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

Journal Article · · Physical Review. B
 [1]; ORCiD logo [1];  [2];  [1]
  1. Temple Univ., Philadelphia, PA (United States)
  2. CIC nanoGUNE Research Centre, BRTA and DIPC, Donostia, Basque Country (Spain)
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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:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0012575; DMR-1553022
OSTI ID:
1851697
Alternate ID(s):
OSTI ID: 1836154
Journal Information:
Physical Review. B, Vol. 104, Issue 12; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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