Hayashi Hisashi, Hiraoka Nozomu
‡Department of Chemical and Biological Sciences, Faculty of Science, Japan Women's University, 2-8-1 Mejirodai, Bunkyo, Tokyo 112-8681, Japan.
†National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan.
J Phys Chem B. 2015 Apr 30;119(17):5609-23. doi: 10.1021/acs.jpcb.5b01567. Epub 2015 Apr 15.
Using a third-generation synchrotron source (the BL12XU beamline at SPring-8), inelastic X-ray scattering (IXS) spectra of liquid water and liquid benzene were measured at energy losses of 1-100 eV with 0.24 eV resolution for small momentum transfers (q) of 0.23 and 0.32 au with ±0.06 au uncertainty for q. For both liquids, the IXS profiles at these values of q converged well after we corrected for multiple scattering, and these results confirmed the dipole approximation for q ≤ ∼0.3 au. Several dielectric and optical functions [including the optical oscillator strength distribution (OOS), the optical energy-loss function (OLF), the complex dielectric function, the complex index of refraction, and the reflectance] in the vacuum ultraviolet region were derived and tabulated from these small-angle (small q) IXS spectra. These new data were compared with previously obtained results, and this comparison demonstrated the strong reproducibility and accuracy of IXS spectroscopy. For both water and benzene, there was a notable similarity between the OOSs of the liquids and amorphous solids, and there was no evidence of plasmon excitation in the OLF. The static structure factor [S(q)] for q ≤ ∼0.3 au was also deduced and suggests that molecular models that include electron correlation effects can serve as a good approximation for the liquid S(q) values over the full range of q.
利用第三代同步辐射源(日本理化学研究所Spring-8的BL12XU光束线),在动量转移量(q)为0.23和0.32原子单位(au)、不确定度为±0.06 au的小动量转移条件下,以0.24 eV的分辨率测量了液态水和液态苯在1 - 100 eV能量损失下的非弹性X射线散射(IXS)光谱。对于这两种液体,在对多重散射进行校正后,这些q值下的IXS谱线收敛良好,这些结果证实了q≤0.3 au时的偶极近似。从这些小角度(小q)IXS光谱中推导并列出了真空紫外区域的几个介电和光学函数[包括光学振子强度分布(OOS)、光学能量损失函数(OLF)、复介电函数、复折射率和反射率]。将这些新数据与先前获得的结果进行了比较,这种比较证明了IXS光谱具有很强的可重复性和准确性。对于水和苯,液体和非晶态固体的OOS之间都存在显著的相似性,并且在OLF中没有等离子体激元激发的迹象。还推导了q≤0.3 au时的静态结构因子[S(q)],这表明包含电子关联效应的分子模型可以很好地近似整个q范围内液体的S(q)值。