title: Time-Dependent Extension of the Long-Range Corrected Density Functional Based Tight-Binding Method.
abstract: We present a consistent linear response formulation of the density functional based tight-binding method for long-range corrected exchange-correlation functionals (LC-DFTB). Besides a detailed account of derivation and implementation of the method, we also test the new scheme on a variety of systems considered to be problematic for conventional local/semilocal time-dependent density functional theory (TD-DFT). To this class belong the optical properties of polyacenes and nucleobases, as well as charge transfer excited states in molecular dimers. We find that the approximate LC-DFTB method exhibits the same general trends and similar accuracy as range-separated DFT methods at significantly reduced computational cost. The scheme should be especially useful in the determination of the electronic excited states of very large molecules, for which conventional TD-DFT is supposed to fail due to a multitude of artificial low energy states.
authors.affiliation: Institute of Physical Chemistry and Institute of Biological Interfaces (IBG-2), Karlsruhe Institute of Technology , Kaiserstrasse 12, 76131 Karlsruhe, Germany.
authors.forename: Julian J
authors.initials: JJ
authors.lastname: Kranz
authors.affiliation: Institute of Physical Chemistry and Institute of Biological Interfaces (IBG-2), Karlsruhe Institute of Technology , Kaiserstrasse 12, 76131 Karlsruhe, Germany.
authors.forename: Marcus
authors.initials: M
authors.lastname: Elstner
authors.affiliation: BCCMS, University of Bremen , 28359 Bremen, Germany.
authors.forename: Bálint
authors.initials: B
authors.lastname: Aradi
authors.affiliation: BCCMS, University of Bremen , 28359 Bremen, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Frauenheim
authors.affiliation: Department of Theoretical Physics, University of Regensburg , 93040 Regensburg, Germany.
authors.forename: Vitalij
authors.initials: V
authors.lastname: Lutsker
authors.affiliation: Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science, Luruper Chaussee 149, 22761 Hamburg, Germany.
authors.forename: Adriel Dominguez
authors.initials: AD
authors.lastname: Garcia
authors.affiliation: Université Lyon, Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière, F-69622 Lyon, France.
authors.forename: Thomas A
authors.identifier: http://orcid.org/0000-0001-9576-7658
authors.initials: TA
authors.lastname: Niehaus
mesh_terms: D001665:Binding Sites; D009705:Nucleosides / Q000737:chemistry*; D011108:Polymers / Q000737:chemistry*; D011789:Quantum Theory; D013997:Time Factors
chemical_list: D009705:Nucleosides; D011108:Polymers