Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Progress towards understanding ultranonlocality through the wave-vector and frequency dependence of approximate exchange-correlation kernels

Journal Article · · Physical Review. B
 [1];  [2];  [3];  [2]
  1. Temple Univ., Philadelphia, PA (United States); OSTI
  2. Temple Univ., Philadelphia, PA (United States)
  3. CIC nanoGUNE Research Centre, BRTA and DIPC, Donostia, Basque Country (Spain)
+ Show Author Affiliations
In the framework of time-dependent density functional theory (TDDFT), the exact exchange-correlation (xc) kernel fxc(n, q, ω) determines the ground-state energy, excited-state energies, lifetimes, and the time-dependent linear density response of any many-electron system. The recently developed MCP07 xc kernel fxc(n, q, ω) of A. Ruzsinszky et al. [Phys. Rev. B 101, 245135 (2020)] yields excellent uniform electron gas (UEG) ground-state energies and plausible plasmon lifetimes. As MCP07 is constructed to describe fxc of the UEG, it cannot capture optical properties of real materials. To verify this claim, we follow Nazarov et al. [Phys. Rev. Lett. 102, 113001 (2009)] to construct the long-range, dynamic xc kernel, limq→0 fxc(n, q, ω) = -α(ω)e2/q2, of a weakly inhomogeneous electron gas, using MCP07 and other common xc kernels. The strong wavevector and frequency dependence of the “ultranonlocality” coefficient α(ω) is demonstrated for a variety of simple metals and semiconductors. We examine how imposing exact constraints on an approximate kernel shapes α(ω). Comparisons to kernels derived from correlated-wavefunction calculations are drawn.
Research Organization:
Temple Univ., Philadelphia, PA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012575
OSTI ID:
1851697
Alternate ID(s):
OSTI ID: 1836154
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 12 Vol. 104; ISSN 2469-9950; ISSN PRBMDO
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (51)

Charge and Spin Density Waves in Jellium journal November 1980
A dielectric formulation of the many body problem: Application to the free electron gas journal August 1958
A Brief Compendium of Time-Dependent Density Functional Theory journal July 2013
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Quantum Theory of the Electron Liquid book August 2012
Accurate and Numerically Efficient r 2 SCAN Meta-Generalized Gradient Approximation journal September 2020
Correction to “Accurate and Numerically Efficient r 2 SCAN Meta-Generalized Gradient Approximation” journal October 2020
Fluctuation-dissipation theorem density-functional theory journal April 2005
Beyond time-dependent exact exchange: The need for long-range correlation journal April 2006
Adiabatic-connection fluctuation-dissipation DFT for the structural properties of solids—The renormalized ALDA and electron gas kernels journal September 2015
Perspective: Fundamental aspects of time-dependent density functional theory journal June 2016
Interpretations of ground-state symmetry breaking and strong correlation in wavefunction and density functional theories journal January 2021
Exchange and Correlation Instabilities of Simple Metals journal March 1968
Constraint-based wave vector and frequency dependent exchange-correlation kernel of the uniform electron gas journal June 2020
Exchange-correlation energy of a metallic surface: Wave-vector analysis journal March 1977
Self-interaction correction to density-functional approximations for many-electron systems journal May 1981
Correlation effects on the third-frequency-moment sum rule of electron liquids journal February 1987
Accurate and simple analytic representation of the electron-gas correlation energy journal June 1992
Ab initiomolecular dynamics for liquid metals journal January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Dominant density parameters and local pseudopotentials for simple metals journal May 1995
Erratum: Dominant density parameters and local pseudopotentials for simple metals journal May 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Analytical expressions for the local-field factor G ( q ) and the exchange-correlation kernel K xc ( r ) of the homogeneous electron gas journal June 1998
Elasticity of an electron liquid journal September 1999
Electron correlation energies from scaled exchange-correlation kernels: Importance of spatial versus temporal nonlocality journal May 2000
Electron-hole excitations and optical spectra from first principles journal August 2000
Dynamical exchange-correlation potentials for an electron liquid journal June 2002
Long-range behavior and frequency dependence of exchange-correlation kernels in solids journal January 2003
Tests of a ladder of density functionals for bulk solids and surfaces journal February 2004
Long-range contribution to the exchange-correlation kernel of time-dependent density functional theory journal April 2004
Erratum: Dynamical exchange-correlation potentials for an electron liquid [Phys. Rev. B 65 , 235121 (2002)] journal April 2005
Energy dependence of the exchange-correlation kernel of time-dependent density functional theory: A simple model for solids journal September 2005
Simple dynamic exchange-correlation kernel of a uniform electron gas journal June 2007
Including nonlocality in the exchange-correlation kernel from time-dependent current density functional theory: Application to the stopping power of electron liquids journal November 2007
Optical spectra of solids obtained by time-dependent density functional theory with the jellium-with-gap-model exchange-correlation kernel journal May 2013
Simple screened exact-exchange approach for excitonic properties in solids journal July 2015
Nonlocal energy-optimized kernel: Recovering second-order exchange in the homogeneous electron gas journal January 2016
Gradient-dependent exchange-correlation kernel for materials optical properties journal August 2018
Exact Dynamical Exchange-Correlation Kernel of a Weakly Inhomogeneous Electron Gas journal March 2009
Bootstrap Approximation for the Exchange-Correlation Kernel of Time-Dependent Density-Functional Theory journal October 2011
Estimating Excitonic Effects in the Absorption Spectra of Solids: Problems and Insight from a Guided Iteration Scheme journal April 2015
Fully Parameter-Free Calculation of Optical Spectra for Insulators, Semiconductors, and Metals from a Simple Polarization Functional journal September 2015
Nonlocal and Nonadiabatic Effects in the Charge-Density Response of Solids: A Time-Dependent Density-Functional Approach journal April 2018
Many-Particle Effects in the Optical Excitations of a Semiconductor journal July 1979
Density-Functional Theory for Time-Dependent Systems journal March 1984
Local density-functional theory of frequency-dependent linear response journal December 1985
Local Density-Functional Theory of Frequency-Dependent Linear Response journal August 1986
Excitation Energies from Time-Dependent Density-Functional Theory journal February 1996
Current-Dependent Exchange-Correlation Potential for Dynamical Linear Response Theory journal September 1996
Time-Dependent Density Functional Theory Beyond the Adiabatic Local Density Approximation journal December 1997

Similar Records

First-principles wave-vector- and frequency-dependent exchange-correlation kernel for jellium at all densities
Journal Article · Mon Jan 17 19:00:00 EST 2022 · Physical Review. B · OSTI ID:1979713
Ab Initio Quantum Monte Carlo Simulation of the Warm Dense Electron Gas in the Thermodynamic Limit
Journal Article · Thu Oct 06 20:00:00 EDT 2016 · Physical Review Letters · OSTI ID:1345155

Related Subjects

36 MATERIALS SCIENCE
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY