Fast, efficient, and accurate dielectric screening using a local real-space approach.

John Vinson, Eric L Shirley
Author Information
  1. John Vinson: Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA. ORCID
  2. Eric L Shirley: Physical Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA. ORCID

Abstract

Various many-body perturbation theory techniques for calculating electron behavior rely on , the screened Coulomb interaction. Computing requires complete knowledge of the dielectric response of the electronic system, and the fidelity of the calculated dielectric response limits the reliability of predicted electronic and structural properties. As a simplification, calculations often begin with the random-phase approximation (RPA). However, even RPA calculations are costly and scale poorly, typically as ( representing the system size). A local approach has been shown to be efficient while maintaining accuracy for screening core-level excitations [Ultramicroscopy , 986 (2006)]. We extend this method to valence-level excitations. We present improvements to the accuracy and execution of this scheme, including reconstruction of the all-electron character of the pseudopotential-based wave functions, improved log scaling, and a parallelized implementation. We discuss applications to Bethe-Salpeter equation calculations of core and valence spectroscopies.

References

  1. Phys Rev B Condens Matter. 1991 Jun 15;43(17):14142-14156 [PMID: 9997284]
  2. Phys Rev B Condens Matter Mater Phys. 2011;83: [PMID: 31080344]
  3. Phys Rev B Condens Matter. 1993 Jun 15;47(23):15404-15412 [PMID: 10005929]
  4. Phys Rev B Condens Matter. 1995 Jul 15;52(4):R2225-R2228 [PMID: 9981377]
  5. Phys Rev B Condens Matter. 1988 Feb 15;37(5):2733-2736 [PMID: 9944839]
  6. Phys Rev Lett. 2010 Oct 1;105(14):146401 [PMID: 21230850]
  7. Phys Rev B. 2017 Nov 15;96(20): [PMID: 29333524]
  8. Phys Rev Lett. 1995 Mar 6;74(10):1827-1830 [PMID: 10057767]
  9. Phys Rev B Condens Matter. 1992 Jun 15;45(23):13244-13249 [PMID: 10001404]
  10. Phys Rev Lett. 2011 Oct 28;107(18):186404 [PMID: 22107653]
  11. J Phys Condens Matter. 2009 Sep 30;21(39):395502 [PMID: 21832390]
  12. Phys Rev Lett. 2005 May 13;94(18):186402 [PMID: 15904386]
  13. Phys Rev B Condens Matter. 1987 Sep 15;36(9):4821-4830 [PMID: 9943498]
  14. J Phys Condens Matter. 2019 Aug 14;31(32):325902 [PMID: 30943462]
  15. J Chem Theory Comput. 2019 Oct 8;15(10):5299-5307 [PMID: 31424933]
  16. J Chem Phys. 2014 Jan 21;140(3):034107 [PMID: 25669363]
  17. Microsc Microanal. 2014 Aug;20(4):1053-9 [PMID: 24758771]
  18. Ultramicroscopy. 2006 Oct-Nov;106(11-12):986-93 [PMID: 16876323]
  19. J Phys Condens Matter. 2017 Oct 24;29(46):465901 [PMID: 29064822]
  20. Phys Rev B Condens Matter. 1992 Nov 1;46(17):10734-10737 [PMID: 10002929]
  21. Phys Rev B Condens Matter. 1994 Mar 15;49(12):8024-8028 [PMID: 10009565]
  22. Phys Rev B Condens Matter. 1994 Dec 15;50(24):17953-17979 [PMID: 9976227]
  23. Phys Rev Lett. 2017 Mar 3;118(9):096402 [PMID: 28306298]
  24. J Chem Theory Comput. 2018 Sep 11;14(9):4856-4869 [PMID: 30092140]
  25. J Phys Condens Matter. 2014 Sep 10;26(36):363202 [PMID: 25135665]

Grants

  1. 9999-NIST/Intramural NIST DOC

Word Cloud

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