论文标题

在CO/PD的内部拉伸模式下,异常的瞬态蓝光(111)

Anomalous transient blueshift in the internal stretch mode of CO/Pd(111)

论文作者

Bombín, Raúl, Muzas, Alberto S., Novko, Dino, Juaristi, J. Iñaki, Alducin, Maite

论文摘要

在时间分辨的泵浦探针振动光谱中,极性分子的内部拉伸模式可用于表征表面上吸附物的超快动力学。吸附物非绝热互层耦合是观察到的瞬态频率移动背后的常见机制。在这里,我们研究了CO/PD(111)系统,该系统具有可靠的理论框架,其中包括电子孔对激发和振动模式之间的电子介导的耦合。揭示了一种机制,该机制筛选了电子 - 光子相互作用,并在超快的非平衡条件下起源于蓝光。结果是根据费米级别附近状态密度的突然变化来解释的,并且有助于理解涉及本地化和标准$ S $或$ p $州的多组分表面的动态。

In time-resolved pump-probe vibrational spectroscopy the internal stretch mode of polar molecules is utilized as a key observable to characterize the ultrafast dynamics of adsorbates on surfaces. The adsorbates non-adiabatic intermode couplings are the commonly accepted mechanisms behind the observed transient frequency shifts. Here, we study the CO/Pd(111) system with a robust theoretical framework that includes electron-hole pair excitations and electron-mediated coupling between the vibrational modes. A mechanism is revealed that screens the electron-phonon interaction and originates a blueshift under ultrafast non-equilibrium conditions. The results are explained in terms of the abrupt change in the density of states around the Fermi level, and are instrumental for understanding dynamics at multi-component surfaces involving localized and standard $s$ or $p$ states.

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