系统间交叉
钌
光化学
联轴节(管道)
自旋轨道相互作用
吸收(声学)
吸收光谱法
自旋(空气动力学)
化学
原子物理学
分子物理学
物理
材料科学
光学
量子力学
热力学
激发态
有机化学
催化作用
单重态
冶金
作者
Justin J. Talbot,Thomas P. Cheshire,Stephen J. Cotton,Frances A. Houle,Martin Head‐Gordon
标识
DOI:10.1021/acs.jpca.4c04122
摘要
The successful use of molecular dyes for solar energy conversion requires efficient charge injection, which in turn requires the formation of states with sufficiently long lifetimes (e.g., triplets). The molecular structure elements that confer this property can be found empirically, however computational predictions using ab initio electronic structure methods are invaluable to identify structure-property relations for dye sensitizers. The primary challenge for simulations to elucidate the electronic and nuclear origins of these properties is a spin-orbit interaction which drives transitions between electronic states. In this work, we present a computational analysis of the spin-orbit corrected linear absorption cross sections and intersystem crossing rate coefficients for a derivative set of phosphonated tris(2,2'-bipyridine)ruthenium(2+) dye molecules. After sampling the ground state vibrational distributions, the predicted linear absorption cross sections indicate that the mixture between singlet and triplet states plays a crucial role in defining the line shape of the metal-to-ligand charge transfer bands in these derivatives. Additionally, an analysis of the intersystem crossing rate coefficients suggests that transitions from the singlet into the triplet manifolds are ultrafast with rate coefficients on the order of 10
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