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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Experimental exploration of the Mulliken-Hush relationship for intramolecular electron transfer reactions
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Experimental exploration of the Mulliken-Hush relationship for intramolecular electron transfer reactions

机译：分子内电子转移反应的Mulliken-Hush关系的实验探索

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摘要

The Mulliken-Hush (M-H) relationship provides the critical link between optical and thermal electron transfer processes, and yet very little direct experimental support for its applicability has been provided. Dicyanovinylazaadamantane (DCVA) represents a simple two-state (neutral/charge-transfer) intramolecular electron transfer system that exhibits charge-transfer absorption and emission spectra that are readily measurable in solvents with a wide range of polarities. In this regard it represents an ideal model system for studying the factors that control both optical charge separation (absorption) and recombination (emission) processes in solution. Here we explore the applicability of the M-H relation to quantitative descriptions of the optical charge-transfer processes in DCVA. For DCVA, the measured radiative rate constants exhibit a linear dependence on transition energy, and transition dipole moments exhibit an inverse dependence on transition energy, consistent with the M-H relationship.
机译：Mulliken-Hush（M-H）关系提供了光电子转移过程和热电子转移过程之间的关键联系，但几乎没有为其应用提供直接的实验支持。双氰基乙烯基氮杂金刚烷（DCVA）代表一种简单的两态（中性/电荷转移）分子内电子转移系统，该系统具有电荷转移吸收和发射光谱，可在具有广泛极性的溶剂中轻松测量。在这方面，它代表了一个理想的模型系统，用于研究溶液中控制光电荷分离（吸收）和重组（发射）过程的因素。在这里，我们探讨了M-H关系对DCVA中光学电荷转移过程的定量描述的适用性。对于DCVA，测得的辐射速率常数与跃迁能量呈线性关系，跃迁偶极矩与跃迁能量呈反相关关系，与M-H关系一致。

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