Theory of quadrupole contributions from interface and bulk in second-order optical processes

Kazuya Shiratori, Akihiro Morita

Research output: Contribution to journalArticlepeer-review

32 Citations (Scopus)

Abstract

A unified treatment of the dipole and quadrupole contributions to the second-order optical response is developed. The concept of the effective susceptibility is expanded to incorporate both the surface and bulk contributions. This treatment allows us to quantitatively evaluate both surface and bulk contributions in experimental SFG/SHG spectra. The present theory clarifies a number of qualitative features in the quadrupole contribution, and is thereby utilized to settle recent confusions about the quadrupole and/or bulk effects on the surface nonlinear spectroscopy.

Original languageEnglish
Pages (from-to)1061-1076
Number of pages16
JournalBulletin of the Chemical Society of Japan
Volume85
Issue number10
DOIs
Publication statusPublished - 2012

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