The Library
Linear-scaling time-dependent density-functional theory in the linear response formalism
Tools
Zuehlsdorff, T. J., Hine, Nicholas, Spencer, J. S., Harrison, Nicholas (Nicholas M.), Riley, D. J. and Haynes, Peter D. (2013) Linear-scaling time-dependent density-functional theory in the linear response formalism. Journal of Chemical Physics, 139 (6). 064104. doi:10.1063/1.4817330 ISSN 0021-9606.
|
PDF
WRAP_Hine_Linear-scaling_paper_revised.pdf - Accepted Version - Requires a PDF viewer. Download (3169Kb) | Preview |
Official URL: http://dx.doi.org/10.1063/1.4817330
Abstract
We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids any explicit reference to canonical representations of either occupied or virtual Kohn-Sham states and thus achieves linear-scaling computational effort with system size. In contrast to conventional localised orbital formulations, where a single set of localised functions is used to span the occupied and unoccupied state manifold, we make use of two sets of in situ optimised localised orbitals, one for the occupied and one for the unoccupied space. This double representation approach avoids known problems of spanning the space of unoccupied Kohn-Sham states with a minimal set of localised orbitals optimised for the occupied space, while the in situ optimisation procedure allows for efficient calculations with a minimal number of functions. The method is applied to a number of medium sized organic molecules and a good agreement with traditional TDDFT methods is observed. Furthermore, linear scaling of computational cost with system size is demonstrated on (10,0) carbon nanotubes of different lengths.
Item Type: | Journal Article | ||||
---|---|---|---|---|---|
Subjects: | Q Science > QD Chemistry | ||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||
Library of Congress Subject Headings (LCSH): | Excited state chemistry, Quantum chemistry, Density functionals, Mathematical physics, Nanostructures | ||||
Journal or Publication Title: | Journal of Chemical Physics | ||||
Publisher: | American Institute of Physics | ||||
ISSN: | 0021-9606 | ||||
Official Date: | 2013 | ||||
Dates: |
|
||||
Volume: | 139 | ||||
Number: | 6 | ||||
Article Number: | 064104 | ||||
DOI: | 10.1063/1.4817330 | ||||
Status: | Peer Reviewed | ||||
Publication Status: | Published | ||||
Access rights to Published version: | Open Access (Creative Commons) | ||||
Date of first compliant deposit: | 1 April 2016 | ||||
Date of first compliant Open Access: | 1 April 2016 | ||||
Funder: | Engineering and Physical Sciences Research Council (EPSRC) | ||||
Grant number: | EP/G036888/1, EP/G05567X/1, EP/J015059/1 |
Request changes or add full text files to a record
Repository staff actions (login required)
View Item |
Downloads
Downloads per month over past year