A thermodynamic evaluation of metal halides for the recrystallization of Cu(In,Ga)Se2

Palmiotti, Elizabeth; Marsillac, Sylvain; Rockett, Angus

doi:10.1002/pip.3604

A thermodynamic evaluation of metal halides for the recrystallization of Cu(In,Ga)Se₂

Journal Article · Fri Jul 01 00:00:00 EDT 2022 · Progress in Photovoltaics

DOI:https://doi.org/10.1002/pip.3604· OSTI ID:1991292

^[1]; Marsillac, Sylvain ^[2]; ^[3]

Colorado School of Mines, Golden, CO (United States); Colorado School of Mines
Old Dominion University, Norfolk, VA (United States)
Colorado School of Mines, Golden, CO (United States)

CdTe films are deposited at low temperatures and recrystallized to photovoltaic device quality using CdCl₂ treatments, leading to competitive manufacturing costs. Cu(In,Ga)Se₂ (CIGS) typically requires high-temperature, low-rate depositions to produce high-efficiency devices, resulting in higher costs. A similar metal halide treatment of CIGS has been demonstrated by us previously for some metal halide sources. To understand and optimize the process, a thermodynamic evaluation of candidate metal halides for such treatments is presented as a guide for their selection. By comparing bond dissociation energies, mono- and di-halide compounds are proposed to be ideal compounds to act as transport agents. Known recrystallization and temperature reduction benefits by Ag alloying suggests that Ag-halides should be used to aid transport of all species. The high vapor pressure and mobility of Ga compounds still poses a problem for metal halide treatment resulting in Ga etching and removal of intentional Ga gradients. Less severe but similar issues with In compounds may occur. As a result, Cu compounds have low vapor pressures which may limit transport, however, Cu is highly mobile in CIGS and recrystallization still occurs.

View Accepted Manuscript (DOE)

Research Organization:: Colorado School of Mines, Golden, CO (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: EE0007551

OSTI ID:: 1991292

Alternate ID(s):: OSTI ID: 1874691

Journal Information:: Progress in Photovoltaics, Journal Name: Progress in Photovoltaics Journal Issue: 1 Vol. 31; ISSN 1062-7995

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (55)

