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arXiv:2506.21428 · Physical review. B./Physical review. B

Imaginary time formalism for causal nonlinear response functions

Sounak Sinha, Barry Bradlyn

Published Jun 24, 2026• 0 citations
arXivHTMLPDF

Abstract

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 $n$-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 $A^3$ term in the $SU(2)$ 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 $n$-th harmonic generation rate. Our work opens the door to using imaginary time approaches to study nonlinear response functions in general condensed matter systems.

DOI
10.1103/7sn8-t9ds

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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.
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.
Computing response functions by following the time evolution of superoperators in Liouville space (whose vectors are ordinary Hilbert space operators) offers an attractive alternative to the diagrammatic perturbative expansion of many-body equilibrium and nonequilibrium Green's functions. The bookkeeping of time ordering is naturally maintained in real (physical) time, allowing the formulation of Wick's theorem for superoperators, giving a factorization of higher order response functions in terms of two fundamental Green's functions. Backward propagations and analytic continuations using artificial times (Keldysh loops and Matsubara contours) are avoided. A generating functional for nonlinear response functions unifies quantum field theory and the classical mode coupling formalism of nonlinear hydrodynamics and may be used for semiclassical expansions. Classical response functions are obtained without the explicit computation of stability matrices.
The general expressions for the number density and current are first considered under the action of an external time-dependent perturbing potential of arbitrary strength and cast in terms of the single-particle lesser Green’s function. The expansion of the number density up to linear order in the perturbing potential is then considered, yielding the density–density correlation function of linear-response theory. A connection is also considered with the temperature correlation function of the Matsubara formalism via an analytic continuation in frequency space.
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.
Abstract 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 f-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.
Abstract Conceptually, the Matsubara formalism (MF), using imaginary frequencies, and the Keldysh formalism (KF), formulated in real frequencies, give equivalent results for systems in thermal equilibrium. The MF has less complexity and is thus more convenient than the KF. However, computing dynamical observables in the MF requires the analytic continuation from imaginary to real frequencies. The analytic continuation is well‐known for two‐point correlation functions (having one frequency argument), but, for multipoint correlators, a straightforward recipe for deducing all Keldysh components from the MF correlator had not been formulated yet. Recently, a representation of MF and KF correlators in terms of formalism‐independent partial spectral functions and formalism‐specific kernels was introduced by Kugler, Lee, and von Delft [Phys. Rev. X 11, 041006 (2021)]. This representation is used to formally elucidate the connection between both formalisms. How a multipoint MF correlator can be analytically continued to recover all partial spectral functions and yield all Keldysh components of its KF counterpart is shown. The procedure is illustrated for various correlators of the Hubbard atom.