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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Information Content in O[1s] K-edge X-ray Emission Spectroscopy of Liquid Water
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Information Content in O[1s] K-edge X-ray Emission Spectroscopy of Liquid Water

机译：液态水的O [1s] K边缘X射线发射光谱中的信息含量

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Does the fine-structure in oxygen K-edge X-ray emission (Fuchs et al. Phys. Rev. Lett. 2008, 100, 027801) imply that liquid water is a two-component mixture or is it the signature of a transient OH species arising in the core-excitation process? As with the interpretation of the X-ray absorption spectrum of liquid water, this question is also intensely discussed in the water and X-ray spectroscopy communities. X-ray emission is an independent probe of the electronic structure yielding complementary information on hydrogen bonding in liquid water. In this study, the angular anisotropy in the resonant inelastic soft X-ray scattering (resonant X-ray emission (XE)) spectrum of liquid water is simulated on the basis of ab initio molecular dynamics simulations to allow for direct comparison to recent experimental data (Forsberg et al. Phys. Rev. B 2009, 79, 132203). Theoretical simulations unequivocally show that the difference in angular anisotropy in the water lone-pair features is related to their fundamentally different origin. The high emission-energy peak is primarily due to the contribution from the out-of-plane Obi) lone-pair in intact water molecules. On the other hand, the low emission-energy lone-pair peak originates from the bonding (3a,) state and is assigned to a transient OH species formed by ultrafast (< 10 fs) photodissociation. The information in the XE spectrum on the structure of liquid water is limited and buried in features arising from excited state dynamics. In combination with available experimental data, the theoretical simulations settle a rising debate on the interpretation of resonant and nonresonant XE spectra of liquid water and there are strong implications for the XE spectroscopy of hydrogen-bonded liquids. The simulations show that the fine-structure in the XE spectrum of liquid water can be explained simply in terms of present day ab initio molecular dynamics simulations.
机译：氧K边缘X射线发射的精细结构（Fuchs等人，Phys。Rev. Lett。2008，100，027801）是否暗示液态水是两组分混合物，还是瞬态OH的标志？核心激发过程中产生了哪些物种？与对液态水的X射线吸收光谱的解释一样，在水和X射线光谱学界也对此问题进行了激烈的讨论。 X射线发射是电子结构的独立探针，可产生有关液态水中氢键的补充信息。在这项研究中，液态水的共振非弹性软X射线散射（共振X射线发射（XE））光谱中的角各向异性是根据从头算分子动力学模拟得出的，可以直接与最新实验数据进行比较（Forsberg et al.Phys.Rev.B 2009，79，132203）。理论模拟清楚地表明，水孤对特征的角度各向异性的差异与其根本不同的成因有关。高发射能峰主要是由于完整水分子中平面外Obi）孤对的贡献所致。另一方面，低发射能量孤对峰起源于键合（3a，）状态，并归因于由超快（<10 fs）光解离形成的瞬态OH物种。 XE光谱中有关液态水结构的信息是有限的，并被隐藏在由激发态动力学产生的特征中。结合可用的实验数据，理论模拟解决了关于液态水的共振XE光谱和非共振XE光谱解释的争论，这对氢键液体的XE光谱学具有重要意义。模拟表明，液态水的XE光谱中的精细结构可以简单地用当今的从头算分子动力学模拟来解释。

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