期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c04958
关键词
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资金
- Institute of Applied Radiation Chemistry of the Lodz University of Technology
- JSPS KAKENHI [19K05395]
Using high-precision simulation calculations and a semianalytical theory, this study resolves the controversy over the role of energetic disorder in geminate electron-hole photoseparation in organic solids. The results show that in efficient photovoltaic systems, the probability of charge-carrier separation decreases with increasing disorder, due to energy relaxation and deepening of the electron-hole Coulomb well. In inefficient systems, the separation probability initially decreases but shows an increasing trend at large disorder. The study also highlights the impact of mismatched electron and hole mobilities on geminate charge-pair separation probability, even in homogeneous systems.
Using high-precision simulation calculations and a semianalytical theory, we finally resolve the controversy over the role of energetic disorder in geminate electron-hole photoseparation in organic solids. We demonstrate that in efficient photovoltaic systems, where the charge-carrier separation probability is high, this probability decreases with increasing disorder, both in the absence and presence of a donor-acceptor heterojunction. This results from energy relaxation of the charged particles in the site energy distribution, which effectively deepens the electron-hole Coulomb well. In inefficient photovoltaic systems, the separation probability also initially decreases but turns into an increasing trend at large disorder. We also demonstrate that in the presence of disorder, the geminate charge-pair separation probability is affected by the mismatch between the electron and hole mobilities, even in homogeneous systems. We show how our theoretical results can be practically applied in an analysis of experimental data in organic photovoltaics.
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