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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Time-Resolved Observation of the Solvation Dynamics of a Rydberg Excited Molecule Deposited on an Argon Cluster. II. DABCO at Long Time Delays
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Time-Resolved Observation of the Solvation Dynamics of a Rydberg Excited Molecule Deposited on an Argon Cluster. II. DABCO at Long Time Delays

机译：沉积在氩簇上的rydberg激发分子的溶剂化动力学的时间分辨观察。 II。 Dabco长时间延迟

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The real-time dynamics of DABCO-argon clusters is investigated in a femtosecond pump-probe experiment where the pump excites DABCO to the S-1 state within the argon cluster. The probe operates by photoionization and documents the energy and angular distributions of the resulting photoelectrons. The present work complements a previous work from our group [Awali et al. Phys. Chem. Chem. Phys., 2014, 16, 516-526] where this dynamics was probed at short time, up to 4 ps after the pump pulse. Here, the dynamics is followed up to 500 ps. A multiscale dynamics is observed. It includes a jump between two solvation sites (time scale 0.27 ps) followed by the relaxation of the solvation cage excess vibrational energy (time scale 14 ps) and then by that of DABCO (time scale >150 ps). Polarization anisotropy, double polarization, and angular anisotropy effects are reported also. They are interpreted (quantitatively for the former effect) in terms of decoherence of rotational alignment, driven by the overall rotation of the DABCO-argon clusters. A tomographic view of the DABCO excited orbital, provided by the double anisotropy effect, is discussed on a qualitative basis.
机译：在飞秒泵浦-探测实验中研究了DABCO氩团簇的实时动力学，其中泵浦将DABCO激发到氩团簇内的S-1态。探测器通过光电离作用，记录产生的光电子的能量和角分布。目前的工作补充了我们小组之前的工作[Awali et al.Phys.Chem.Chem.Phys.，2014，16516-526]，在短时间内，在泵脉冲后高达4ps的时间内，对这种动力学进行了探测。在这里，动态跟踪到500 ps。观察到多尺度动态。它包括两个溶剂化位点之间的跃迁（时间标度0.27 ps），然后是溶剂化笼过剩振动能的弛豫（时间标度14 ps），然后是DABCO的弛豫（时间标度>150 ps）。还报道了极化各向异性、双极化和角各向异性效应。根据DABCO氩团簇的整体旋转驱动的旋转排列退相干，对它们进行了解释（前者的影响是定量的）。在定性的基础上讨论了由双各向异性效应提供的DABCO激发轨道的层析图。

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