Article (Scientific journals)
Defect Formation and Healing at Grain Boundaries in Lead-Halide Perovskites
Kaiser, Waldemar; Hussain, Kashif; Singh, Ajay et al.
2022In Journal of Materials Chemistry A
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Abstract :
[en] Polycrystalline perovskite solar cells show high power conversion efficiencies despite the presence of grain boundaries (GBs). The benign nature of GBs on the electronic properties and structural stability in metal-halide perovskites contradicts their propensity for point defect formation, a controversy that is far from being understood. In this work, we combine ab initio molecular dynamics and density functional theory calculations on the S5[130] GB of cesium lead iodide, CsPbI3, to shed light on the structural and electronic properties of such GBs. Our results present the first evidence of structural healing of GBs driven by the facile migration of iodine ions, resulting in stabilized GB structures with reduced hole trap states and shallow electron trap states by strain-induced Pb–Pb dimers. Drift-diffusion simulations reveal that shallow electron trap states in GB mainly lower open-circuit voltage by enhanced non-radiative recombination. Finally, we observe the spontaneous formation of iodine Frenkel defects with reduced formation energies compared to the perovskite bulk. Overall, our study reveals a controversy of GBs showing a moderate impact on the electronic properties by structural healing but a detrimental impact on the point defect densities, both being connected to the facile migration of iodine ions in GBs.
Disciplines :
Materials science & engineering
Author, co-author :
Kaiser, Waldemar;  Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO) > Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, Perugiav 06123, Italy
Hussain, Kashif;  Department of Electrical and Computer Engineering, Technical University of Munich, Hans-Piloty-Straße 1, 85748 Garching, Germany ; Department of Electrical Engineering, Sukkur IBA University, Sukkur 65200, Pakistan
Singh, Ajay ;  University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS)
Alothman, Asma A.;  Chemistry Department, College of Science, King Saud University, Riyadh 1451, Kingdom of Saudi Arabia
Meggiolaro, Daniele;  Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO) > Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, Perugiav 06123, Italy
Gagliardi, Alessio;  Department of Electrical and Computer Engineering, Technical University of Munich, Hans-Piloty-Straße 1, 85748 Garching, Germany
Mosconi, Edoardo;  Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO) > Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, Perugiav 06123, Italy ; Chemistry Department, College of Science, King Saud University, Riyadh 1451, Kingdom of Saudi Arabia
De Angelis, Filippo;  Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO) > Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, Perugiav 06123, Italy ; Department of Chemistry, Biology and Biotechnology, University of Perugia and UdR INSTM, Via Elce di Sotto 8, Perugia 06123, Italy
External co-authors :
yes
Language :
English
Title :
Defect Formation and Healing at Grain Boundaries in Lead-Halide Perovskites
Publication date :
11 November 2022
Journal title :
Journal of Materials Chemistry A
ISSN :
2050-7496
Publisher :
Royal Society of Chemistry
Peer reviewed :
Peer Reviewed verified by ORBi
Focus Area :
Physics and Materials Science
Funders :
Deutsche Forschungsgemeinschaft: Germany's Excellence Strategy/EXC 2089/1 – 390, TUM Innovation Network for Artificial Intelligence
King Saud University Saudi Arabia: Distinguished Scientist Fellowship Program
Ministero dell’Istruzione, dell’Universit` a e della Ricerca Italy
Universit` a degli Studi di Perugia Italy
Horizon 20220 Framework Programme European Union: LION-HEARTED/828984
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