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Physical Review Letters

The Sham-Schlüter Equation in Time-Dependent Density-Functional Theory

Robert van Leeuwen

Published May 6, 1996• 60 citations
Publisher

Abstract

We present an exact equation for the exchange-correlation potential of time-dependent density-functional theory. This relation is derived using a many-particle Green's function formalism due to Keldysh. We furthermore show how this equation can be derived from an action principle. The method presented provides a systematic way to derive correlation contributions to the time-dependent exchange-correlation potential.

DOI
10.1103/physrevlett.76.3610

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We have considered application the Keldysh formalism in time-dependent \ndensity functional theory. It is shown that effects of electron-electron interaction can \nbe taken systematically into account in the framework of the Kadanoff-Baym \nequations for Green functions determined on the Keldysh contour for the second-order \n47 \nself-energy approximation. With the help of these Green functions we have derived \nthe time-dependent Kohn-Sham potential from an action functional. The Keldysh \nformalism in a similar way leads to response functions that obey the causality \nprinciple that is illustrated on the case of the time-dependent optimized effective \npotential equations.
This paper gives an introduction to the Keldysh formalism, with emphasis on its usefulness in time-dependent density functional theory. In the first part we introduce the Keldysh contour and the one-particle Green function defined on this contour. We then discuss how to combine and manipulate functions with time-arguments on the contour. The effects of electron-electron interaction can be taken systematically into account, as we illustrate by propagating the Kadanoff-Baym equations for the second-order self-energy approximation. It is important to use conserving approximations such that the evolution of the electron density, momentum, and total energy agrees with the macroscopic conservation laws. One of the main topics in this paper is the non-interacting Green function, which is the relevant quantity for time-dependent density functional theory. We discuss this Green function in detail, and show how the Keldysh contour in a simple way allows us to derive the time-dependent Kohn-Sham potential from an action functional. The formalism in a similar way leads to response functions that obey the causality principle. To illustrate these points, we discuss the time-dependent optimized effective potential equations.
This chapter presents various techniques from many-body theory to construct time-dependent exchange-correlation (xc) functionals. The first section introduces a perturbation theory along the so-called adiabatic connection. This leads to a perturbative expansion of the xc potential, with exact exchange representing the lowest order. The following section introduces nonequilibrium Green's functions along the Keldysh contour. A Keldysh action principle is formulated which yields a formally exact representation of the time-dependent xc potential. As an alternative, the xc potential is expressed through the so-called Sham-Schlüter equation. The third section establishes a connection between the xc kernels of time-dependent density-functional theory in linear response and many-body perturbation theory. A diagrammatic expansion of the xc kernel is given. Finally, an expression for the xc kernel is derived starting from the Bethe-Salpeter equation. This xc kernel gives excellent agreement with experimental optical absorption spectra of insulators, including excitonic features.
Most present applications of time-dependent density functional theory use adiabatic functionals, i.e., the effective potential at time t is determined solely by the density at the same time. This paper discusses a method that aims to go beyond this approximation, by incorporating "memory" effects: the derived exchange-correlation potential will depend not only on present densities but also on the past. In order to ensure the potentials are causal, we formulate the action on the Keldysh contour for electrons in electromagnetic fields, from which we derive suitable Kohn-Sham equations. The exchange-correlation action is now a functional of the electron density and velocity field. A specific action functional is constructed which is Galilean invariant and yields a causal exchange-correlation vector potential for the Kohn-Sham equations incorporating memory effects. We show explicitly that the net exchange-correlation Lorentz force is zero. The potential is consistent with known dynamical properties of the homogeneous electron gas (in the linear response limit).
Within density-functional theory a time-dependent perturbation theory is derived that yields exact orbital-dependent expressions for the time-dependent exchange-correlation potential in the form of a perturbation series. This leads to an exact time-dependent Kohn-Sham scheme based on perturbation theory. In first order an ``exchange-only'' Kohn-Sham procedure is obtained, that is a generalization of a recently presented time-dependent optimized potential method. The exact, in higher order, but quite complicated expressions for the exchange-correlation potential may serve as a starting point for the construction of approximate exchange-correlation potentials. An adiabatic connection or coupling constant path between a time-dependent physical system and its corresponding Kohn-Sham system is introduced.
The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle, exactly by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation potential as an implicit density functional. It is shown that this suggests a reformulation of TDDFT in terms of the second time derivative of the density, rather than the density itself. The result is a time-local Kohn-Sham scheme of second-order in time whose causal structure is more transparent than that of the usual Kohn-Sham formalism. The scheme can be used to construct new approximations at the exchange-only level and beyond, and it offers a straightforward definition of the exact adiabatic approximation.