Physics of grain boundaries in polycrystalline photovoltaic semiconductors

Yan, Yanfa; Yin, Wan-Jian; Wu, Yelong; Shi, Tingting; Paudel, Naba R.; Li, Chen; Poplawsky, Jonathan D.; Wang, Zhiwei; Moseley, John; Guthrey, Harvey; Moutinho, Helio; Pennycook, Stephen J.; Al-jassim, Mowafak

doi:10.1063/1.4913833

Physics of grain boundaries in polycrystalline photovoltaic semiconductors

Journal Article · Mon Mar 16 00:00:00 EDT 2015 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4913833· OSTI ID:1265414

Yan, Yanfa ^[1]; Yin, Wan-Jian ^[1]; Wu, Yelong ^[1]; Shi, Tingting ^[1]; Paudel, Naba R. ^[1]; Li, Chen ^[2]; Poplawsky, Jonathan D. ^[3]; Wang, Zhiwei ^[4]; Moseley, John ^[5]; Guthrey, Harvey ^[5]; Moutinho, Helio ^[5]; Pennycook, Stephen J. ^[6]; Al-jassim, Mowafak ^[5]

Univ. of Toledo, OH (United States). Wright Center for Photovoltaics Innovation and Commercialization (PVIC)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Univ. of Toledo, OH (United States). Wright Center for Photovoltaics Innovation and Commercialization (PVIC) ; National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Tennessee, Knoxville, TN (United States)

Thin-film solar cells based on polycrystalline Cu(In,Ga)Se₂ (CIGS) and CdTe photovoltaic semiconductors have reached remarkable laboratory efficiencies. It is surprising that these thin-film polycrystalline solar cells can reach such high efficiencies despite containing a high density of grain boundaries (GBs), which would seem likely to be nonradiative recombination centers for photo-generated carriers. In this study, we review our atomistic theoretical understanding of the physics of grain boundaries in CIGS and CdTe absorbers. We show that intrinsic GBs with dislocation cores exhibit deep gap states in both CIGS and CdTe. Although, in each solar cell device, the GBs can be chemically modified to improve their photovoltaic properties. In CIGS cells, GBs are found to be Cu-rich and contain O impurities. Density-functional theory calculations reveal that such chemical changes within GBs can remove most of the unwanted gap states. In CdTe cells, GBs are found to contain a high concentration of Cl atoms. Cl atoms donate electrons, creating n-type GBs between p-type CdTe grains, forming local p-n-p junctions along GBs. This leads to enhanced current collections. In conclusion, chemical modification of GBs allows for high efficiency polycrystalline CIGS and CdTe thin-film solar cells.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1265414

Alternate ID(s):: OSTI ID: 1220744
OSTI ID: 22399288

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 11 Vol. 117; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (39)

