Dresden 2017 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 78: Electronic Structure Theory: New Concepts and Developments in Density Functional Theory and Beyond - V
O 78.5: Vortrag
Mittwoch, 22. März 2017, 16:00–16:15, GER 38
Insight into time-propagation TDDFT excitations via Kohn–Sham decomposition — •Tuomas P. Rossi1, Mikael Kuisma2,3, Martti J. Puska1, Risto M. Nieminen1, and Paul Erhart2 — 1Aalto University, Espoo, Finland — 2Chalmers University of Technology, Gothenburg, Sweden — 3University of Jyväskylä, Jyväskylä, Finland
The real-time-propagation formulation of time-dependent density-functional theory (RT-TDDFT) is an efficient method for calculating optical excitations of large molecules and nanoparticles. However, within RT-TDDFT, the analysis of the response is often limited to photoabsorption spectra and induced densities, in contrast to linear-response formulations of TDDFT, such as the Casida method, in which one can obtain further understanding on the basis of the Kohn–Sham electron-hole decomposition of the excitations.
In this work, we show that the Kohn–Sham decomposition
can be equivalently obtained from RT-TDDFT calculations.
We demonstrate the approach for the optical response of
organic molecules and large metallic nanoparticles.
The focus is especially on plasmonic applications,
for which the method enables the analysis in terms of transition contribution maps [1].
By using the decomposition, we can
shed light on the microscopic origin of plasmon resonances
and their damping via plasmon–single-electron coupling,
while retaining the favorable scaling of RT-TDDFT compared to linear-response formulations.
[1] S. Malola et al., ACS Nano 7, 10263 (2013).