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arXiv:1810.00183 · Physical review. B./Physical review. B

Dynamics of the Anderson impurity model: Benchmarking a nonadiabatic exchange-correlation potential in time-dependent density-functional theory

Niklas Dittmann, N. Helbig, Dante Marvin Kennes

Published Feb 13, 2019• 11 citations
arXivHTMLPDF

Abstract

In this comparative study we benchmark a recently developed nonadiabatic exchange-correlation potential within time-dependent density-functional theory (TDDFT) [Phys. Rev. Lett. 120, 157701 (2018)] by (a) validating the transient dynamics using a numerically exact density-matrix renormalization-group approach as well as by (b) comparing the $RC$ time, a typical linear-response quantity, to up to second-order perturbation theory results. As a test bed we use the dynamics of the single-impurity Anderson model. These benchmarks show that the nonadiabatic potential yields quantitatively accurate results for the transient dynamics for temperatures of the order of the hybridization strength, while the TDDFT $RC$ times quantitatively agree with those from second-order perturbation theory for temperatures which are large compared to the hybridization strength. Both results are particularly intriguing given the relatively low numerical cost of a TDDFT calculation.

DOI
10.1103/physrevb.99.075417

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In this comparative study we benchmark a recently developed nonadiabatic exchange-correlation potential within time-dependent density-functional theory (TDDFT) [Phys. Rev. Lett. 120, 157701 (2018)] by (a) validating the transient dynamics using a numerically exact density-matrix renormalization-group approach as well as by (b) comparing the RCRCRC time, a typical linear-response quantity, to up to second-order perturbation theory results. As a test bed we use the dynamics of the single-impurity Anderson model. These benchmarks show that the nonadiabatic potential yields quantitatively accurate results for the transient dynamics for temperatures of the order of the hybridization strength, while the TDDFT RCRCRC times quantitatively agree with those from second-order perturbation theory for temperatures which are large compared to the hybridization strength. Both results are particularly intriguing given the relatively low numerical cost of a TDDFT calculation.
Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t){V}_{\mathrm{xc}}(\mathbf{r},t)Vxc​(r,t), defined as a nonlocal functional of the density $n({\mathbf{r}}^{\ensuremath{'}},{t}^{\ensuremath{'}})$. The popular adiabatic local-density approximation (ALDA) for Vxc(r,t){V}_{\mathrm{xc}}(\mathbf{r},t)Vxc​(r,t) uses only densities at the same space-time point (r,t)(\mathbf{r},t)(r,t). To go beyond the ALDA, two local approximations have been proposed based on quantum hydrodynamics and elasticity theory: (a) using the current as the basic variable (C-TDDFT) [G. Vignale, C. A. Ullrich, and S. Conti, Phys. Rev. Lett. 79, 4847 (1997)], (b) working in a comoving Lagrangian reference frame (L-TDDFT) [I. V. Tokatly, Phys. Rev. B 71, 165105 (2005)]. In this paper we illustrate, compare, and analyze both nonadiabatic theories for simple time-dependent model densities in the linear and nonlinear regime, for a broad range of time and frequency scales. C- and L-TDDFT are identical in certain limits, but, in general, exhibit qualitative and quantitative differences in their respective treatment of elastic and dissipative electron dynamics. In situations where the electronic density rapidly undergoes large deformations, it is found that nonadiabatic effects can become significant, causing the ALDA to break down.
The exact time-dependent correlation energy in time-dependent density-functional theory is shown to sometimes become positive, which is impossible with most present TDDFT approximations. Both the correlation potential and energy can be strongly nonlocal in time. A new inequality is derived for the time-dependent exchange-correlation energy. The correlation energy appears to scale to a constant function of scaled time in the high-density limit. In the linear response regime, the correlation energy is shown to become purely adiabatic, but the correlation potential is generally nonadiabatic. The usefulness of the virial theorem as a test of numerical accuracy is demonstrated. All results are found or inspired by exact numerical solution of a simple model system (Hooke’s atom), and inversion of the corresponding Kohn–Sham equations.
We study time-dependent electron transport through an Anderson model. The electronic interactions on the impurity site are included via the self-energy approximations at Hartree-Fock (HF), second Born (2B), GW, and TTT-matrix levels as well as within a time-dependent density functional (TDDFT) scheme based on the adiabatic Bethe-ansatz local density approximation (ABALDA) for the exchange-correlation potential. The Anderson model is driven out of equilibrium by applying a bias to the leads, and its nonequilibrium dynamics is determined by real-time propagation. The time-dependent currents and densities are compared to benchmark results obtained with the time-dependent density matrix renormalization group (tDMRG) method. Many-body perturbation theory beyond HF gives results in close agreement with tDMRG, especially within the 2B approximation. We find that the TDDFT approach with the ABALDA approximation produces accurate results for the densities on the impurity site, but overestimates the currents. This problem is found to have its origin in an overestimation of the lead densities, which indicates that the exchange-correlation potential must attain nonzero values in the leads.
In this work, nonadiabatic exchange-correlation (XC) potentials for time-dependent density-functional theory (TDDFT) for strongly correlated materials are derived in the limits of strong and weak correlations. After summarizing some essentials of the available dynamical mean-field theory (DMFT) XC potentials valid for these systems, we present details of the Sham–Schluter equation approach that we use to obtain, in principle, an exact XC potential from a many-body theory solution for the nonequilibrium electron self-energy. We derive the XC potentials for the one-band Hubbard model in the limits of weak and strong on-site Coulomb repulsion. To test the accuracy of the obtained potentials, we compare the TDDFT results obtained with these potentials with the corresponding nonequilibrium DMFT solution for the one-band Hubbard model and find that the agreement between the solutions is rather good. We also discuss possible directions to obtain a universal XC potential that would be appropriate for the case of intermediate interaction strengths, i.e., a nonadiabatic potential that can be used to perform TDDFT analysis of nonequilibrium phenomena, such as transport and other ultrafast properties of materials with any strength of electron correlation at any value in the applied perturbing field.
Time-dependent density-functional theory (TDDFT) is a powerful tool in studying the nonequilibrium dynamics of inhomogeneous interacting many-body systems. Here we show that the simple adiabatic local-spin-density approximation for the time-dependent exchange-correlation potential is surprisingly accurate in describing collective density and spin dynamics in strongly correlated one-dimensional ultracold Fermi gases. Our conclusions are based on extensive comparisons between our TDDFT results and accurate results based on the adaptive time-dependent density-matrix renormalization-group method.
Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential V(xc)(r,t). An exact (i.e., nonadiabatic) extension of the ground-state LDA into the dynamical regime leads to a V(xc)(r,t) with a memory, which causes the electron dynamics to become dissipative. To illustrate and explain this nonadiabatic behavior, this paper studies the dynamics of two interacting electrons on a two-dimensional quantum strip of finite size, comparing TDDFT within and beyond the ALDA with numerical solutions of the two-electron time-dependent Schrodinger equation. It is shown explicitly how dissipation arises through multiple particle-hole excitations, and how the nonadiabatic extension of the ALDA fails for finite systems but becomes correct in the thermodynamic limit.