Optimization of vapor post-deposition processing for evaporated CdS/CdTe solar cells McCandless, B. E.; Youm, I.; Birkmire, R. W. Progress in Photovoltaics: Research and Applications, Vol. 7, Issue 1 https://doi.org/10.1002/(SICI)1099‐159X(199901/02)7:1%3C21::AID‐PIP244%3E3.0.CO;2‐D	journal	January 1999
Structural Properties of CuGaxIn1-xSe2 Thin Films Deposited by Spray Pyrolysis Ramakrishna Reddy, K. T.; Chalapathy, R. B. V. Crystal Research and Technology, Vol. 34, Issue 1 https://doi.org/10.1002/(SICI)1521‐4079(199901)34:1%3C127::AID‐CRAT127%3E3.0.CO;2‐5	journal	January 1999
A model for the successful growth of polycrystalline films of CuInSe2 by multisource physical vacuum evaporation Klenk, Reiner; Walter, Thomas; Schock, Hans-Werner Advanced Materials, Vol. 5, Issue 2 https://doi.org/10.1002/adma.19930050209	journal	February 1993
A Comparative Study of the Effects of Nontoxic Chloride Treatments on CdTe Solar Cell Microstructure and Stoichiometry Williams, Benjamin L.; Major, Jonathan D.; Bowen, Leon Advanced Energy Materials, Vol. 5, Issue 21 https://doi.org/10.1002/aenm.201500554	journal	July 2015
Solar cell efficiency tables (Version 55) Green, Martin A.; Dunlop, Ewan D.; Hohl‐Ebinger, Jochen Progress in Photovoltaics: Research and Applications, Vol. 28, Issue 1 https://doi.org/10.1002/pip.3228	journal	December 2019
Cu(In,Ga)Se ₂ thin films grown with a Cu-poor/rich/poor sequence: growth model and structural considerations: Cu(In,Ga)Se ₂ THIN-FILM GROWTH Kessler, J.; Chityuttakan, C.; Lu, J. Progress in Photovoltaics: Research and Applications, Vol. 11, Issue 5 https://doi.org/10.1002/pip.495	journal	July 2003
Vapour pressures and sublimation enthalpy of solid indium(III) iodide Brunetti, Bruno; Giustini, Antonio; Piacente, Vincenzo The Journal of Chemical Thermodynamics, Vol. 29, Issue 2 https://doi.org/10.1006/jcht.1996.0156	journal	February 1997
Effects of CdCl2 in CdTe on the properties of sintered CdS/CdTe solar cells Roh, J. S.; Im, H. B. Journal of Materials Science, Vol. 23, Issue 6 https://doi.org/10.1007/BF01115799	journal	June 1988
Mass-spectrometric study of (indium + chlorine)(g) Enthalpies of formation of InCl(g), In2Cl2(g), In2Cl4(g), InCl3(g), and In2Cl6(g) Defoort, F.; Chatillon, C.; Bernard, C. The Journal of Chemical Thermodynamics, Vol. 20, Issue 12 https://doi.org/10.1016/0021‐9614(88)90039‐0	journal	December 1988
The preparation and vapour pressures of the indium(I) halides and the standard molar Gibbs free energy change for formation of InX from In(g) and X2(g), (X = Cl, Br, or I) Brumleve, T. R.; Mucklejohn, S. A.; O'Brien, N. W. The Journal of Chemical Thermodynamics, Vol. 21, Issue 11 https://doi.org/10.1016/0021‐9614(89)90106‐7	journal	November 1989
Vapor phase equilibria in the systems In-InCl3 and Ga-GaCl3 Kuniya, Y.; Hosaka, M. Journal of Crystal Growth, Vol. 28, Issue 3 https://doi.org/10.1016/0022‐0248(75)90077‐9	journal	April 1975
Photovoltaic properties of CdS/CdTe solar cells sintered with CdCl2 Moon, J. T.; Park, K. C.; Im, H. B. Solar Energy Materials, Vol. 18, Issue 1-2 https://doi.org/10.1016/0165‐1633(88)90044‐5	journal	December 1988
The structure of CuInSe2 films formed by co-evaporation of the elements Don, E. R.; Hill, R.; Russell, G. J. Solar Cells, Vol. 16 https://doi.org/10.1016/0379‐6787(86)90079‐7	journal	January 1986
