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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Instantaneous and Permanent Photoionization
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Instantaneous and Permanent Photoionization

机译：瞬时和永久光电离

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The bimolecular ionization of photoexcited molecules is theoretically investigated assuming the light pumping of moderate intensity is either instantaneous or permanent. The kinetics of energy quenching and ion-radical accumulation and recombination after O-pulse excitation are studied beyond the rate concept, in the framework of Integral Encounter Theory (IET). The results are compared with those obtained within extended Unified Theory (UT), contact and Markovian approximations, and a widely accepted exponential model. When there is a shortage of acceptors the theory becomes nonlinear and discloses the striking effect of electron-transfer saturation. In such conditions and under permanent illumination lET is the sole formalism appropriate for a full time-scale (non-Markovian) description of system relaxation. The original program for solving nonlinear lET equations for particle concentrations was developed and first used to calculate the kinetics of relaxation to equilibrium and to a stationary regime. The non-Markovian corrections to the quantum yields of fluorescence and charge separation obtained numerically are in good correspondence with analytic estimates of these quantities.
机译：从理论上研究光激发分子的双分子电离，假设中等强度的光泵浦是瞬时的或永久的。在积分相遇理论（IET）的框架下，研究了速率概念之外的O脉冲激发后的能量猝灭和离子自由基累积与重组的动力学。将结果与在扩展统一理论（UT），接触和马尔可夫近似以及广泛接受的指数模型中获得的结果进行比较。当受体短缺时，该理论变成非线性并揭示了电子转移饱和的惊人效应。在这种情况下，在永久照明下，lET是适用于系统松弛的完整时间尺度（非马尔可夫式）描述的唯一形式主义。开发了用于求解颗粒浓度非线性lET方程的原始程序，该程序首先用于计算从松弛到平衡和稳态的动力学。通过数值获得的荧光和电荷分离的量子产率的非马尔可夫校正与这些量的解析估计非常吻合。

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