Coherent Spectroscopic Probes of Topology: A Velocity-Gauge Perspective

TL;DR

This paper introduces a velocity-gauge formalism for analyzing nonlinear optical responses in topological materials, revealing how spectra encode topological features and phase coherence, demonstrated on the SSH model.

Contribution

It develops a gauge-consistent velocity-gauge approach for nonlinear response calculations in topological systems, avoiding common approximations and capturing topological signatures in spectra.

Findings

Nonlinear spectra encode topological phase information.

Third-order response shows phase inversions in topological phase.

Framework applicable beyond dipole approximation.

Abstract

We present a velocity-gauge formalism for computing nonlinear current response functions in periodic systems and apply it to the Su-Schrieffer-Heeger (SSH) model as a minimal topological testbed. By retaining the full minimal coupling Hamiltonian and avoiding the rotating wave approximation, we construct gauge-consistent expressions for the linear and third-order current susceptibilities using retarded Green's functions. Our results reveal how nonlinear optical spectra encode not only energy-level transitions but also interband phase coherence and topological winding. In the topological phase, the third-order response exhibits characteristic phase inversions and spectral asymmetries that are absent in the trivial phase. These features reflect geometric changes in the Bloch eigenstates and highlight the role of virtual pathways in shaping the nonlinear signal. Our framework offers a robust and extensible platform for modeling nonlinear light-matter interactions in topological materials beyond the dipole approximation and the standard Coulomb-gauge formulation in molecular spectroscopy.