极化子
量子退相干
钙钛矿(结构)
激发态
化学物理
载流子
凝聚态物理
电子
物理
分子物理学
量子
化学
材料科学
原子物理学
量子力学
结晶学
标识
DOI:10.1021/acs.jpclett.2c02211
摘要
We conducted ab initio molecular dynamics (AIMD) and nonadiabatic MD to simulate polaron formation and recombination in all-inorganic Cs3Bi2Br9 perovskite. The meticulously designed AIMD simulations show that two types of small hole polaron, including localized and semidelocalized small hole polaron on either an intralayer or an interlayer Br dimer, are adiabatically formed within 1.71 ps. The localized small hole polaron reduces nonadiabatic coupling and decoherence time and, thus, delays charge recombination to 213 ns. In contrast, the dominant semidelocalized polaron increases nonadiabatic coupling by enhancing electron–hole overlap and restores the energy gap and decoherence time to the pristine system, accelerating recombination to 4.7 ns compared to a 10 ns charge carrier lifetime in the pristine system. All the obtained time scales agree well with experiments. The study offers a fundamental understanding of the excited-state dynamics of small hole polaron in Cs3Bi2Br9 and helps to design high-performance perovskite optoelectronics and photovoltaics.
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