Spectral Density and Sum Rules for Second-Order Response Functions

TL;DR

This paper develops a formalism to derive sum rules for second-order response functions in quantum materials, linking spectral densities to ground state properties and providing constraints on nonlinear optical responses.

Contribution

It introduces a general method using Kramers-Kronig relations to derive sum rules for second-order response functions, connecting spectral densities with ground state properties and response asymptotics.

Findings

Derived sum rules for second-order density-density response functions.

Expressed sum rules in terms of Bloch Hamiltonian matrix elements for noninteracting electrons.

Established constraints on high-frequency behavior of nonlinear responses.

Abstract

Sum rules for linear response functions give powerful and experimentally-relevant relations between frequency moments of response functions and ground state properties. In particular, renewed interest has been drawn to optical conductivity and density-density sum rules and their connection to quantum geometry in topological materials. At the same time, recent work has also illustrated the connection between quantum geometry and second-order nonlinear response functions in quantum materials, motivating the search for exact sum rules for second-order response that can provide experimental probes and theoretical constraints for geometry and topology in these systems. Here we begin to address these questions by developing a general formalism for deriving sum rules for second-order response functions. Using generalized Kramers-Kronig relations, we show that the second-order Kubo formula can be expressed in terms of a spectral density that is a sum of Dirac delta functions in frequency. We show that moments of the spectral density can be expressed in terms of averages of equal-time commutators, yielding a family of generalized sum rules; furthermore, these sum rules constrain the large-frequency asymptotic behavior of the second harmonic generation rate. We apply our formalism to study generalized $f$-sum rules for the second-order density-density response function and the longitudinal nonlinear conductivity. We show that for noninteracting electrons in solids, the generalized $f$-sum rule can be written entirely in terms of matrix elements of the Bloch Hamiltonian. Finally, we derive a family of sum rules for rectification response, determining the large-frequency asymptotic behavior of the time-independent response to a harmonic perturbation.