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Title: Finite-Field Approach to Solving the Bethe-Salpeter Equation

Journal Article · · Physical Review Letters
 [1];  [2];  [3];  [4];  [5]
  1. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering
  2. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering, and Dept. of Chemistry
  3. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division, and Inst. for Molecular Engineering
  4. Univ. of California, Davis, CA (United States). Dept. of Computer Science
  5. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering, and Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division, and Inst. for Molecular Engineering
+ Show Author Affiliations

In this paper, we present a method to compute optical spectra and exciton binding energies of molecules and solids based on the solution of the Bethe-Salpeter equation and the calculation of the screened Coulomb interaction in a finite field. The method does not require either the explicit evaluation of dielectric matrices or of virtual electronic states, and can be easily applied without resorting to the random phase approximation. In addition, it utilizes localized orbitals obtained from Bloch states using bisection techniques, thus greatly reducing the complexity of the calculation and enabling the efficient use of hybrid functionals to obtain single particle wave functions. We report exciton binding energies of several molecules and absorption spectra of condensed systems of unprecedented size, including water and ice samples with hundreds of atoms.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1530398
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 23 Vol. 122; ISSN 0031-9007; ISSN PRLTAO
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
electron-hole excitation
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