Kohn-Sham Decomposition in Real-Time Time-Dependent Density-Functional Theory An Efficient Tool for Analyzing Plasmonic Excitations
| Autor: | Paul Erhart, Tuomas P. Rossi, Mikael Kuisma, Risto M. Nieminen, Martti J. Puska |
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| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
plasmonic excitations
Theoretical computer science Kohn-Sham decomposition Computer science ta221 Kohn–Sham equations FOS: Physical sciences Physics::Optics 02 engineering and technology 01 natural sciences Physics - Chemical Physics 0103 physical sciences Mesoscale and Nanoscale Physics (cond-mat.mes-hall) Decomposition (computer science) Physics::Atomic and Molecular Clusters Statistical physics Physical and Theoretical Chemistry Physics::Chemical Physics 010306 general physics ta116 Plasmon Eigenvalues and eigenvectors Chemical Physics (physics.chem-ph) Condensed Matter - Materials Science Condensed Matter - Mesoscale and Nanoscale Physics ta114 tiheysfunktionaaliteoria Materials Science (cond-mat.mtrl-sci) Time-dependent density functional theory 16. Peace & justice 021001 nanoscience & nanotechnology Computer Science Applications plasmonit Benzene derivatives nanohiukkaset 0210 nano-technology |
| Zdroj: | JOURNAL OF CHEMICAL THEORY AND COMPUTATION. 13(10):4779-4790 |
| ISSN: | 1549-9618 |
| Popis: | The real-time-propagation formulation of time-dependent density-functional theory (RT-TDDFT) is an efficient method for modeling the optical response of molecules and nanoparticles. Compared to the widely adopted linear-response TDDFT approaches based on, e.g., the Casida equations, RT-TDDFT appears, however, lacking efficient analysis methods. This applies in particular to a decomposition of the response in the basis of the underlying single-electron states. In this work, we overcome this limitation by developing an analysis method for obtaining the Kohn-Sham electron-hole decomposition in RT-TDDFT. We demonstrate the equivalence between the developed method and the Casida approach by a benchmark on small benzene derivatives. Then, we use the method for analyzing the plasmonic response of icosahedral silver nanoparticles up to Ag$_{561}$. Based on the analysis, we conclude that in small nanoparticles individual single-electron transitions can split the plasmon into multiple resonances due to strong single-electron-plasmon coupling whereas in larger nanoparticles a distinct plasmon resonance is formed. 11 pages, 3 figures |
| Databáze: | OpenAIRE |
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