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Title: Quasi-particle energy spectra in local reduced density matrix functional theory

Recently, we introduced [N. N. Lathiotakis, N. Helbig, A. Rubio, and N. I. Gidopoulos, Phys. Rev. A 90, 032511 (2014)] local reduced density matrix functional theory (local RDMFT), a theoretical scheme capable of incorporating static correlation effects in Kohn-Sham equations. Here, we apply local RDMFT to molecular systems of relatively large size, as a demonstration of its computational efficiency and its accuracy in predicting single-electron properties from the eigenvalue spectrum of the single-particle Hamiltonian with a local effective potential. We present encouraging results on the photoelectron spectrum of molecular systems and the relative stability of C{sub 20} isotopes. In addition, we propose a modelling of the fractional occupancies as functions of the orbital energies that further improves the efficiency of the method useful in applications to large systems and solids.
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, Vass. Constantinou 48, GR-11635 Athens (Greece)
  2. Peter-Grünberg Institut and Institute for Advanced Simulation, Forschungszentrum Jülich, D-52425 Jülich (Germany)
  3. Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Dpto. Física de Materiales, Universidad del País Vasco, CFM CSIC-UPV/EHU-MPC and DIPC, Av. Tolosa 72, E-20018 San Sebastián (Spain)
  4. Department of Physics, Durham University, South Road, Durham DH1 3LE (United Kingdom)
Publication Date:
OSTI Identifier:
22310737
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 141; Journal Issue: 16; 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; ACCURACY; DENSITY MATRIX; EFFICIENCY; EIGENVALUES; ELECTRONS; ENERGY SPECTRA; HAMILTONIANS; ISOTOPES; PARTICLES; PHOTOELECTRON SPECTROSCOPY; QUASI PARTICLES; SIMULATION; SOLIDS