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arXiv:0812.2296 · Physical Review Letters

Exact Dynamical Exchange-Correlation Kernel of a Weakly Inhomogeneous Electron Gas

V. U. Nazarov, Giovanni Vignale, Yih Chang

Published Mar 18, 2009• 18 citations
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Abstract

The dynamical exchange-correlation kernel f{xc} of a nonuniform electron gas is an essential input for the time-dependent density-functional theory of electronic systems. The long-wavelength behavior of this kernel is known to be of the form f{xc}=alpha/q{2} where q is the wave vector and alpha is a frequency-dependent coefficient. We show that in the limit of weak nonuniformity the coefficient alpha has a simple and exact expression in terms of the ground-state density and the frequency-dependent kernel of a uniform electron gas at the average density. We present an approximate evaluation of this expression for Si and discuss its implications for the theory of excitonic effects.

DOI
10.1103/physrevlett.102.113001

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The dynamical exchange-correlation kernel f{xc} of a nonuniform electron gas is an essential input for the time-dependent density-functional theory of electronic systems. The long-wavelength behavior of this kernel is known to be of the form f{xc}=alpha/q{2} where q is the wave vector and alpha is a frequency-dependent coefficient. We show that in the limit of weak nonuniformity the coefficient alpha has a simple and exact expression in terms of the ground-state density and the frequency-dependent kernel of a uniform electron gas at the average density. We present an approximate evaluation of this expression for Si and discuss its implications for the theory of excitonic effects.
We express the high-frequency (antiadiabatic) limit of the exchange-correlation (xc) kernels of an inhomogeneous electron gas in terms of the following equilibrium properties: the ground-state density, the xc kinetic stress tensor, the pair-correlation function and the ground-state xc potential. Of these quantities, the first three are amenable to exact evaluation by quantum Monte Carlo methods while the last can be obtained from the inversion of the Kohn-Sham equation for the ground-state orbitals. The exact scalar kernel, in this limit, is found to be of very long range in space, at variance with the kernel that is used in the standard local density approximation. The antiadiabatic xc kernels will be useful in calculations of excitation energies by time-dependent density-functional theory in atoms, molecules, and solids, and provide a solid basis for interpolation between the low- and high-frequency limits of the xc kernels.
The key quantity in the formulation of linear-response theory within time-dependent density-functional theory is the so-called exchange-correlation (xc) kernel. This chapter discusses the properties of the xc kernel. In general, it is a complex and frequency-dependent object, and a functional of the ground-state density. Several exact properties such as the zero-force theorem, static and high-frequency limit, and the long-range behaviour are discussed. The xc kernel can be related to a time-dependent variational principle provided one pays attention to certain time-dependent boundary conditions to ensure causality. The adiabatic approximation of the xc kernel is discussed. Finally, the third section of the chapter reviews the xc kernel of the homogeneous electron liquid. Many of its exact properties are covered, such as the high- and low-frequency limit and the long-wavevector limit. Three widely used parametrizations are presented and the analytical behaviour in the complex frequency plane is investigated.
A simple approximate expression in real and reciprocal spaces is given for the static exchange-correlation kernel of a uniform electron gas interacting with the long-range part only of the Coulomb interaction. This expression interpolates between the exact asymptotic behaviors of this kernel at small and large wave vectors which in turn requires, among other things, information from the momentum distribution of the uniform electron gas with the same interaction that have been calculated in the G0W0{G}_{0}{W}_{0}G0​W0​ approximation. This exchange-correlation kernel as well as its complement analog associated to the short-range part of the Coulomb interaction are more local than the Coulombic exchange-correlation kernel and constitute potential ingredients in approximations for recent adiabatic connection fluctuation-dissipation and/or density functional theory approaches of the electronic correlation problem based on a separate treatment of long- and short-range interaction effects.
The scalar f(xc) and tensor f(xc) exchange-correlation (xc) kernels are key ingredients of the time-dependent density functional theory and the time-dependent current density functional theory, respectively. We derive a comparatively simple relation between these two kernels under the assumption that the dynamic xc can be considered "weak." A calculation of the frequency-dependent dielectric function of silicon using this relation in conjunction with Vignale-Kohn f(xc) demonstrates a potential of our method to account for the dynamic many-body effects within the rigorous scheme of time-dependent density functional theory. Our formula provides a bridge between the scalar f(xc), which directly enters many applications, and the tensor f(xc) which, due to its locality in space, is much easier to approximate.
For two prototype systems, we calculate the exact exchange-correlation kernels ${f}_{\mathrm{xc}}(x,{x}^{\ensuremath{'}},\ensuremath{\omega})$ of time-dependent density functional theory. fxc{f}_{\mathrm{xc}}fxc​, the key quantity for optical absorption spectra of electronic systems, is normally subject to uncontrolled approximation. We find that, up to the first excitation energy, the exact fxc{f}_{\mathrm{xc}}fxc​ has weak frequency dependence and a simple, though nonlocal, spatial form. For higher excitations, the spatial behavior and frequency dependence become more complex. The accuracy of the underlying exchange-correlation potential is of crucial importance.
We present some details of our recently-proposed Time-Dependent Density-Functional Theory (TDDFT) for strongly-correlated materials in which the exchange-correlation (XC) kernel is derived from the charge susceptibility obtained using Dynamical Mean-Field Theory (the TDDFT + DMFT approach). We proceed with deriving the expression for the XC kernel for the one-band Hubbard model by solving DMFT equations via two approaches, the Hirsch–Fye Quantum Monte Carlo (HF-QMC) and an approximate low-cost perturbation theory approach, and demonstrate that the latter gives results that are comparable to the exact HF-QMC solution. Furthermore, through a variety of applications, we propose a simple analytical formula for the XC kernel. Additionally, we use the exact and approximate kernels to examine the nonhomogeneous ultrafast response of two systems: a one-band Hubbard model and a Mott insulator YTiO3. We show that the frequency dependence of the kernel, i.e., memory effects, is important for dynamics at the femtosecond timescale. We also conclude that strong correlations lead to the presence of beats in the time-dependent electric conductivity in YTiO3, a feature that could be tested experimentally and that could help validate the few approximations used in our formulation. We conclude by proposing an algorithm for the generalization of the theory to non-linear response.