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Quantum mechanical molecular dynamics simulations of polaron formation in methylammonium lead iodide perovskite

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Abstract

We investigated the atomistic and dynamical mechanism of polaron formation in methylammonium lead iodide perovskite (MAPbI3), which is a representative perovskite solar cell absorber, through the quantum mechanical molecular dynamics simulations. The simulations were conducted on the spatial scale of several nanometres, which can describe charge localization and the associated structural deformation, using the divide-and-conquer-type density-functional tight-binding method, which enables a quantum chemical treatment of systems comprising thousands of atoms. We found that both the structural parts of MAPbI3, namely, the inorganic framework (PbI3) and the MA cations, involve the structural deformation associated with polaron formation. We elucidated that in the process of polaron formation, charge localization is invoked by thermal structural fluctuation, and a further structural deformation is caused by the relaxation of the charge carrier. Finally, importance of the two structural parts, PbI3 and MA, was examined from the energetical viewpoint.

Graphical abstract: Quantum mechanical molecular dynamics simulations of polaron formation in methylammonium lead iodide perovskite

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Publication details

The article was received on 27 Aug 2019, accepted on 26 Nov 2019 and first published on 27 Nov 2019


Article type: Paper
DOI: 10.1039/C9CP04739E
Phys. Chem. Chem. Phys., 2020, Advance Article

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    Quantum mechanical molecular dynamics simulations of polaron formation in methylammonium lead iodide perovskite

    H. Uratani, C. Chou and H. Nakai, Phys. Chem. Chem. Phys., 2020, Advance Article , DOI: 10.1039/C9CP04739E

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