Abstract
A theoretical description of the time-resolved infrared-visible sum-frequency-generation (IV-SFG) process when the incident infrared pulsed beam is either left- or right-circularly-polarized (CP) is presented. Even for isotropic chiral molecular liquids, the CP IV-SFG polarization does not vanish because the chiral component of the associated response function is nonzero due to the breakdown of the Born–Oppenheimer approximation as well as to the finite polarizability-electric-quadrupole response function, which is a fourth-rank tensor. For a specific perpendicular detection scheme, it is shown that the three different contributions, originated from (1) all-electric-dipole-allowed polarization, (2) polarizability-quadrupole-induced polarization, and (3) interference between the above two polarizations, to the CP IV-SFG signal can be sperately measured. Also, the circular intensity difference, which is the difference between the left-CP IV-SFG intensity and the right-CP IV-SFG intensity, is theoretically investigated and found to be solely determined by the interference between the all-electric-dipole-allowed polarization and the polarizability-quadrupole-induced polarization. Thus, it is shown that the time-resolved CP IV-SFG methods are useful for the investigation of the molecular chirality of liquids and vibrational optical activity.
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