Jump to main content
Jump to site search

Issue 1, 2020
Previous Article Next Article

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

Author affiliations

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

Back to tab navigation

Supplementary files

Article information


Submitted
27 Aug 2019
Accepted
26 Nov 2019
First published
27 Nov 2019

Phys. Chem. Chem. Phys., 2020,22, 97-106
Article type
Paper

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, 22, 97
DOI: 10.1039/C9CP04739E

Social activity

Search articles by author

Spotlight

Advertisements