期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 23, 期 10, 页码 6182-6189出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cp06629j
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资金
- Center for Solar Energy and Energy Storage at McKelvey School of Engineering at Washington University in Saint Louis
This study investigated the photophysical properties of two benchmark sensitizers used in dye-sensitized solar cells, providing detailed information on the excited MLCT states and their dynamics. Results showed that the excitation decay pathway involves rapid intersystem crossing to the triplet MLCT state, with the lifetime of the fully relaxed triplet MLCT strongly dependent on dye concentration, offering an explanation for inconsistencies seen in previous studies.
Two benchmark sensitizers used for dye-sensitized solar cells, ruthenium polypyridyl N719 and Z907 dyes were investigated with spectroscopic methods as steady-state absorption, time-gated phosphorescence and femto-/nanosecond time-resolved transient absorption at room temperature and at 160 K. Aim of this study was to perform comprehensive photophysical study of dye excited singlet and triplet metal-to-ligand charge transfer (MLCT) states including states lifetimes, dependency on temperature and dye concentration and obtain detailed information on the excitation decay pathway. Transient absorption and phosphorescence decay data provided a clearer picture of the dynamics of the excited MLCT states. Based on data analysis, the excitation decay pathway consists of rapid intersystem crossing to the triplet MLCT state that undergoes state solvation and vibrational relaxation. It was demonstrated that the lifetime of the fully relaxed triplet MLCT is also strongly dependent on dye concentration for both molecules, providing a viable explanation for a large inconsistency seen in previous studies.
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