3D-to-2D Transition of Anion Vacancy Mobility in CsPbBr3under Hydrostatic Pressure

Thijs J.A.M. Smolders, Alison B. Walker, Matthew J. Wolf

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Anion vacancy migration in the orthorhombic Pnma phase of the lead-halide perovskite CsPbBr3 under hydrostatic pressure is studied computationally. Density functional theory calculations are used to determine transition states, activation enthalpies, and attempt frequencies for vacancies to hop between nearby lattice sites, under pressure in the range 0.0-2.0 GPa. The resulting data are used to parametrize a kinetic model of vacancy migration under the influence of an electric field, which is solved in the steady state to determine the anion vacancy mobility tensor as a function of pressure. It is found that the mobility tensor becomes increasingly anisotropic with increasing pressure, such that at 2.0 GPa, the mobility within the (010) lattice plane is 3 orders of magnitude greater than the mobility normal to it. The results demonstrate the potentially significant influence of pressure, and by extension, other forms of stress, on defect migration in lead-halide perovskites.

Original languageEnglish
Pages (from-to)5169-5177
Number of pages9
JournalJournal of Physical Chemistry Letters
Issue number21
Early online date25 May 2021
Publication statusPublished - 3 Jun 2021

Bibliographical note

Funding Information:
We acknowledge funding from the European Union’s Horizon 2020 MSCA Innovative Training Network MAESTRO under grant agreement number 764787, and the Energy Oriented Centre of Excellence (EoCoE-II), grant agreement number 824158. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath and the Isambard UK National Tier-2 HPC Service ( http://gw4.ac.uk/isambard/ ) operated by GW4 and the UK Meteorological Office and funded by the EPSRC (EP/P020224/1). We thank Dr. I. R. Thompson and Dr. W. R. Saunders for discussions pertaining to kinetic modelling and Dr. T. Duchoň, Dr. J. Kullgren, Prof. R. A. De Souza and the anonymous reviewers for their constructive criticism of the manuscript.

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry


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