Organohalide lead-perovskites have revolutionized the hybrid/organic photovoltaics landscape. Further advances in the perovskite solar cells field may be boosted by computational design and screening of new materials, with researchers examining material characteristics that can improve device performance and/or stability. Suitable modeling strategies may allow researchers to observe the otherwise inaccessible but crucial hetero-interfaces that control device operation, allowing researchers to develop new and more efficient materials and devices. We illustrate the results of ab initio molecular dynamics simulations coupled to electronic structure calculations on the interplay of nuclear dynamics and electronic properties in the prototypical MAPbI3 and related perovskites. A possible polaronic mechanism, triggered by a photoinduced structural deformation, is presented which may be responsible for the reduced electron/hole recombination observed in organohalide perovskites.
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