Kohn-Sham Decomposition in Real-Time Time-Dependent Density-Functional Theory: An Efficient Tool for Analyzing Plasmonic Excitations

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Kohn-Sham Decomposition in Real-Time Time-Dependent Density-Functional Theory : An Efficient Tool for Analyzing Plasmonic Excitations. / Rossi, Tuomas P.; Kuisma, Mikael; Puska, Martti J.; Nieminen, Risto M.; Erhart, Paul.

julkaisussa: Journal of Chemical Theory and Computation, Vuosikerta 13, Nro 10, 10.10.2017, s. 4779-4790.

Tutkimustuotos: Lehtiartikkelivertaisarvioitu

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Bibtex - Lataa

@article{8c8d45c9246f40f8930874e8b52450d2,
title = "Kohn-Sham Decomposition in Real-Time Time-Dependent Density-Functional Theory: An Efficient Tool for Analyzing Plasmonic Excitations",
abstract = "Electronic excitations can be efficiently analyzed in terms of the underlying Kohn-Sham (KS) electron-hole transitions. While such a decomposition is readily available in the linear-response time-dependent density-functional theory (TDDFT) approaches based on the Casida equations, a comparable analysis is less commonly conducted within the real-time-propagation TDDFT (RT-TDDFT). To improve this situation, we present here an implementation of a KS decomposition tool within the local-basis-set RT-TDDFT code in the free GPAW package. Our implementation is based on postprocessing of data that is readily available during time propagation, which is important for retaining the efficiency of the underlying RT-TDDFT to large systems. After benchmarking our implementation on small benzene derivatives by explicitly reconstructing the Casida eigenvectors from RT-TDDFT, we demonstrate the performance of the method by analyzing the plasmon resonances of icosahedral silver nanoparticles up to Ag561. The method provides a clear description of the splitting of the plasmon in small nanoparticles due to individual single-electron transitions as well as the formation of a distinct d-electron-screened plasmon resonance in larger nanoparticles.",
author = "Rossi, {Tuomas P.} and Mikael Kuisma and Puska, {Martti J.} and Nieminen, {Risto M.} and Paul Erhart",
year = "2017",
month = "10",
day = "10",
doi = "10.1021/acs.jctc.7b00589",
language = "English",
volume = "13",
pages = "4779--4790",
journal = "Journal of Chemical Theory and Computation",
issn = "1549-9618",
publisher = "AMERICAN CHEMICAL SOCIETY",
number = "10",

}

RIS - Lataa

TY - JOUR

T1 - Kohn-Sham Decomposition in Real-Time Time-Dependent Density-Functional Theory

T2 - An Efficient Tool for Analyzing Plasmonic Excitations

AU - Rossi, Tuomas P.

AU - Kuisma, Mikael

AU - Puska, Martti J.

AU - Nieminen, Risto M.

AU - Erhart, Paul

PY - 2017/10/10

Y1 - 2017/10/10

N2 - Electronic excitations can be efficiently analyzed in terms of the underlying Kohn-Sham (KS) electron-hole transitions. While such a decomposition is readily available in the linear-response time-dependent density-functional theory (TDDFT) approaches based on the Casida equations, a comparable analysis is less commonly conducted within the real-time-propagation TDDFT (RT-TDDFT). To improve this situation, we present here an implementation of a KS decomposition tool within the local-basis-set RT-TDDFT code in the free GPAW package. Our implementation is based on postprocessing of data that is readily available during time propagation, which is important for retaining the efficiency of the underlying RT-TDDFT to large systems. After benchmarking our implementation on small benzene derivatives by explicitly reconstructing the Casida eigenvectors from RT-TDDFT, we demonstrate the performance of the method by analyzing the plasmon resonances of icosahedral silver nanoparticles up to Ag561. The method provides a clear description of the splitting of the plasmon in small nanoparticles due to individual single-electron transitions as well as the formation of a distinct d-electron-screened plasmon resonance in larger nanoparticles.

AB - Electronic excitations can be efficiently analyzed in terms of the underlying Kohn-Sham (KS) electron-hole transitions. While such a decomposition is readily available in the linear-response time-dependent density-functional theory (TDDFT) approaches based on the Casida equations, a comparable analysis is less commonly conducted within the real-time-propagation TDDFT (RT-TDDFT). To improve this situation, we present here an implementation of a KS decomposition tool within the local-basis-set RT-TDDFT code in the free GPAW package. Our implementation is based on postprocessing of data that is readily available during time propagation, which is important for retaining the efficiency of the underlying RT-TDDFT to large systems. After benchmarking our implementation on small benzene derivatives by explicitly reconstructing the Casida eigenvectors from RT-TDDFT, we demonstrate the performance of the method by analyzing the plasmon resonances of icosahedral silver nanoparticles up to Ag561. The method provides a clear description of the splitting of the plasmon in small nanoparticles due to individual single-electron transitions as well as the formation of a distinct d-electron-screened plasmon resonance in larger nanoparticles.

UR - http://www.scopus.com/inward/record.url?scp=85031023846&partnerID=8YFLogxK

U2 - 10.1021/acs.jctc.7b00589

DO - 10.1021/acs.jctc.7b00589

M3 - Article

VL - 13

SP - 4779

EP - 4790

JO - Journal of Chemical Theory and Computation

JF - Journal of Chemical Theory and Computation

SN - 1549-9618

IS - 10

ER -

ID: 15848104