Sum-frequency vibrational spectroscopy of chiral liquids off and close to electronic resonance and the antisymmetric Raman tensor.
The strength of the chiral vibrational peaks in infrared-visible sum-frequency (SF) vibrational spectra from isotropic chiral liquids is proportional to the square of the corresponding antisymmetric Raman element. Under the Born-Oppenheimer adiabatic approximation with nonadiabatic corrections, the antisymmetric Raman tensor is much weaker than the symmetric counterpart, but becomes significantly stronger as the input frequency (or the sum-frequency in SF generation) approaches electronic resonance. We verify the theory with experimental results obtained from infrared-visible doubly resonant sum-frequency generation from an isotropic solution of chiral molecules.
Department of Physics, University of California-Berkeley, Berkeley, CA 94720, USA. mbelkin@socrates.berkeley.edu
M A
MA
Belkin
Y R
YR
Shen
R A
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Harris