Antisymmetric Raman response

TL;DR

This paper develops a theory for antisymmetric Raman response, a unique signal in low-symmetry systems, useful for probing interband energies and symmetry breaking.

Contribution

It introduces a theoretical framework for antisymmetric Raman response, highlighting its differences from standard responses and its applications in specific materials.

Findings

Antisymmetric Raman response is related to cross-susceptibilities of Raman operators.

Such responses lack intraband contributions, unlike standard Raman signals.

The theory is applied to charge density wave materials and excitonic insulators.

Abstract

We develop the theory of antisymmetric Raman response, defined as the difference between the Raman signals of two scattering geometries related by an exchange of mutually perpendicular incoming and the outgoing photon polarizations. Such responses, finite in orthorhombic or lower symmetry systems, are related to cross-susceptibilities of two Raman operators and are characterized by the absence of intraband terms. This is in contrast to standard Raman responses which measure auto-susceptibilities where both intra- and interband processes contribute. We illustrate the theory with examples from the charge density wave rare-earth tritellurides and the excitonic insulator Ta$_2$NiSe$_5$. Our theory establishes antisymmetric Raman response as a unique tool to probe microscopic features such as interband energy scales and to detect reflection symmetry breaking.