Representation independent algorithms for molecular response calculations in time-dependent self-consistent field theories.
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.
Tretiak
Sergei
S
Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA. serg@lanl.gov
Isborn
Christine M
CM
Niklasson
Anders M N
AM
Challacombe
Matt
M