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Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O

机译：液态H2O氢键网络中的超快存储损耗和能量重新分布

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Many of the unusual properties of liquid water are attributed to its unique structure, comprised of a random and fluctuating three-dimensional network of hydrogen bonds that link the highly polar water molecules(1,2). One of the most direct probes of the dynamics of this network is the infrared spectrum of the OH stretching vibration(3-11), which reflects the distribution of hydrogen-bonded structures and the intermolecular forces controlling the structural dynamics of the liquid. Indeed, water dynamics has been studied in detail(5-14), most recently using multi-dimensional nonlinear infrared spectroscopy(15,16) for acquiring structural and dynamical information on femtosecond timescales. But owing to technical difficulties, only OH stretching vibrations in D2O or OD vibrations in H2O could be monitored. Here we show that using a specially designed, ultrathin sample cell allows us to observe OH stretching vibrations in H2O. Under these fully resonant conditions, we observe hydrogen bond network dynamics more than one order of magnitude faster than seen in earlier studies that include an extremely fast sweep in the OH frequencies on a 50-fs timescale and an equally fast disappearance of the initial inhomogeneous distribution of sites. Our results highlight the efficiency of energy redistribution within the hydrogen-bonded network, and that liquid water essentially loses the memory of persistent correlations in its structure within 50 fs.
机译：液态水的许多非同寻常性质归因于其独特的结构，该结构由连接高极性水分子的氢键的随机且波动的三维网络组成（1,2）。该网络动力学最直接的探究之一是OH拉伸振动的红外光谱（3-11），它反映了氢键结构的分布以及控制液体结构动力学的分子间力。实际上，已经对水动力学进行了详细研究（5-14），最近使用多维非线性红外光谱法（15,16）来获取飞秒时标上的结构和动力学信息。但是由于技术上的困难，只能监测D2O中的OH拉伸振动或H2O中的OD振动。在这里，我们表明使用经过特殊设计的超薄样品池可以观察到H2O中的OH拉伸振动。在这些完全共振的条件下，我们观察到的氢键网络动力学比以前的研究快了一个数量级，其中包括在50 fs的时间尺度上以非常快的频率扫描OH频率，并且初始不均匀分布也迅速消失了。网站。我们的结果强调了氢键网络内能量重新分配的效率，并且液态水在50 fs内基本上失去了其结构中持久相关性的记忆。

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