Analysis of post deposition processing for CdTe/CdS thin film solar cells McCandless, Brian E.; Birkmire, Robert W. Solar Cells, Vol. 31, Issue 6 https://doi.org/10.1016/0379‐6787(91)90095‐7	journal	December 1991
Structural and chemical interface characterization of CdTe solar cells by transmission electron microscopy Terheggen, M.; Heinrich, H.; Kostorz, G. Thin Solid Films, Vol. 431-432 https://doi.org/10.1016/S0040‐6090(03)00268‐2	journal	May 2003
Recrystallization of CIGSe layers grown by three-step processes: A model based on grain boundary migration Barreau, N.; Painchaud, T.; Couzinié-Devy, F. Acta Materialia, Vol. 58, Issue 17 https://doi.org/10.1016/j.actamat.2010.06.025	journal	October 2010
Diffusion-induced grain boundary migration as mechanism for grain growth and defect annihilation in chalcopyrite thin films Stange, Helena; Brunken, Stephan; Greiner, Dieter Acta Materialia, Vol. 111 https://doi.org/10.1016/j.actamat.2016.03.073	journal	June 2016
Reaction kinetics study of CdTe thin films during CdCl2 heat treatment Kim, MaengJun; Sohn, SangHo; Lee, SungHo Solar Energy Materials and Solar Cells, Vol. 95, Issue 8 https://doi.org/10.1016/j.solmat.2011.03.044	journal	August 2011
Ag incorporation in low-temperature grown Cu(In,Ga)Se2 solar cells using Ag precursor layers Kim, Kihwan; Park, Joo Wan; Yoo, Jin Su Solar Energy Materials and Solar Cells, Vol. 146 https://doi.org/10.1016/j.solmat.2015.11.028	journal	March 2016
Vapor pressure measurements of CuBr and ZnBr2 by the Knudsen effusion method and their vapor species identification Iizuka, Atsushi; Shibata, Etsuro; Sato, Makiko Thermochimica Acta, Vol. 593 https://doi.org/10.1016/j.tca.2014.08.003	journal	October 2014
Vapor pressure measurements of AgBr by the Knudsen effusion method Nagata, Tetsuya; Iizuka, Atsushi; Shibata, Etsuro Thermochimica Acta, Vol. 671 https://doi.org/10.1016/j.tca.2018.10.027	journal	January 2019
High sensitivity and wide bandwidth image sensor using CuIn1−xGaxSe2 thin films Miyazaki, K.; Matsushima, O.; Moriwake, M. Thin Solid Films, Vol. 517, Issue 7 https://doi.org/10.1016/j.tsf.2008.11.029	journal	February 2009
Thinning of CIGS solar cells: Part I: Chemical processing in acidic bromine solutions Bouttemy, M.; Tran-Van, P.; Gerard, I. Thin Solid Films, Vol. 519, Issue 21 https://doi.org/10.1016/j.tsf.2010.12.219	journal	August 2011
Impact of Post-Deposition Recrystallization by Alkali Fluorides on Cu(In,Ga)Se2Thin-Film Materials and Solar Cells Rajan, Grace; Belfore, Benjamin; Karki, Shankar Thin Solid Films, Vol. 690 https://doi.org/10.1016/j.tsf.2019.137526	journal	November 2019
Recrystallization of Cu(In,Ga)Se2 Semiconductor Thin Films via InCl3 Treatment Belfore, Benjamin; Poudel, Deewakar; Karki, Shankar Thin Solid Films, Vol. 735 https://doi.org/10.1016/j.tsf.2021.138897	journal	October 2021
The Powder Diffraction File: a quality materials characterization database Gates-Rector, Stacy; Blanton, Thomas Powder Diffraction, Vol. 34, Issue 4 https://doi.org/10.1017/S0885715619000812	journal	November 2019
Vapor Pressure of Pure Substances. Organic and Inorganic Compounds Stull, Daniel R. Industrial & Engineering Chemistry, Vol. 39, Issue 4 https://doi.org/10.1021/ie50448a022	journal	April 1947
The Vapor Pressures of Selenium Tetrachloride. the Existence of Selenium Dichloride Yost, Don M.; Kircher, Charles E. Journal of the American Chemical Society, Vol. 52, Issue 12 https://doi.org/10.1021/ja01375a008	journal	December 1930
