DataVXACS Energy LettersPaper
journal article·2018-04-13Open access

Density of States Broadening in CH3NH3PbI3 Hybrid Perovskites Understood from ab Initio Molecular Dynamics Simulations

Liujiang Zhou, Amanda J. Neukirch, Dayton J. Vogel, Dmitri S. Kilin, Laurent Pedesseau, Marcelo A. Carignano, Aditya D. Mohite, Jacky Even, Claudine Katan, Sergei Tretiak

ACS Energy Letters· Volume 3· Issue 4
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Source abstract

Abstract

Lead-halide perovskites are promising materials in optoelectronic devices for their unique properties including direct band gap, strong light absorption, high carrier mobility, and low fabrication cost. Here, by using ab inito molecular dynamics and electronic structure calculations, we report a systematic study on the broadening density of states (DOS) deep in the valence bands that has been experimentally observed but absent in static calculations. We quantify the broadening DOS reduction from the cubic phase to lower-temperature tetragonal and orthorhombic phases and attribute observed effects to the molecular vibrations and the anharmonicity of iodine atoms motion. Specifically, the MA cations’ vibrations are strongly linked to the moderate C–N stretch and CH3 bend, as well as the strong CH3 and NH3+ stretches. These results present a theoretical perspective on the structural dynamics in lead-halide perovskites which may be valuable for future studies toward desired functionalities in perovskite-based optoelectronic devices.
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Research context

Electronic materials

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Organic and Molecular Conductors Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Theoretical Division, Center for Nonlinear Studies and Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Department of Chemistry, University of South Dakota, Vermillion, South Dakota 57069, United States

Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United States

Univ Rennes, INSA Rennes, CNRS, Institut FOTON−UMR 6082, F-35000 Rennes, France

Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, Qatar Foundation, P.O. Box 34110, Doha, Qatar

Materials Physics and Application Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes)−UMR 6226, F-35000 Rennes, France

Funding

Centre National de la Recherche Scientifique · Laboratory Directed Research and Development · Universit? de Rennes 1

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