Interfacial Vibrational Dynamics of Ice Ih and Liquid Water
Interfacial Vibrational Dynamics of Ice Ih and Liquid Water
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DOI：
10.1021/jacs.0c04526
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发表时间：
2020-07-15
影响因子：
15
通讯作者：
Bonn, Mischa
中科院分区：
文献类型：
--
作者：
Sudera, Prerna;Cyran, Jenee D.;Bonn, Mischa
深入了解冰表面的能量流动动力学对于理解与大气和地理科学相关的化学动力学至关重要。在这里，采用超快表面特异性光谱，我们报告的冰I-H的界面振动动力学。与液态水表面的比较揭示了氢键OH基团在冰表面的加速振动能弛豫和耗散。相比之下，游离OH基团粘到气相表现出实质上较慢的振动动力学在冰上。这些不同的OH基团在冰面上的振动动力学的加速和减速归因于增强的分子间耦合和减少的旋转流动性，分别。我们的研究结果突出了冰上自由OH基团的独特性质，这与冰表面的高催化活性有关。
Insights into energy flow dynamics at ice surfaces are essential for understanding chemical dynamics relevant to atmospheric and geographical sciences. Here, employing ultrafast surface-specific spectroscopy, we report the interfacial vibrational dynamics of ice I-h. A comparison to liquid water surfaces reveals accelerated vibrational energy relaxation and dissipation at the ice surface for hydrogen-bonded OH groups. In contrast, free-OH groups sticking into the vapor phase exhibit substantially slower vibrational dynamics on ice. The acceleration and deceleration of vibrational dynamics of these different OH groups at the ice surface are attributed to enhanced intermolecular coupling and reduced rotational mobility, respectively. Our results highlight the unique properties of free-OH groups on ice, putatively linked to the high catalytic activities of ice surfaces.