Vapor Pressure and Heat of Vaporization of Some Simple Molten Electrolytes Bloom, H.; Bockris, J. O'M.; Richards, N. E. Journal of the American Chemical Society, Vol. 80, Issue 9 https://doi.org/10.1021/ja01542a004	journal	May 1958
A Study on the Sublimation of Gallium Tribromide Brunetti, Bruno; Piacente, Vincenzo; Scardala, Paolo Journal of Chemical & Engineering Data, Vol. 54, Issue 8 https://doi.org/10.1021/je900182h	journal	May 2009
Vapor Pressures of Gallium Trifluoride, Trichloride, and Triiodide and Their Standard Sublimation Enthalpies Brunetti, Bruno; Piacente, Vincenzo; Scardala, Paolo Journal of Chemical & Engineering Data, Vol. 55, Issue 1 https://doi.org/10.1021/je900276q	journal	August 2009
A Torsion Study on the Sublimation Process of InCl ₃ Brunetti, Bruno; Piacente, Vincenzo; Scardala, Paolo Journal of Chemical & Engineering Data, Vol. 43, Issue 1 https://doi.org/10.1021/je970188a	journal	January 1998
Analysis of Bulk and Interface Phenomena in CdTe/CdS Thin-Film Solar Cells Terheggen, M.; Heinrich, H.; Kostorz, G. Interface Science, Vol. 12, Issue 2/3 https://doi.org/10.1023/B:INTS.0000028655.11608.c7	journal	April 2004
Vapour pressures of the solid copper (I) halides Shelton, R. A. J. Transactions of the Faraday Society, Vol. 57 https://doi.org/10.1039/TF9615702113	journal	January 1961
Specular CuInSe ₂ films for solar cells Birkmire, R. W.; McCandless, B. E. Applied Physics Letters, Vol. 53, Issue 2 https://doi.org/10.1063/1.100576	journal	July 1988
High‐efficiency CuIn _x Ga _{1− x} Se ₂ solar cells made from (In _x ,Ga _{1− x} ) ₂ Se ₃ precursor films Gabor, Andrew M.; Tuttle, John R.; Albin, David S. Applied Physics Letters, Vol. 65, Issue 2 https://doi.org/10.1063/1.112670	journal	July 1994
Epitaxial growth of Cu(In, Ga)Se2 on GaAs(110) Liao, D.; Rockett, A. Journal of Applied Physics, Vol. 91, Issue 4 https://doi.org/10.1063/1.1434549	journal	February 2002
The structure and morphology of (112)-oriented Cu(In,Ga)Se2 epitaxial films Liao, Dongxiang; Rockett, Angus Journal of Applied Physics, Vol. 104, Issue 9 https://doi.org/10.1063/1.3009961	journal	November 2008
Surface segregation model for Sn‐doped GaAs grown by molecular beam epitaxy Rockett, A.; Drummond, T. J.; Greene, J. E. Journal of Applied Physics, Vol. 53, Issue 10 https://doi.org/10.1063/1.330013	journal	October 1982
Structural properties of CuIn _x Ga _{1− x} Se ₂ thin films prepared by rf sputtering Yamaguchi, Toshiyuki; Matsufusa, Jiro; Yoshida, Akira Journal of Applied Physics, Vol. 72, Issue 12 https://doi.org/10.1063/1.351966	journal	December 1992
High V oc in (Cu,Ag)(In,Ga)Se 2 Solar Cells Edoff, Marika; Jarmar, Tobias; Nilsson, Nina Shariati IEEE Journal of Photovoltaics, Vol. 7, Issue 6 https://doi.org/10.1109/JPHOTOV.2017.2756058	journal	November 2017
Vapor phase treatment of CdTe/CdS thin films with CdCl/sub 2/:O/sub 2/ McCandless, B. E.; Hichri, H.; Hanket, G. Conference Record of the Twenty Fifth IEEE Photovoltaic Specialists Conference - 1996 https://doi.org/10.1109/PVSC.1996.564244	conference	January 1996
Post-Deposition Recrystallization of Chloride Treated Cu(In x Ga (1-x)) Se 2 Thin-Film Solar Cells Palmiotti, Elizabeth; Soltanmohammad, Sina; Rockett, Angus 2018 IEEE 7th World Conference on Photovoltaic Energy Conversion (WCPEC) (A Joint Conference of 45th IEEE PVSC, 28th PVSEC & 34th EU PVSEC) https://doi.org/10.1109/PVSC.2018.8547595	conference	June 2018
