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Journal of Chemical Physics / Volume 133 / Issue 16 / ARTICLES / Theoretical Methods and Algorithms

J. Chem. Phys. 133, 164109 (2010); http://dx.doi.org/10.1063/1.3494540 (10 pages)

Ab initio calculations of optical absorption spectra: Solution of the Bethe–Salpeter equation within density matrix perturbation theory

Dario Rocca1, Deyu Lu1, and Giulia Galli1,2

1Department of Chemistry, University of California, Davis, Davis, California 95616, USA
2Department of Physics, University of California, Davis, Davis, California 95616, USA

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(Received 28 May 2010; accepted 8 September 2010; published online 27 October 2010)

We describe an ab initio approach to compute the optical absorption spectra of molecules and solids, which is suitable for the study of large systems and gives access to spectra within a wide energy range. In this approach, the quantum Liouville equation is solved iteratively within first order perturbation theory, with a Hamiltonian containing a static self-energy operator. This procedure is equivalent to solving the statically screened Bethe–Salpeter equation. Explicit calculations of single particle excited states and inversion of dielectric matrices are avoided using techniques based on density functional perturbation theory. In this way, full absorption spectra may be obtained with a computational workload comparable to ground state Hartree–Fock calculations. We present results for small molecules, for the spectra of a 1 nm Si cluster in a wide energy range (20 eV), and for a dipeptide exhibiting charge transfer excitations.

© 2010 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. METHOD
  3. ANALYSIS OF APPROXIMATIONS
    1. Tamm–Dancoff approximation
    2. Dynamical screening effects
    3. Choice of the quasiparticle ground state wave functions
  4. RESULTS
    1. Code verification
    2. Efficiency of the technique for computation of large systems
    3. Description of charge transfer excitations
  5. CONCLUSIONS

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KEYWORDS and PACS

Keywords

ab initio calculations, absorption coefficients, Bethe-Salpeter equation, charge exchange, density functional theory, excited states, ground states, HF calculations, Liouville equation, molecular biophysics, perturbation theory, silicon

PACS

  • 31.15.ap

    Polarizabilities and other atomic and molecular properties

  • 31.15.am

    Relativistic configuration interaction (CI) and many-body perturbation calculations

  • 31.15.E-

    Density-functional theory

  • 78.20.Ci

    Optical constants (including refractive index, complex dielectric constant, absorption, reflection and transmission coefficients, emissivity)

  • 31.15.xr

    Self-consistent-field methods

  • 87.15.-v

    Biomolecules: structure and physical properties

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3494540

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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