Progress towards understanding ultranonlocality through the wave-vector and frequency dependence of approximate exchange-correlation kernels
| Autor: | Niraj K. Nepal, Aaron D. Kaplan, Adrienn Ruzsinszky, José María Pitarke |
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| Přispěvatelé: | Department of Energy (US), Temple University, National Science Foundation (US), Energy Frontier Research Centers (US) |
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Physics
Chemical Physics (physics.chem-ph) Condensed Matter - Materials Science Materials Science (cond-mat.mtrl-sci) FOS: Physical sciences 02 engineering and technology Frequency dependence Time-dependent density functional theory 021001 nanoscience & nanotechnology 01 natural sciences 7. Clean energy Omega Physics - Chemical Physics 0103 physical sciences Density functional theory Variety (universal algebra) 010306 general physics 0210 nano-technology Fermi gas Kernel (category theory) Energy (signal processing) Mathematical physics Optics (physics.optics) Physics - Optics |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| Popis: | 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 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→0fxc(n,q,ω)=−α(ω)e2/q2, of a weakly inhomogeneous electron gas, using MCP07 and other common xc kernels. The strong wave-vector 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-wave-function calculations are drawn. The authors acknowledge support from the U.S. National Science Foundation under Grant No. DMR-1553022. A.D.K. acknowledges support from the U.S. Department of Energy, Basic Energy Sciences, through the Energy Frontier Research Center for Complex Materials from First Principles Grant No. DE-SC0012575; and Temple University. |
| Databáze: | OpenAIRE |
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