Representation independent algorithms for molecular response calculations in time-dependent self-consistent field theories

Journal Article · Tue Jan 01 04:00:00 EST 2008 · Journal of Chemical Physics

OSTI ID:960966

Tretiak, Sergei ^[1]

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1. Los Alamos National Laboratory

Four different numerical algorithms suitable for a linear scaling implementation of time-dependent Hartree-Fock and Kohn-Sham self-consistent field theories are examined. We compare the performance of modified Lanczos, Arooldi, Davidson, and Rayleigh quotient iterative procedures to solve the random-phase approximation (RPA) (non-Hermitian) and Tamm-Dancoff approximation (TDA) (Hermitian) eigenvalue equations in the molecular orbital-free framework. Semiempirical Hamiltonian models are used to numerically benchmark algorithms for the computation of excited states of realistic molecular systems (conjugated polymers and carbon nanotubes). Convergence behavior and stability are tested with respect to a numerical noise imposed to simulate linear scaling conditions. The results single out the most suitable procedures for linear scaling large-scale time-dependent perturbation theory calculations of electronic excitations.

• Research Organization: Los Alamos National Laboratory (LANL)
• Sponsoring Organization: DOE
• DOE Contract Number: AC52-06NA25396
• OSTI ID: 960966
• Report Number(s): LA-UR-08-06811; LA-UR-08-6811
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
ALGORITHMS
APPROXIMATIONS
BENCHMARKS
CALCULATION METHODS
CARBON
COMPARATIVE EVALUATIONS
CONVERGENCE
DENSITY FUNCTIONAL METHOD
EIGENVALUES
EQUATIONS
EXCITED STATES
HAMILTONIANS
IMPLEMENTATION
NANOTUBES
NOISE
PERFORMANCE
PERTURBATION THEORY
POLYMERS
SCALING
SELF-CONSISTENT FIELD
STABILITY