Studies of chemical reactivity in the condensed phase. IV. Density dependent molecular dynamics simulations of vibrational relaxation in simple liquids
Studies of chemical reactivity in the condensed phase. IV. Density dependent molecular dynamics simulations of vibrational relaxation in simple liquids
复制标题
凝聚相化学反应性的研究。
DOI：
10.1063/1.455341
复制
发表时间：
1988
影响因子：
4.4
通讯作者：
J. Tully
中科院分区：
文献类型：
--
作者：
J. K. Brown;C. Harris;J. Tully
本文报道了几种密度下碘在液体氙气中的光解/复合过程的分子动力学模拟。进行这些模拟是为了帮助理解和解释最近对模型化学反应系统进行的皮秒实验研究。从这些计算中发现，在所有考虑的密度下，双子复合主要发生在几皮秒内。这与以前用小得多的系统进行的分子动力学模拟是一致的，也与目前对实验结果的解释是一致的。模拟的碘基态电子振动弛豫时间从最低密度下的约1 ns到最高密度下的约250ps不等。此外，观察到平均碘振动能衰变的泛函形式几乎与密度无关。用简单的气相隔离二元碰撞模型对这一结果进行了讨论。..。
Molecular dynamics simulations of the photodissociation/recombination process for iodine in liquid xenon at several densities are reported in this paper. These simulations were performed to aid in the understanding and interpretation of recent picosecond experimental investigations on model chemical reaction systems. From these calculations, it was found that geminate recombination occurs primarily within a few picoseconds at all densities considered. This is in agreement with previous molecular dynamics simulations with significantly smaller systems, and with the current interpretation of experimental results. Simulated iodine ground electronic state vibrational relaxation times range from about 1 ns at the lowest density to approximately 250 ps at the highest density reported here. In addition, the functional form of the decay of the average iodine vibrational energy was observed to be nearly independent of density. This result is discussed in terms of simple gas phase isolated binary collision models. ...