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

Hiroki Uratani, Chien Pin Chou, Hiromi Nakai

Research output: Contribution to journalArticle

4 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)97-106
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume22
Issue number1
DOIs
Publication statusPublished - 2019

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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