Multi-scale model for the structure of hybrid perovskites: Analysis of charge migration in disordered MAPbI${}_3$ structures

Abstract

We have developed a multi-scale model for organic-inorganic hybrid perovskites (HPs) that applies quantum mechanical (QM) calculations of small HP supercell models to large coarse-grained structures. With a mixed quantum-classical hopping model, we have studied the effects of cation disorder on charge mobilities in HPs, which is a key feature to optimize their photovoltaic performance. Our multi-scale model parametrizes the interaction between neighboring methylammonium cations (MA${}^{+}$) in the prototypical HP material, methylammonium lead triiodide (CH${}_3$NH${}_3$PbI${}_3$, or MAPbI${}_3$). For the charge mobility analysis with our hopping model, we solved the QM site-to-site hopping probabilities analytically and computed the nearest-neighbor electronic coupling energies from the band structure of MAPbI${}_3$ with density-functional theory. We investigated the charge mobility in various MAPbI${}_3$ supercell models of ordered and disordered MA${}^{+}$ cations. Our results indicate a structure-dependent mobility, in the range of 50$-$66 cm${}^2$V${}^{-1}$s${}^{-1}$, with the highest observed in the ordered tetragonal phase.

arXiv comment28 pages, 13 figures

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Cited by in corpus (1)

• Long-range order imposed by short-range interactions in methylammonium lead iodide: Comparing point-dipole models to machine-learning force fields