Kohn–Sham Time-Dependent Density Functional Theory with Applications to Linear and Nonlinear Properties
2006 (English)In: Nonlinear optical properties of matter: From molecules to condensed phases / [ed] Manthos G. Papadopoulos, Andrzej J. Sadlej, Jerzy Leszczynski., Springer Netherlands, 2006, 151-209 p.Chapter in book (Refereed)
We review Kohn–Sham density-functional theory for time-dependent response functionsup to and including cubic response. The working expressions are derived from anexplicit exponential parametrization of the density operator and the Ehrenfest principle,alternatively the quasi-energy ansatz. While the theory retains the adiabatic approximation,implying that the time-dependency of the functional is obtained only implicitly—through the time-dependency of the density itself rather than through the form ofthe exchange-correlation functionals—our implementation generalizes previous timedependentapproaches in that arbitrary functionals can be chosen for the perturbed densities(energy derivatives or response functions). Thus, the response of the density canalways be obtained using the stated density functional, or optionally different functionalscan be applied for the unperturbed and perturbed densities, even different functionals fordifferent response order. In particular, general density functionals beyond the local densityapproximation can be applied, such as hybrid functionals with exchange–correlation atthe generalized gradient-approximation level and fractional exact Hartree–Fock exchange.We also review some recent progress in time-dependent density functional theory foropen-shell systems, in particular spin-restricted and spin restricted-unrestricted formalismsfor property calculations. We highlight a sample of applications of the theory
Place, publisher, year, edition, pages
Springer Netherlands, 2006. 151-209 p.
, Challenges and Advances in Computational Chemistry and Physics, 1
IdentifiersURN: urn:nbn:se:kth:diva-90834DOI: 10.1007/1-4020-4850-5_5ISBN: 978-1-4020-4850-0OAI: oai:DiVA.org:kth-90834DiVA: diva2:506793
QC 201205252012-02-292012-02-292012-05-25Bibliographically approved