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Updated: May 14, 2026

Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
Published on: April 8, 2020
Computational analysis of the quadrupole contribution in the second-harmonic generation spectroscopy for the
Kazuya Shiratori1, Shiratori Kazuya, Shoichi Yamaguchi
1Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
Abstract:
Second-order susceptibility for water/vapor interface is calculated theoretically using molecular dynamics simulation, which considers both the dipole and quadrupole contributions. We find that the nonresonant second harmonic generation (SHG) signal is dominated by the quadrupole contribution from the bulk. We also elucidate the fact that the nonresonant susceptibility tends to be negative in general, irrespective of the molecular orientation. The present argument for SHG is commonly applicable to the nonresonant vibrational sum-frequency generation (SFG) spectra, and should be valid for other liquid interfaces.
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