Effects of Sodium on Polycrystalline Cu(In,Ga)Se2 and Its Solar Cell Performance Kronik, Leeor.; Cahen, David; Schock, Hans Werner Advanced Materials, Vol. 10, Issue 1 https://doi.org/10.1002/(SICI)1521-4095(199801)10:1<31::AID-ADMA31>3.0.CO;2-3	journal	January 1998
Understanding the Beneficial Role of Grain Boundaries in Polycrystalline Solar Cells from Single-Grain-Boundary Scanning Probe Microscopy Visoly-Fisher, I.; Cohen, S. R.; Gartsman, K. Advanced Functional Materials, Vol. 16, Issue 5 https://doi.org/10.1002/adfm.200500396	journal	March 2006
How Polycrystalline Devices Can Outperform Single-Crystal Ones: Thin Film CdTe/CdS Solar Cells Visoly-Fisher, I.; Cohen, S. R.; Ruzin, A. Advanced Materials, Vol. 16, Issue 11 https://doi.org/10.1002/adma.200306624	journal	June 2004
Confined and Chemically Flexible Grain Boundaries in Polycrystalline Compound Semiconductors Abou-Ras, Daniel; Schmidt, Sebastian S.; Caballero, Raquel Advanced Energy Materials, Vol. 2, Issue 8 https://doi.org/10.1002/aenm.201100764	journal	May 2012
Engineering Grain Boundaries in Cu ₂ ZnSnSe ₄ for Better Cell Performance: A First-Principle Study Yin, Wan-Jian; Wu, Yelong; Wei, Su-Huai Advanced Energy Materials, Vol. 4, Issue 1 https://doi.org/10.1002/aenm.201300712	journal	August 2013
Direct Imaging of Cl- and Cu-Induced Short-Circuit Efficiency Changes in CdTe Solar Cells Poplawsky, Jonathan D.; Paudel, Naba R.; Li, Chen Advanced Energy Materials, Vol. 4, Issue 15 https://doi.org/10.1002/aenm.201400454	journal	May 2014
The electronic structure of chalcopyrites-bands, point defects and grain boundaries Siebentritt, Susanne; Igalson, Malgorzata; Persson, Clas Progress in Photovoltaics: Research and Applications, Vol. 18, Issue 6 https://doi.org/10.1002/pip.936	journal	August 2010
Grain boundaries in Cu(In, Ga)(Se, S)2 thin-film solar cells Rau, Uwe; Taretto, Kurt; Siebentritt, Susanne Applied Physics A, Vol. 96, Issue 1 https://doi.org/10.1007/s00339-008-4978-0	journal	December 2008
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
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Processing options for CdTe thin film solar cells McCandless, Brian E.; Dobson, Kevin D. Solar Energy, Vol. 77, Issue 6 https://doi.org/10.1016/j.solener.2004.04.012	journal	December 2004
CdTe thin film solar cells: device and technology issues Ferekides, C. S.; Balasubramanian, U.; Mamazza, R. Solar Energy, Vol. 77, Issue 6 https://doi.org/10.1016/j.solener.2004.05.023	journal	December 2004
From atomic structure to photovoltaic properties in CdTe solar cells Li, Chen; Poplawsky, Jonathan; Wu, Yelong Ultramicroscopy, Vol. 134 https://doi.org/10.1016/j.ultramic.2013.06.010	journal	November 2013
Defect chemical explanation for the effect of air anneal on CdS/CuInSe ₂ solar cell performance Cahen, David; Noufi, Rommel Applied Physics Letters, Vol. 54, Issue 6 https://doi.org/10.1063/1.100930	journal	February 1989
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
High-efficiency solar cells on edge-defined film-fed grown (18.2%) and string ribbon (17.8%) silicon by rapid thermal processing Rohatgi, A.; Kim, D. S.; Nakayashiki, K. Applied Physics Letters, Vol. 84, Issue 1 https://doi.org/10.1063/1.1638636	journal	January 2004
Passivation of double-positioning twin boundaries in CdTe Yan, Yanfa; Al-Jassim, M. M.; Jones, K. M. Journal of Applied Physics, Vol. 96, Issue 1 https://doi.org/10.1063/1.1758313	journal	July 2004
The impact of charged grain boundaries on thin-film solar cells and characterization Metzger, W. K.; Gloeckler, M. Journal of Applied Physics, Vol. 98, Issue 6 https://doi.org/10.1063/1.2042530	journal	September 2005
Compositionally induced valence-band offset at the grain boundary of polycrystalline chalcopyrites creates a hole barrier Persson, Clas; Zunger, Alex Applied Physics Letters, Vol. 87, Issue 21 https://doi.org/10.1063/1.2132537	journal	November 2005
