Femtosecond Vibrational Sum-Frequency Generation Spectroscopy of Chiral Molecules in Isotropic Liquid

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Title
Femtosecond Vibrational Sum-Frequency Generation Spectroscopy of Chiral Molecules in Isotropic Liquid
Author(s)
Taegon Lee; Hanju Rhee; Minhaeng Cho
Publication Date
2018-12
Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.9, no.23, pp.6723 - 6730
Publisher
AMER CHEMICAL SOC
Abstract
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. © XXXX American Chemical Society
URI
https://pr.ibs.re.kr/handle/8788114/5390
ISSN
1948-7185
Appears in Collections:
Center for Molecular Spectroscopy and Dynamics(분자 분광학 및 동력학 연구단) > Journal Papers (저널논문)
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