Theoretical insights into hybrid perovskites for photovoltaic applications

Abstract

In this paper, we examine recent theoretical investigations on 3D hybrid perovskites (HOP) that combine concepts developed for classical bulk solid-state physics and empirical simulations of their optoelectronic properties. In fact, the complexity of HOP calls for a coherent global view that combines usually disconnected concepts. For the pseudocubic high temperature reference perovskite structure that plays a central role for 3D HOP, we introduce a new tight-binding Hamiltonian, which specifically includes spin-orbit coupling. The resultant electronic band structure is compared to that obtained using state of the art density functional theory (DFT). Next, recent experimental investigations of excitonic properties in HOP will be revisited within the scope of theoretical concepts already well implemented in the field of conventional semiconductors. Last, possible plastic crystal and orientational glass behaviors of HOP will be discussed, building on Car-Parrinello molecular dynamics simulations.