- Accepted Paper
Effect of organic molecular arrangement on carrier recombination in BF-doped CHNHPbI perovskite
Phys. Rev. B - Accepted 14 October, 2026
DOI: https://doi.org/10.1103/v39k-tbcf
Phys. Rev. B - Accepted 14 October, 2026
DOI: https://doi.org/10.1103/v39k-tbcf
Methylammonium lead iodide perovskite, CH3NH3PbI3 (MAPbI3), has attracted tremendous interest for its exceptional optoelectronic performance. However, the effect of MA arrangement on charge carrier recombination remains unclear. Here, BF4 doping is introduced to preserve distinguishable ferroelectric (FE) and antiferroelectric (AFE) MA configurations over the accessible simulation timescale, enabling a direct comparison of the influence of MA arrangement on carrier recombination. Using time-domain density functional theory and ab initio nonadiabatic molecular dynamics, we demonstrate that the nonradiative recombination in BF4-doped MAPbI3 perovskite with an AFE MA arrangement (BF4-AFE) decelerates an order of magnitude when compared with that in FE structure. The strong spatial variation of the built-in electric field in AFE structure introduces the effective charge separation. The strong electrostatic repulsion between adjacent MA molecules in BF4-AFE structure weakens MA-related atomic fluctuations, which strongly suppresses the high-frequency electron-vibration interaction. These effects in a short pure dephasing time and a weak nonadiabatic coupling in BF4-AFE structure, finally revealing its long carrier lifetime. This work provides mechanistic insight into how MA molecular arrangement influences carrier recombination in MAPbI3.
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