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Electron dynamics with real‐time time‐dependent density functional theory
Author(s) -
Provorse Makenzie R.,
Isborn Christine M.
Publication year - 2016
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.25096
Subject(s) - time dependent density functional theory , physics , adiabatic process , density functional theory , electron , picosecond , nonlinear system , statistical physics , ground state , time domain , dynamics (music) , density matrix , computational physics , quantum mechanics , computer science , laser , quantum , acoustics , computer vision
Real‐time time‐dependent functional theory (RT‐TDDFT) directly propagates the electron density in the time domain by integrating the time‐dependent Kohn–Sham equations. This is in contrast to the popular linear response TDDFT matrix formulation that computes transition frequencies from a ground state reference. RT‐TDDFT is, therefore, a potentially powerful technique for modeling atto‐ to picosecond electron dynamics, including charge transfer pathways, the response to a specific applied field, and frequency dependent linear and nonlinear properties. However, qualitatively incorrect electron dynamics and time‐dependent resonant frequencies can occur when perturbing the density away from the ground state due to the common adiabatic approximation. An overview of the RT‐TDDFT method is provided here, including examples of some cases that lead to this qualitatively incorrect behavior. © 2016 Wiley Periodicals, Inc.