Molecular disorder and translation/rotation coupling in the plastic crystal phase of hybrid perovskites

Abstract

The complexity of hybrid organic perovskites calls for an innovative theoretical view that combines usually disconnected concepts in order to achieve a comprehensive picture: (i) the intended applications of this class of materials are currently in the realm of conventional semiconductors, which reveal the key desired properties for the design of efficient devices. (ii) The reorientational dynamics of the organic component resembles that observed in plastic crystals, therefore requiring a stochastic treatment that can be done in terms of pseudospins and rotator functions. (iii) The overall structural similarity with all inorganic perovskites suggests the use of the high temperature pseudo cubic phase as the reference platform on which further refinements can be built. In this paper we combine the existing knowledge on these three fields to define a general scenario based on which we can continue the quest towards a fundamental understanding of hybrid organic perovskites. With the introduction of group theory as the main tool to rationalize the different ideas and with the help of molecular dynamics simulations, several experimentally observed properties are naturally explained with possible suggestions for future work.