TY - JOUR
T1 - Time-Variable Chiroptical Vibrational Sum-Frequency Generation Spectroscopy of Chiral Chemical Solution
AU - Lee, Taegon
AU - Oh, Juntaek
AU - Nah, Sanghee
AU - Choi, Dae Sik
AU - Rhee, Hanju
AU - Cho, Minhaeng
N1 - Funding Information:
This work was supported by the Korea Basic Science Institute (KBSI, Grant C140670) for H.R. and the Institute for Basic Science (IBS-R023-D1) for M.C. All the femtosecond chiroptical VSFG measurements were performed using the femtosecond Multi-Dimensional Laser Spectroscopic System (FMLS) at the KBSI.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/10/21
Y1 - 2021/10/21
N2 - Vibrational sum-frequency generation (VSFG) spectroscopy, a surface-specific technique, was shown to be useful even for characterizing the vibrational optical activity of chiral molecules in isotropic bulk liquids. However, accurately determining the spectroscopic parameters is still challenging because of the spectral congestion of chiroptical VSFG peaks with different amplitudes and phases. Here, we show that a time-variable infrared-visible chiroptical three-wave-mixing technique can be used to determine the spectroscopic parameters of second-order vibrational response signals from chiral chemical liquids. For varying the delay time between infrared and temporally asymmetric visible laser pulses, we measure the chiral VSFG, achiral VSFG, and their interference spectra of bulk R-(+)-limonene liquid and perform a global fitting analysis for those time-variable spectra to determine their spectroscopic parameters accurately. We anticipate that this time-variable VSFG approach will be useful for developing nearly background-free chiroptical characterization techniques with enhanced spectral resolution.
AB - Vibrational sum-frequency generation (VSFG) spectroscopy, a surface-specific technique, was shown to be useful even for characterizing the vibrational optical activity of chiral molecules in isotropic bulk liquids. However, accurately determining the spectroscopic parameters is still challenging because of the spectral congestion of chiroptical VSFG peaks with different amplitudes and phases. Here, we show that a time-variable infrared-visible chiroptical three-wave-mixing technique can be used to determine the spectroscopic parameters of second-order vibrational response signals from chiral chemical liquids. For varying the delay time between infrared and temporally asymmetric visible laser pulses, we measure the chiral VSFG, achiral VSFG, and their interference spectra of bulk R-(+)-limonene liquid and perform a global fitting analysis for those time-variable spectra to determine their spectroscopic parameters accurately. We anticipate that this time-variable VSFG approach will be useful for developing nearly background-free chiroptical characterization techniques with enhanced spectral resolution.
UR - http://www.scopus.com/inward/record.url?scp=85118138023&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.1c02479
DO - 10.1021/acs.jpclett.1c02479
M3 - Article
C2 - 34647735
AN - SCOPUS:85118138023
SN - 1948-7185
VL - 12
SP - 10218
EP - 10224
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 41
ER -