Grain-boundary recombination in Cu(In,Ga)Se2 solar cells Gloeckler, Markus; Sites, James R.; Metzger, Wyatt K. Journal of Applied Physics, Vol. 98, Issue 11 https://doi.org/10.1063/1.2133906	journal	December 2005
The electrical properties of polycrystalline silicon films Seto, John Y. W. Journal of Applied Physics, Vol. 46, Issue 12 https://doi.org/10.1063/1.321593	journal	December 1975
Defect segregation at grain boundary and its impact on photovoltaic performance of CuInSe ₂ Yin, Wan-Jian; Wu, Yelong; Noufi, Rommel Applied Physics Letters, Vol. 102, Issue 19 https://doi.org/10.1063/1.4804606	journal	May 2013
Accurate and simple analytic representation of the electron-gas correlation energy Perdew, John P.; Wang, Yue Physical Review B, Vol. 45, Issue 23, p. 13244-13249 https://doi.org/10.1103/PhysRevB.45.13244	journal	June 1992
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Defect-induced nonpolar-to-polar transition at the surface of chalcopyrite semiconductors Jaffe, John; Zunger, Alex Physical Review B, Vol. 64, Issue 24 https://doi.org/10.1103/PhysRevB.64.241304	journal	November 2001
Reconstruction and energetics of the polar (112) and ( 1 ¯ 1 ¯ 2 ¯ ) versus the nonpolar (220) surfaces of CuInSe 2 Zhang, S. B.; Wei, S. -H. Physical Review B, Vol. 65, Issue 8 https://doi.org/10.1103/PhysRevB.65.081402	journal	February 2002
Effect of hydrogen passivation on the electronic structure of ionic semiconductor nanostructures Deng, Hui-Xiong; Li, Shu-Shen; Li, Jingbo Physical Review B, Vol. 85, Issue 19 https://doi.org/10.1103/PhysRevB.85.195328	journal	May 2012
Effect of Copassivation of Cl and Cu on CdTe Grain Boundaries Zhang, Lixin; Da Silva, Juarez L. F.; Li, Jingbo Physical Review Letters, Vol. 101, Issue 15 https://doi.org/10.1103/PhysRevLett.101.155501	journal	October 2008
Large Neutral Barrier at Grain Boundaries in Chalcopyrite Thin Films Hafemeister, Michael; Siebentritt, Susanne; Albert, Jürgen Physical Review Letters, Vol. 104, Issue 19 https://doi.org/10.1103/PhysRevLett.104.196602	journal	May 2010
Direct Insight into Grain Boundary Reconstruction in Polycrystalline Cu ( In , Ga ) Se 2 with Atomic Resolution Abou-Ras, Daniel; Schaffer, Bernhard; Schaffer, Miroslava Physical Review Letters, Vol. 108, Issue 7 https://doi.org/10.1103/PhysRevLett.108.075502	journal	February 2012
Electrostatic Potentials at Cu(In,Ga) Se 2 Grain Boundaries: Experiment and Simulations Schmidt, Sebastian S.; Abou-Ras, Daniel; Sadewasser, Sascha Physical Review Letters, Vol. 109, Issue 9 https://doi.org/10.1103/PhysRevLett.109.095506	journal	August 2012
Carrier Separation at Dislocation Pairs in CdTe Li, Chen; Wu, Yelong; Pennycook, Timothy J. Physical Review Letters, Vol. 111, Issue 9 https://doi.org/10.1103/PhysRevLett.111.096403	journal	August 2013
Grain-Boundary-Enhanced Carrier Collection in CdTe Solar Cells Li, Chen; Wu, Yelong; Poplawsky, Jonathan Physical Review Letters, Vol. 112, Issue 15 https://doi.org/10.1103/PhysRevLett.112.156103	journal	April 2014
Anomalous Grain Boundary Physics in Polycrystalline C u I n S e 2 : The Existence of a Hole Barrier Persson, Clas; Zunger, Alex Physical Review Letters, Vol. 91, Issue 26 https://doi.org/10.1103/PhysRevLett.91.266401	journal	December 2003
Grain-Boundary Physics in Polycrystalline CuInSe 2 Revisited: Experiment and Theory Yan, Yanfa; Noufi, R.; Al-Jassim, M. M. Physical Review Letters, Vol. 96, Issue 20 https://doi.org/10.1103/PhysRevLett.96.205501	journal	May 2006
Evidence for a Neutral Grain-Boundary Barrier in Chalcopyrites Siebentritt, Susanne; Sadewasser, Sascha; Wimmer, Mark Physical Review Letters, Vol. 97, Issue 14 https://doi.org/10.1103/PhysRevLett.97.146601	journal	October 2006
Electrically Benign Behavior of Grain Boundaries in Polycrystalline CuInSe 2 Films Yan, Yanfa; Jiang, C. -S.; Noufi, R. Physical Review Letters, Vol. 99, Issue 23 https://doi.org/10.1103/PhysRevLett.99.235504	journal	December 2007

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