Nonradiative deexcitation dynamics of 9H-adenine: An OM2 surface hopping study
Nonradiative deexcitation dynamics of 9H-adenine: An OM2 surface hopping study
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DOI：
10.1021/jp8033402
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发表时间：
2008-07-31
影响因子：
2.9
通讯作者：
Thiel, W.
中科院分区：
文献类型：
--
作者：
Fabiano, E.;Thiel, W.
使用表面跳跃方法在半经验 OM2/MR-CI 水平上研究了 9H-腺嘌呤的非辐射弛豫。进行了能量最小值和圆锥交点的几何优化以及关键点激发能的单点计算，以表征 9H-腺嘌呤的相关势能表面并评估 OM2 结果的准确性。进行表面跳跃计算来描述 9H-腺嘌呤在垂直激发到光学活性状态后的非辐射动力学。他们表明，去励磁过程主要由由超短分量和较长分量组成的两步弛豫控制。这些发现与时间分辨光电子能谱的实验结果非常吻合。
The nonradiative relaxation of 9H-adenine was studied at the semiempirical OM2/MR-CI level using the surface-hopping approach. Geometry optimizations of energy minima and conical intersections as well as single-point calculations of excitation energies at critical points were performed to characterize the relevant potential energy surfaces of 9H-adenine and to assess the accuracy of the OM2 results. Surface-hopping calculations were performed to describe the nonradiative dynamics of 9H-adenine after vertical excitation into the optically active state. They showed that the de-excitation process is mainly governed by a two-step relaxation consisting of an ultrashort component and a longer component. These findings compare well with experimental results from time-resolved photoelectron spectroscopy.