Charge transfer in time-dependent density-functional theory via spin-symmetry breaking

Journal Article · Fri Apr 15 00:00:00 EDT 2011 · Physical Review. A

DOI:https://doi.org/10.1103/PHYSREVA.83.042501· OSTI ID:21544608

Fuks, Johanna I ^[1]; Rubio, Angel ^[1]; Maitra, Neepa T ^[2]

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1. Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Departamento de Fisica de Materiales, Universidad del Pais Vasco, CFM CSIC-UPV/EHU-MPC, and DIPC, Avenida Tolosa 72, E-20018 San Sebastian (Spain)
2. Department of Physics and Astronomy, Hunter College and City University of New York, 695 Park Avenue, New York, New York 10065 (United States)

Long-range charge-transfer excitations pose a major challenge for time-dependent density-functional approximations. We show that spin-symmetry breaking offers a simple solution for molecules composed of open-shell fragments, yielding accurate excitations at large separations when the acceptor effectively contains one active electron. Unrestricted exact-exchange and self-interaction-corrected functionals are performed on one-dimensional models and on the real LiH molecule within the pseudopotential approximation to demonstrate our results.

• OSTI ID: 21544608
• Journal Information: Physical Review. A, Vol. 83, Issue 4; Other Information: DOI: 10.1103/PhysRevA.83.042501; (c) 2011 American Institute of Physics; ISSN 1050-2947
• Country of Publication: United States
• Language: English

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
74 ATOMIC AND MOLECULAR PHYSICS
APPROXIMATIONS
DENSITY FUNCTIONAL METHOD
ELECTRONS
EXCITATION
FUNCTIONALS
INTERACTIONS
LITHIUM HYDRIDES
MATHEMATICAL SOLUTIONS
MOLECULES
ONE-DIMENSIONAL CALCULATIONS
POTENTIALS
SPIN
SYMMETRY BREAKING
TIME DEPENDENCE
ALKALI METAL COMPOUNDS
ANGULAR MOMENTUM
CALCULATION METHODS
ELEMENTARY PARTICLES
ENERGY-LEVEL TRANSITIONS
FERMIONS
FUNCTIONS
HYDRIDES
HYDROGEN COMPOUNDS
LEPTONS
LITHIUM COMPOUNDS
PARTICLE PROPERTIES
VARIATIONAL METHODS