液态水第一配位壳层瞬时不对称性的电子特征
Electronic signature of the instantaneous asymmetry in the first coordination shell of liquid water
摘要：
解释水的X射线光谱作为其不对称结构的证据已经挑战了传统的对称近四面体模型，并引发了激烈的辩论的顺序和对称性的氢键网络在水中。在这里，我们提出了新的见解，在水中获得使用一种新的能量分解方法的局部相互作用的性质。我们的模拟结果表明，虽然一个水分子的形式，平均而言，两个强的施主和两个强的受体键，有一个显着的不对称，这些接触的能量。我们证明，这种不对称性是一个小的瞬时扭曲的氢键，这似乎是一个平均对称结构周围的数百飞秒的时间尺度上的波动的结果。此外，我们表明，X射线吸收光谱的显着特点源于分子具有高瞬时不对称性。我们的研究结果具有重要意义，因为它们有助于调和水结构的对称和不对称观点。
英文摘要：
Interpretation of the X-ray spectra of water as evidence for its asymmetric structure has challenged the conventional symmetric nearly-tetrahedral model and initiated an intense debate about the order and symmetry of the hydrogen bond network in water. Here, we present new insights into the nature of local interactions in water obtained using a novel energy decomposition method. Our simulations reveal that while a water molecule forms, on average, two strong donor and two strong acceptor bonds, there is a significant asymmetry in the energy of these contacts. We demonstrate that this asymmetry is a result of small instantaneous distortions of hydrogen bonds, which appear as fluctuations on a timescale of hundreds of femtoseconds around the average symmetric structure. Furthermore, we show that the distinct features of the X-ray absorption spectra originate from molecules with high instantaneous asymmetry. Our findings have important implications as they help reconcile the symmetric and asymmetric views on the structure of water.
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