论文标题

谐振Terahertz激发后水的氢键网络中的能量转移

Energy Transfer within the Hydrogen Bonding Network of Water Following Resonant Terahertz Excitation

论文作者

Elgabarty, Hossam, Kampfrath, Tobias, Bonthuis, Douwe Jan, Balos, Vasileios, Kaliannan, Naveen Kumar, Loche, Philip, Netz, Roland R., Wolf, Martin, Kühne, Thomas D., Sajadi, Mohsen

论文摘要

与许多其他液体相比,水中的能量耗散非常快,更高效。这种行为通常归因于与氢键相关的分子间相互作用。在这里,我们通过泵探针实验研究了液态水氢键网络中的动态能流。我们与超舒服的单周terahertz脉冲共同激发了分子间的自由度,并监测其拉曼反应。通过使用Ultrathin样品细胞窗口,可以获得无背景的双极信号,其尾巴可轻松地指数。弛豫归因于分子平移运动,使用互补实验,力场和从头算分子动力学模拟。他们揭示了Terahertz电场与分子旋转自由度的初始耦合,在激发脉冲持续时间内,能量在激发脉冲持续时间内迅速传递到相邻分子的受限翻译运动。这种快速的能量转移可以通过分子间相互作用的强烈非谐度来合理化。

Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow in the hydrogen-bond network of liquid water by a pump-probe experiment. We resonantly excite intermolecular degrees of freedom with ultrashort single-cycle terahertz pulses and monitor its Raman response. By using ultrathin sample-cell windows, a background-free bipolar signal whose tail relaxes mono-exponentially is obtained. The relaxation is attributed to the molecular translational motions, using complementary experiments, force-field and ab initio molecular dynamics simulations. They reveal an initial coupling of the terahertz electric field to the molecular rotational degrees of freedom whose energy is rapidly transferred, within the excitation pulse duration, to the restricted-translational motion of neighboring molecules. This rapid energy transfer may be rationalized by the strong anharmonicity of the intermolecular interactions.

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