Halász Gábor J, Csehi András, Vibók Ágnes, Cederbaum Lorenz S
Department of Information Technology, University of Debrecen , P.O. Box 12, H-4010 Debrecen, Hungary.
J Phys Chem A. 2014 Dec 26;118(51):11908-15. doi: 10.1021/jp504889e. Epub 2014 Jun 26.
Previous works have shown that dressing of diatomic molecules by standing or by running laser waves gives rise to the appearance of so-called light-induced conical intersections (LICIs). Because of the strong nonadiabatic couplings, the existence of such LICIs may significantly change the dynamical properties of a molecular system. In our former paper (J. Phys. Chem. A 2013, 117, 8528), the photodissociation dynamics of the D(2)(+) molecule were studied in the LICI framework starting the initial vibrational nuclear wave packet from the superposition of all the vibrational states initially produced by ionizing D(2). The present work complements our previous investigation by letting the initial nuclear wave packets start from different individual vibrational levels of D(2)(+), in particular, above the energy of the LICI. The kinetic energy release spectra, the total dissociation probabilities, and the angular distributions of the photofragments are calculated and discussed. An interesting phenomenon has been found in the spectra of the photofragments. Applying the light-induced adiabatic picture supported by LICI, explanations are given for the unexpected structure of the spectra.
先前的研究表明,通过驻波或行波激光对双原子分子进行缀饰会导致所谓的光诱导锥形交叉点(LICIs)的出现。由于强烈的非绝热耦合,这种LICIs的存在可能会显著改变分子系统的动力学性质。在我们之前的论文(《物理化学杂志A》2013年,第117卷,第8528页)中,在LICI框架下研究了D(2)(+)分子的光解离动力学,初始振动核波包由电离D(2)最初产生的所有振动态的叠加开始。目前的工作通过让初始核波包从D(2)(+)的不同单个振动能级开始,特别是在LICI能量之上,对我们之前的研究进行了补充。计算并讨论了动能释放谱、总解离概率和光碎片的角分布。在光碎片的光谱中发现了一个有趣的现象。应用由LICI支持的光诱导绝热图像,对光谱中意外的结构给出了解释。