Vibrational Spectroscopic Response of Intermolecular Orientational Correlation at the Water Surface
Vibrational Spectroscopic Response of Intermolecular Orientational Correlation at the Water Surface
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DOI：
10.1021/jp9060957
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发表时间：
2009-09-17
影响因子：
3.7
通讯作者：
Morita, Akihiro
中科院分区：
文献类型：
--
作者：
Ishiyama, Tatsuya;Morita, Akihiro
基于时间相关公式，通过分子动力学模拟计算了汽水界面的二阶非线性极化率，它是产生窄频(SFG)谱的来源。计算的磁化率很好地重现了最近的相敏SFG实验(纪万昌等人)。太棒了。莱特牧师。2008、100、096102)，包括3,000-3,200厘米(-1)区域的正虚部，这是作业中有争议的问题。发现虚磁化率的这一正部分是通过各向异性局域场在界面上的分子间取向耦合引起的。
The second-order nonlinear susceptibility, which is the source of the SLIM frequency generation (SFG) spectrum, for the vapor-water interface is calculated by molecular dynamics simulation based on the time con-elation formula. The calculated susceptibility well reproduces that of the recent phase-sensitive SFG experiment (Ji et al. Phys. Rev. Lett. 2008, 100, 096102), including the positive imaginary part in the 3000-3200 cm(-1) region, which is a controversial problem in the assignment. It is found that this positive part of the imaginary susceptibility is induced by the intermolecular orientational con-elation at the interface through the anisotropic local field.