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arXiv:cond-mat/0307390 · Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics

Superoperator representation of nonlinear response: Unifying quantum field and mode coupling theories

Shaul Mukamel

Published Aug 26, 2003• 47 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreve.68.021111

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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.
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Time-ordered superoperators are used to develop a unified description of nonlinear density response and spontaneous fluctuations of many-electron systems. The pthp\mathrm{th}pth-order density response functions are decomposed into 2p+1{2}^{p+1}2p+1 non-causal Liouville space pathways. Individual pathways are symmetric to the interchange of their space, time, and superoperator indices and can thus be calculated as functional derivatives. Other combinations of these pathways represent spontaneous density fluctuations and the response of such fluctuations to an external field. The resolution of the causality paradox of time-dependent density-functional theory (TDDFT) is shown to be intimately connected with the nonretarded nature of fluctuations.
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This chapter considers a general form of the Wick’s theorem, which leads to a perturbation expansion of the (contour) single- and two-particle Green’s functions, which are expressed in terms of the contour time-ordering operator. The strategy for proving the Wick’s theorem is similar to that adopted within the Matsubara formalism for the Green’s functions at finite temperature and relies on the Gibbs form of the statistical operator in the interaction picture. An extension to superfluid Bose and Fermi systems is also considered.
We study perturbation expansions for quantum systems which are nonlinear in the sense that they may contain derivative couplings. The characteristic feature of these systems is the occurrence of products of noncommuting operators in the interaction Hamiltonian. In order to perform perturbation expansions in the Dyson-Wick manner it is in general necessary to order these operators according to some ordering scheme. We determine the most general scheme of this sort which allows a Dyson-Wick expansion with pair contractions. It involves a set $\ensuremath{\lambda}$ of three dimensionless ordering parameters which are related to the three aaa priori undetermined equal-time contractions. Different $\ensuremath{\lambda}$-ordering schemes are related via an "equal-time" or "static" Wick theorem. In order to be able to contract operators which may be taken either at equal or at different times we introduce a time-ordering operation ${T}_{\ensuremath{\lambda}}$ which extends Dyson's time-ordering operation to equal times in a fashion dependent on the $\ensuremath{\lambda}$ ordering. We arrive at a "dynamic" Wick theorem which enables us to decompose the ${T}_{\ensuremath{\lambda}}$ product of a set of operators taken at arbitrary times into a sum of ${\ensuremath{\lambda}}^{\ensuremath{'}}$ products, where the most important case is that in which ${\ensuremath{\lambda}}^{\ensuremath{'}}$ represents normal ordering. Contrary to the usual Wick theorem ours works also in the case when two or more times coincide. Applying this theorem to the scattering operator expressed as a ${T}_{\ensuremath{\lambda}}$ product we obtain a class of Dyson-Wick expansions for nonlinear systems. Different expansions correspond to different choices of the ordering $\ensuremath{\lambda}$ and lead to different Feynman rules. The resulting diagrammatic technique for nonlinear systems is seen to have the following special features: (i) The interaction vertices include terms which arise from "quantum corrections," which are dependent on the ordering \ensuremath{\lambda} chosen for the noncommuting factors in the interaction Hamiltonian, and (ii) the equal-time contractions which occur in the closed-loop diagrams must be assigned corresponding $\ensuremath{\lambda}$-dependent values. In this way individual diagrams are $\ensuremath{\lambda}$ dependent. Nevertheless their sum is $\ensuremath{\lambda}$ independent, confirming the fact that the complete scattering operator is independent of the particular ordering chosen. The ordering multiplicity is also reflected in functional versions of the Dyson-Wick expansion. In the path-integral version this multiplicity lurks in the different possible discretization prescriptions. We discuss the relevance of our considerations to the question of the invariance of a quantum theory with respect to nonlinear point transformations. For the special case of a reducible system we present explicit calculations which show how this invariance is maintained in perturbation theory, for any ordering scheme belonging to the $\ensuremath{\lambda}$ class. In any particular scheme the invariance is ensured by a more or less intricate cancellation mechanism between the individual diagrams.