Reference : Defect Formation and Healing at Grain Boundaries in Lead-Halide Perovskites
Scientific journals : Article
Engineering, computing & technology : Materials science & engineering
Physics and Materials Science
http://hdl.handle.net/10993/52763
Defect Formation and Healing at Grain Boundaries in Lead-Halide Perovskites
English
Kaiser, Waldemar mailto [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 mailto [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 mailto [University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS) >]
Alothman, Asma A. mailto [Chemistry Department, College of Science, King Saud University, Riyadh 1451, Kingdom of Saudi Arabia]
Meggiolaro, Daniele mailto [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 mailto [Department of Electrical and Computer Engineering, Technical University of Munich, Hans-Piloty-Straße 1, 85748 Garching, Germany]
Mosconi, Edoardo mailto [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 mailto [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]
11-Nov-2022
Journal of Materials Chemistry A
Royal Society of Chemistry
Yes
International
2050-7496
[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.
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
Researchers ; Professionals ; Students
http://hdl.handle.net/10993/52763
10.1039/D2TA06336K
https://doi.org/10.1039/D2TA06336K
NA

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