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Title: Electronic and optical properties of pure and modified diamondoids studied by many-body perturbation theory and time-dependent density functional theory

Diamondoids are small diamond nanoparticles (NPs) that are built up from diamond cages. Unlike usual semiconductor NPs, their atomic structure is exactly known, thus they are ideal test-beds for benchmarking quantum chemical calculations. Their usage in spintronics and bioimaging applications requires a detailed knowledge of their electronic structure and optical properties. In this paper, we apply density functional theory (DFT) based methods to understand the electronic and optical properties of a few selected pure and modified diamondoids for which accurate experimental data exist. In particular, we use many-body perturbation theory methods, in the G{sub 0}W{sub 0} and G{sub 0}W{sub 0}+BSE approximations, and time-dependent DFT in the adiabatic local density approximation. We find large quasiparticle gap corrections that can exceed thrice the DFT gap. The electron-hole binding energy can be as large as 4 eV but it is considerably smaller than the GW corrections and thus G{sub 0}W{sub 0}+BSE optical gaps are about 50% larger than the Kohn-Sham (KS) DFT gaps. We find significant differences between KS time-dependent DFT and GW+BSE optical spectra on the selected diamondoids. The calculated G{sub 0}W{sub 0} quasiparticle levels agree well with the corresponding experimental vertical ionization energies. We show that nuclei dynamics in the ionizationmore » process can be significant and its contribution may reach about 0.5 eV in the adiabatic ionization energies.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [2]
  1. Institute of Physics, Loránd Eötvös University, Pázmány Péter sétány 1/A, H-1117 Budapest (Hungary)
  2. (Hungary)
  3. Department of Atomic Physics, Budapest University of Technology and Economics, Budafoki út 8., H-1111 Budapest (Hungary)
  4. Dipartimento di Fisica, Universitá di Roma “Tor Vergata”, Via della Ricerca Scientifica 1, 00133 Roma (Italy)
  5. Institute for Solid State Physics and Optics, Wigner Research Center for Physics, Hungarian Academy of Sciences, P.O. Box 49, H-1525 Budapest (Hungary)
Publication Date:
OSTI Identifier:
22420025
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 141; Journal Issue: 6; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BINDING ENERGY; DENSITY; DENSITY FUNCTIONAL METHOD; ELECTRONIC STRUCTURE; EV RANGE; IONIZATION; NANOPARTICLES; OPTICAL PROPERTIES; PERTURBATION THEORY; SPECTRA; TIME DEPENDENCE