TY - JOUR
T1 - Multi-scale model for the structure of hybrid perovskites
T2 - Analysis of charge migration in disordered MAPbI3 structures
AU - Järvi, Jari
AU - Li, Jingrui
AU - Rinke, Patrick
PY - 2018/10/10
Y1 - 2018/10/10
N2 - 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 (CH3NH3PbI3, or MAPbI3). 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 MAPbI3 with density-functional theory. We investigated the charge mobility in various MAPbI3 supercell models of ordered and disordered MA+ cations. Our results indicate a structure-dependent mobility, in the range of 50-66 cm2 V-1 s-1, with the highest observed in the ordered tetragonal phase.
AB - 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 (CH3NH3PbI3, or MAPbI3). 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 MAPbI3 with density-functional theory. We investigated the charge mobility in various MAPbI3 supercell models of ordered and disordered MA+ cations. Our results indicate a structure-dependent mobility, in the range of 50-66 cm2 V-1 s-1, with the highest observed in the ordered tetragonal phase.
KW - charge mobility
KW - DFT
KW - hybrid perovskites
KW - multi-scale modeling
KW - photovoltaics
KW - solar cells
UR - http://www.scopus.com/inward/record.url?scp=85056001090&partnerID=8YFLogxK
U2 - 10.1088/1367-2630/aae295
DO - 10.1088/1367-2630/aae295
M3 - Article
AN - SCOPUS:85056001090
VL - 20
SP - 1
EP - 19
JO - New Journal of Physics
JF - New Journal of Physics
SN - 1367-2630
IS - 10
M1 - 103013
ER -