Functional Mode Hot Electron Transfer Theory
Functional Mode Hot Electron Transfer Theory
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功能模式热电子转移理论
DOI：
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发表时间：
2016
期刊：
影响因子：
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通讯作者：
Hanning Chen
中科院分区：
文献类型：
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作者：
J. Elenewski;J. Cai;Wei Jiang;Hanning Chen
由于过高的振动能而使载流子脱离热平衡的载流子被称为热载流子。通过显式地解释电子转移驱动振动模式的随时间变化的热弛豫，发展了一种理论来模拟这些被振动激发的电子的注入，正如用泛函模式分析所确定的那样。具体地说，首先通过所谓的冻结声子方法确定驱动模式的热弛豫率，然后在费米黄金法则的框架内重新考虑依赖能量的线形函数，以包括对振动量子的记忆效应。通过对结合在锐钛矿型二氧化钛[101]表面的6-甲基偶氮烯-2-羧酸染料分子的数值模拟，我们的新理论不仅产生了持续较快的电子注入速率和较高的入射光子能量，而且当光激发染料分子的振动量发生变化时，电子注入速率急剧增加。
Charge carriers that have been driven out of thermal equilibrium by their excessive vibrational energies are termed hot carriers. A theory has been developed to model the injection of these vibrationally excited electrons by explicitly accounting for the time-dependent thermal relaxation of the electron-transfer driving vibrational mode, as ascertained using functional mode analysis. Specifically, the thermal relaxation rate of the driving mode is first determined through the so-called frozen-phonon approach after which the energy-dependent line shape function is revisited to include memory effects for the vibrational quanta within the framework of Fermi’s golden rule. As shown by the numerical simulations of a 6-methyl-azulene-2-carboxylic acid dye molecule bound to an anatase TiO2[101] surface, our new theory not only yields persistently faster electron injection rates with higher incident photon energy but also exhibits a sharp increase when the vibrational quanta of the photoexcited dye molecule chang...
影响因子：
6.3
作者：
Li, Wu;Carrete, Jesus;Mingo, Natalio
通讯作者：
Mingo, Natalio