结构变异性在固液界面计算反射各向异性光谱时域分析中的相关性
The relevance of structural variability in the time-domain for computational reflection anisotropy spectroscopy at solid-liquid interfaces
AI总结：
本研究结合从头算分子动力学与计算光谱学，揭示Au(110)缺失行重构在水界面处反射各向异性光谱的时域演化，解释理论与实验强度差异，并强调结构变异性与RAS探测动态界面的潜力。
摘要：
在电化学中，反应和电荷转移在很大程度上由固液界面的原子结构决定。然而，由于液体电解质的存在，许多表面科学方法无法在此应用。因此，在操作条件下存在的确切微观结构往往仍然未知。反射各向异性光谱（RAS）是少数允许对固液界面结构进行原位研究的技术之一。然而，要在原子尺度上解释RAS数据，只能通过与计算光谱学进行比较来获得。虽然目前与电化学系统相关的计算RAS研究数量仍然有限，但迄今为止这些研究尚未考虑固液界面的动态性质。在本工作中，我们通过结合从头算分子动力学与计算光谱学，研究了Au(110)缺失行重构在水接触下的光谱响应的时域演化。我们的结果表明，RA光谱的时间演化发生了显著变化，特别是为理论计算与实验比较时通常观察到的强度差异提供了解释。此外，这些发现指出了结构表面/界面变异性的重要性，同时强调了RAS在探测这些动态界面方面的潜力。
英文摘要：
In electrochemistry, reactions and charge-transfer are to a large extent determined by the atomistic structure of the solid-liquid interface. Yet due to the presence of the liquid electrolyte, many surface-science methods cannot be applied here. Hence, the exact microscopic structure that is present under operating conditions often remains unknown. Reflection anisotropy spectroscopy (RAS) is one of the few techniques that allow for an in operando investigation of the structure of solid-liquid interfaces. However, an interpretation of RAS data on the atomistic scale can only be obtained by comparison to computational spectroscopy. While the number of computational RAS studies related to electrochemical systems is currently still limited, those studies so far have not taken into account the dynamic nature of the solid-liquid interface. In this work, we investigate the temporal evolution of the spectroscopic response of the Au(110) missing row reconstruction in contact with water by combining ab initio molecular dynamics with computational spectroscopy. Our results show significant changes in the time evolution of the RA spectra, in particular providing an explanation for the typically observed differences in intensity when comparing theory and experiment. Moreover, these findings point to the importance of structural surface/interface variability while at the same time emphasising the potential of RAS for probing these dynamic interfaces.
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