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arXiv:2102.04425 · Annals of Physics

Gauge invariance and Ward identities in nonlinear response theory

Habib Rostami, Mikhail I. Katsnelson, Giovanni Vignale, Marco Polini

Published May 26, 2021• 40 citations
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Abstract

We present a formal analysis of nonlinear response functions in terms of correlation functions in real- and imaginary-time domains. In particular, we show that causal nonlinear response functions, expressed in terms of nested commutators in real time, can be obtained from the analytic continuation of time-ordered response functions, which are more easily amenable to diagrammatic calculation. This generalizes the well-known result of linear response theory. We then use gauge invariance arguments to derive exact relations between second-order response functions in density and current channels. These identities, which are non-perturbative in the strength of inter-particle interactions, allow us to establish exact connections between nonlinear optics calculations done in different electromagnetic gauges.

DOI
10.1016/j.aop.2021.168523

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We present a formal analysis of nonlinear response functions in terms of correlation functions in real- and imaginary-time domains. In particular, we show that causal nonlinear response functions, expressed in terms of nested commutators in real time, can be obtained from the analytic continuation of time-ordered response functions, which are more easily amenable to diagrammatic calculation. This generalizes the well-known result of linear response theory. We then use gauge invariance arguments to derive exact relations between second-order response functions in density and current channels. These identities, which are non-perturbative in the strength of inter-particle interactions, allow us to establish exact connections between nonlinear optics calculations done in different electromagnetic gauges.
It is well established that causal linear response functions can be found by computing the much simpler imaginary time-ordered Matsubara functions and performing an analytic continuation. This principle is the basis for much of our understanding of linear response for interacting and disordered systems, via diagrammatic perturbation theory. Similar imaginary-time approaches have recently been introduced for computing nonlinear response functions as well, for example in [Annalen der Physik 536, 2300504 (2024); Physical Review X 11, 041006 (2021)], where the authors analytically continue the Matsubara functions to obtain the Keldysh response functions. In this work, we provide a proof of this connection to all orders in perturbation theory using an equation of motion based approach. We show by induction that causal nonlinear response functions at every order can be obtained from an analytic continuation of an appropriate time-ordered Matsubara function. We demonstrate this connection explicitly for second order response functions in the Lehmann representation. As a byproduct of our approach, we derive an explicit expression for the Lehmann representation of nnn-th order response functions by solving the equations of motion. We also use our result to find an analytic spectral density representation for both causal response functions and Matsubara functions. As an example, we apply our method to derive the non-linear A3A^3A3 term in the SU(2)SU(2)SU(2) spin Hall response of an insulator with spin rotation symmetry. Finally, we show how our results lead to a family of generalized sum rules, focusing explicitly on the asymptotic expression for nnn-th harmonic generation rate. Our work opens the door to using imaginary time approaches to study nonlinear response functions in general condensed matter systems.
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Motivated by the recent developments in terahertz spectroscopy using pump-probe setups to study correlated electronic materials, we review the field theoretical formalism to compute finite frequency nonlinear electro-optical responses in centrosymmetric systems starting from basic time dependent perturbation theory. We express the nonlinear current kernel as a sum of several causal response functions. These causal functions cannot be evaluated using perturbative field theory methods, since they are not contour ordered. Consequently, we associate each response function with a corresponding imaginary time ordered current correlation function, since the latter can be factorized using Wick's theorem. The mapping between the response functions and the correlation functions, suitably analytically continued to real frequencies, is proven exactly. We derive constraints satisfied by the nonlinear current kernel and we prove a generalized fff-sum rule for the nonlinear conductivity, all of which are consequences of particle number conservation. The constraints guarantee that the nonlinear static responses are free from spurious divergences. We apply the theory to compute the gauge invariant nonlinear conductivity of a system of noninteracting electrons in the presence of weak disorder. As special cases of this generalized nonlinear response, we discuss its third harmonic and its instantaneous terahertz Kerr signals. The formalism can be used to compute the nonlinear conductivity in symmetry broken phases of electronic systems such as superconductors, density waves and nematic states.
Motivated by the recent developments in terahertz spectroscopy using pump-probe setups, we develop the theory of finite frequency nonlinear electro-optical responses in centrosymmetric metals starting from basic time dependent perturbation theory. We express the nonlinear current kernel as a sum of several causal response functions. These functions cannot be evaluated using perturbative field theory methods. Consequently, we associate each response function with an imaginary time ordered current correlation function, which can be factorized using Wick's theorem. The mapping between the response functions and the correlation functions, suitably analytically continued to real frequencies, is proven exactly. We derive constraints satisfied by the nonlinear current kernel and we prove a generalized fff-sum rule for the nonlinear conductivity, all of which are consequences of particle number conservation. We apply the theory to compute the gauge invariant nonlinear conductivity of a system of noninteracting electrons in the presence of weak disorder. As special cases of this generalized nonlinear response, we discuss its third harmonic and its instantaneous terahertz Kerr signals. Our formalism can be used to compute the nonlinear conductivity in symmetry broken phases such as density waves and nematic states.
We present a diagrammatic theory for determining consistent electromagnetic response functions in strongly correlated fermionic superfluids. While a gauge-invariant electromagnetic response is well understood at the BCS level, a treatment of correlations beyond BCS theory requires extending this theoretical formalism. The challenge in such systems is to maintain gauge invariance, while simultaneously incorporating additional self-energy terms arising from strong correlation effects. Central to our approach is the application of the Ward-Takahashi identity, which introduces collective mode contributions in the response functions and guarantees that the fff-sum rule is satisfied. We outline a powerful method, which determines these collective modes in the presence of correlation effects and in a manner compatible with gauge invariance. Since this method is based on fundamental aspects of quantum field theory, the underlying principles are broadly applicable to strongly correlated superfluids. As an illustration of the technique, we apply it to a simple class of theoretical models that contain a frequency-independent order parameter. These models include BCS-BEC crossover theories of the ultracold Fermi gases, along with models specifically associated with the high-Tc{T}_{c}Tc​ cuprates. Finally, as an alternative approach, we contrast with the path integral formalism. Here, the calculation of gauge-invariant response appears more straightforward. However, the collective modes introduced are those of strict BCS theory, without any modification from additional correlations. As the path integral simultaneously addresses electrodynamics and thermodynamics, we emphasize that it should be subjected to a consistency test beyond gauge invariance, namely that of the compressibility sum rule. We show how this sum rule fails in the conventional path integral approach.
Response theory describes the reaction of observales to perturbations in external fields. We review this formalism for quantum fiels in isolation that have unitary time evolution. An emphasis is put on consequences of causality and the resulting spectral representations for linear and nonlinear response functions, on functional techniques and generating functionals, including the description of the initial state, the evolution, and measurements. We review consequences of time reversal symmetry and relations for the statistics of work, and discuss a large class of quantum correlation functions, and their relation to response functions through fluctuation-dissipation relations. Consequences of conservation laws and gauge symmetries are mentioned briefly.