Post-Deposition Recrystallization of Co-Evaporated CuIn _x Ga _(1-x) Se ₂ Films by Bromide Vapor Treatments Palmiotti, Elizabeth; Karki, Shankar; Belfore, Ben 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) https://doi.org/10.1109/PVSC40753.2019.8980803	conference	June 2019
Grain Growth in CdTe Films During CdCl ₂ Treatment: TeCl ₄ Theory Winger, Joshua R.; Scarpulla, Michael A. 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) https://doi.org/10.1109/PVSC40753.2019.8980923	conference	June 2019
Studying the Recrystallization of Cu(InGa)Se ₂ Semiconductor Thin Films by Silver Bromide In-situ Treatment Poudel, Deewakar; Lepetit, Thomas; Belfore, Benjamin 2021 IEEE 48th Photovoltaic Specialists Conference (PVSC) https://doi.org/10.1109/PVSC43889.2021.9518578	conference	June 2021
Vapor chloride treatment of polycrystalline CdTe/CdS films Zhou, T. X.; Reiter, N.; Powell, R. C. Proceedings of 1994 IEEE 1st World Conference on Photovoltaic Energy Conversion - WCPEC (A Joint Conference of PVSC, PVSEC and PSEC) https://doi.org/10.1109/WCPEC.1994.519818	conference	January 1994
Analysis of the rate of vaporization of CuCl for solar cell fabrication Brestovansky, D. F.; Baron, B. N.; Rocheleau, R. E. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 1, Issue 1 https://doi.org/10.1116/1.572305	journal	January 1983
Ceramic Thin Film CdTe Solar Cell Nakayama, Nobuo; Matsumoto, Hitoshi; Yamaguchi, Kazufumi Japanese Journal of Applied Physics, Vol. 15, Issue 11 https://doi.org/10.1143/JJAP.15.2281	journal	November 1976
Comprehensive Handbook of Chemical Bond Energies Luo, Yu-Ran https://doi.org/10.1201/9781420007282	book	March 2007
Copper Extraction from Chloride Solutions by Evaporation and Reduction with Hydrogen Kekesi, Tamas; Mimura, Kouji; Isshiki, Minoru Materials Transactions, JIM, Vol. 36, Issue 5 https://doi.org/10.2320/matertrans1989.36.649	journal	January 1995
In Situ Recrystallization of Co-Evaporated Cu(In,Ga)Se2 Thin Films by Copper Chloride Vapor Treatment towards Solar Cell Applications Poudel, Deewakar; Belfore, Benjamin; Ashrafee, Tasnuva Energies, Vol. 14, Issue 13 https://doi.org/10.3390/en14133938	journal	July 2021
Analysis of Post-Deposition Recrystallization Processing via Indium Bromide of Cu(In,Ga)Se2 Thin Films Poudel, Deewakar; Belfore, Benjamin; Ashrafee, Tasnuva Materials, Vol. 14, Issue 13 https://doi.org/10.3390/ma14133596	journal	June 2021
Studies on the Vapor Phase Reaction in the System In-Cl₂ Kuniya, Yasuo; Hosoda, Shozo; Hosaka, Masahiro Denki Kagaku oyobi Kogyo Butsuri Kagaku, Vol. 42, Issue 1 https://doi.org/10.5796/kogyobutsurikagaku.42.20	journal	January 1974
Studies on the Vapor Phase Reaction in the System Ga-Cl₂ Kuniya, Yasuo; Hosaka, Masahiro; Shindo, Isamu Denki Kagaku oyobi Kogyo Butsuri Kagaku, Vol. 43, Issue 7 https://doi.org/10.5796/kogyobutsurikagaku.43.372	journal	January 1975

Similar Records

Ex-Situ Recrystallization of CIGS via Metal Halides

Journal Article · Sat Jun 13 20:00:00 EDT 2020 · Conference Record of the IEEE Photovoltaic Specialists Conference · OSTI ID:1991341

Post-growth Recrystallization by Halides for High Throughput CIGS Photovoltaics

Technical Report · Fri Mar 31 00:00:00 EDT 2023 · OSTI ID:2217674

Related Subjects

14 SOLAR ENERGY

A thermodynamic evaluation of metal halides for the recrystallization of Cu(In,Ga)Se2

Citation Formats

References (55)

Similar Records

Related Subjects

A thermodynamic evaluation of metal halides for the recrystallization of Cu(In,Ga)Se₂