5285 Port Royal Road Springfield, VA 22161 phone: 800.553.6847 fax: 703.605.6900 email: [email protected] online ordering: http://www.ntis.gov/ordering.htm Printed on paper containing at least 50% wastepaper, including 20% postconsumer waste SUMMARY The overall mission of the Institute of Energy Conversion is the development of thin film photovoltaic cells, modules, and related manufacturing technology and the education of students and professionals in photovoltaic technology. The objectives of this 12 month NREL subcontract are to advance the state of the art and the acceptance of thin film PV solar cells in the areas of improved technology for thin film deposition, device fabrication, and material and device characterization and modeling, relating to solar cells based on CuInSe2 and its alloys, on a-Si and its alloys, and on CdTe. CuInSe2-BASED SOLAR CELLS CIS-based Solar Cells with Improved Manufacturability For solar cells based on thin film Cu(InGa)Se2 to become a commercially viable technology, manufacturing costs must be reduced. One means to accomplish this is by reducing the substrate temperature at which the Cu(InGa)Se2 layer is deposited This report addresses material and device issues related to reducing Tss from 550ûC to 400ûC for the deposition of Cu(InGa)Se2 by physical vapor deposition using multisource elemental evaporation. The CuInGaSe2 deposition sequence was varied to determine the effect of a Cu- rich growth step, i.e., deposition with the Cu molar flux greater than the sum of the In and Ga fluxes. The connection between grain size, morphology, compositional uniformity, and device performance, as they are affected by substrate temperature and growth process, was investigated. The objective was to develop a process for improved device performance with Tss = 400ûC. Device results with Tss = 400ûC show that a Cu-rich growth step during the Cu(InGa)Se2 deposition is needed for improved device performance. However, the film and device results are the same whether the Cu-rich growth occurs during the initial nucleation or later in the process. This indicates tolerance to different process sequences, which allows flexibility in deposition process design. Films grown at 550ûC have larger grains and give better performance than films deposited at 400ûC. But, with a given substrate temperature there is no simple correlation between grain size and device performance. At the lower temperature the improved cell results with Cu-rich growth cannot be explained by increased lateral grain size at the surface. Conversely, at the higher temperature, the increased grain size with the Cu-rich growth does not provide improved device performance. At Tss = 550ûC, the device performance is insensitive to the use of Cu-rich growth. A simple process with constant fluxes throughout the deposition gives as high a device efficiency as processes incorporating graded fluxes to give Cu-rich growth. At 400ûC, the uniform process gives more columnar grains but the same lateral grain size as the graded, Cu-rich processes. However, the best devices result from Cu-rich growth although not necessarily during the initial film nucleation. i In-line Evaporation of Cu(InGa)Se2 In-line evaporation is a potentially effective means to achieve the high rate uniform deposition necessary for commercial-scale manufacture of CIGS modules. In this process, the substrate is linearly translated over thermal sources from which the elemental materials are evaporated. The Institute of Energy Conversion has co-developed and installed an in-line deposition system for CIGS processing. The IEC system is configured to handle a rigid substrate with uniform deposition of Cu, In, Ga and Se. The sequencing and spacing of the sources can be varied to allow different relative flux profiles to be investigated. To date, the in-line system has been installed at IEC. Cu, In and Ga effusion sources have been developed, demonstrated and calibrated. Software for vacuum system and substrate drive control has been developed. High Bandgap Alloys of Cu(In,Ga)(S,Se)2 It has been demonstrated previously at IEC that the loss in efficiency of Cu(In,Ga)Se2 solar cells with increasing Ga content is due to a decrease in fill factor, and to a lesser extent Voc which is caused by a drop in the light generated current with increasing forward voltage. Devices were fabricated with semi-transparent (0.04 µm) Mo contacts. Bi-facial spectral response measurements were made as a function of bias voltage and analyzed in order to determine the changes in collection efficiency as a function of changing Ga composition and applied voltage. Analysis of these measurements on devices with increasing Ga content made as a function of light intensity have shown that the main cause of the decrease is a voltage dependent light generated current. Bi-facial spectral response measurements have shown that the minority carrier diffusion length decreases with increasing EG, thereby making the minority carrier collection from the voltage dependent space charge region more important. Sulfurization of Cu, In, and Cu/In Precursors The incorporation of sulfur into CuInSe2 thin films was quantitatively investigated to establish a scientific and engineering basis for the fabrication of homogeneous and compositionally graded CuIn(Se,S)2 thin films. The approach taken was the reaction of thin-film Cu/In layers and CuInSe2 thin films in H2S and/or H2Se gases at atmospheric pressure. This work was largely performed as the Ph.D. dissertation research of Michael Engelmann. CuIn(SeS)2 polycrystalline thin films were fabricated by reaction of layered Cu/In metal precursors in an H2S:H2Se:O2:Ar atmosphere. The H2S/(H2Se+H2S) fraction was controlled and varied from 0.5 to 0.99 and temperature was maintained at 450ûC for all treatments. The solid phase composition of the CuIn(Se,S)2 films after reaction for 120 minutes was found to correspond to the compositional dependence predicted by an equilibrium replacement reaction between H2S-H2Se and CuInSe2-CuInS2, including ideal and non-ideal mixing effects. This reaction was shown to strongly favor the presence of CuInSe2 at 450ûC. Based on these results, prediction and control of the bandgap in the fabrication of homogeneous films is possible. However, the use of hydride gases results in a high degree of compositional ii sensitivity in the solid phase to the gas phase composition in the range of interest. Control of the flow rates becomes critical in this situation. With improved control of the gas phase composition, this method is feasible for the engineering of CuIn(Se,S)2 to optimize the band gap for the solar spectrum. CuInSe2 Team Participation IEC is an active member of four sub-teams under the National CIS Team for the NREL Thin Film Partnership program. The CIS team was restructured into sub-teams designed to directly support the industrial partners. IEC is active with the following: Global Solar Energy. This team is focusing on helping GSE develop a low temperature process for the roll-to-roll deposition of Cu(InGa)Se2. IEC is providing direct support through materials characterization and device fabrication and characterization. ISET. IEC is assisting in the development of improved performance of ISET's CIS-based materials by investigating the use of sulfur incorporation to increase the voltages in the devices and modules.
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