Circular dichroism of second harmonic generation response

TL;DR

This paper demonstrates how polarization-dependent second-harmonic generation spectroscopy can reveal chiral and magnetic properties of materials, with explicit theoretical expressions for dichroic signals involving electric-dipole and quadrupole interactions.

Contribution

It provides a theoretical framework for analyzing circular dichroism in SHG, including explicit formulas for electronic multipoles in NCD and MCD responses.

Findings

Dichroic signals depend on circular polarization and scattering events.

Explicit expressions for electronic multipoles in SHG dichroism are derived.

Theoretical techniques from atomic physics are applied to nonlinear optical responses.

Abstract

Polarization-dependent photon spectroscopy (dichroism) of the second-harmonic generation (SHG) response is shown to reveal chiral and magnetic properties of a sample. Two dichroic signals are allowed with electric-dipole (E1) and electric-quadrupole (E2) scattering events, and both require circular polarization in the primary beam. Explicit expressions for electronic multipoles, which benefit from equivalent electronic operators, in NCD and MCD of the SHG response are derived using theoretical techniques from atomic physics.