Femtosecond Vibrational Sum-Frequency Generation Spectroscopy of Chiral Molecules in Isotropic Liquid,The Journal of Physical Chemistry Letters

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Femtosecond Vibrational Sum-Frequency Generation Spectroscopy of Chiral Molecules in Isotropic Liquid
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-11-07 00:00:00 , DOI: 10.1021/acs.jpclett.8b02947
Taegon Lee ₁ , Hanju Rhee ₁ , Minhaeng Cho _{2,

3}

Affiliation

Vibrationally resonant optically active (VOA) sum-frequency generation (SFG) is a second-order nonlinear process sensitive to the stereospecific vibrational structure of chiral molecules. We demonstrate that a femtosecond VOA SFG signal can be measured in the isotropic bulk of a chiral liquid. The chiral, achiral, and VOA SFG spectra of R- and S-limonene and their racemic mixture in the C–H stretching frequency region are characterized. In particular, it is shown that the observed circular intensity difference (CID) signal, which can provide distinguishable stereochemical vibrational information between enantiomers, arises from interference of the electric-dipole allowed antisymmetric Raman tensor-induced and Raman optical activity (ROA) tensor-induced SFG fields. Furthermore, we show that the CID and linear polarization intensity difference (LID) SFG spectra are connected to the real and imaginary parts of the effective chiral VOA SFG susceptibility, respectively. We anticipate that the present technique will be of use in transient chiroptical spectroscopy and stereochemical vibrational imaging studies.

中文翻译：

各向同性液体中手性分子的飞秒振动和频产生光谱

振动共振光学活性（VOA）和频率生成（SFG）是对手性分子的立体定向振动结构敏感的二阶非线性过程。我们证明，可以在手性液体的各向同性体积中测量飞秒VOA SFG信号。R-和S的手性，非手性和VOA SFG光谱柠檬烯及其外消旋混合物在C–H拉伸频率范围内的特征。特别地，表明观察到的圆强度差（CID）信号可提供对映异构体之间的明显立体化学振动信息，这是由电偶极子允许的非对称拉曼张量诱发和拉曼光学活性（ROA）张量的干扰引起的。诱导的SFG场。此外，我们表明，CID和线性极化强度差（LID）SFG谱分别与有效手性VOA SFG磁化率的实部和虚部相关。我们期望本技术将用于瞬态手法光谱学和立体化学振动成像研究中。

更新日期：2018-11-07

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