Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium

Ian M. Lane; David A. King; Zhi-Pan Liu; Heike Arnolds

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Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium

机译：非绝热表面动力学的实时观察：铱上NO离解的第一个皮秒

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Ultrafast laser pulses on Ir{111} cause a highly temperature-dependent redshift of the intramolecular stretch frequency of adsorbed NO. The time-resolved spectral changes are driven by charge transfer of hot electrons to the NO 2π~*d antibonding orbital, which leads to bending of NO and internal bond weakening. The nonadiabatic change in the NO adsorption geometry follows the charge transfer within a time scale of 700 femtoseconds. This geometrical change is the same as the mechanism predicted for thermally induced dissociation.

机译：Ir {111}上的超快激光脉冲引起吸附的NO的分子内拉伸频率高度依赖于温度的红移。时间分辨的光谱变化是由热电子向NO2π〜* d反键轨道的电荷转移驱动的，这导致NO的弯曲和内部键的减弱。 NO吸附几何形状的非绝热变化在700飞秒的时间范围内跟随电荷转移。这种几何变化与热诱导解离的预测机理相同。

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来源
《Physical review letters》 |2006年第18期|p.186105.1-186105.4|共4页
作者
Ian M. Lane; David A. King; Zhi-Pan Liu; Heike Arnolds;
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作者单位

Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom;

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正文语种 eng
中图分类物理学;
关键词
surface and interface dynamics and vibrations; time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter; electronically non-adiabatic reactions; femtochemistry of adsorbed molecules;

机译：表面和界面动力学和振动;时间分辨光学光谱学和凝聚态物质的其他超快光学测量;电子非绝热反应;吸附分子的光化学;

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Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium

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