From discrete electronic states to plasmons

TDDFT optical absorption properties of Agn (n = 10, 20, 35, 56, 84, 120) tetrahedral clusters

Christine M. Aikens, Shuzhou Li, George C Schatz

Research output: Contribution to journalArticle

175 Citations (Scopus)

Abstract

Time-dependent density functional theory calculations are employed to calculate the optical absorption spectra of silver tetrahedral Agn (n = 10, 20, 35, 56, 84, 120) clusters with emphasis on neutral and ion clusters that correspond to shell closings. For the Ag20 cluster, the convergence properties of the spectra with respect to basis set and density functional are examined, and the most accurate results are found to be in good agreement with experimental data. The Agn spectra evolve from molecular-like to plasmon-like with increasing n, and from this we are able to extrapolate the plasmon energy and width to the large particle limit, leading to results that are in excellent agreement with continuum electrodynamics results. The results show that for the selected tetrahedral clusters, the plasmon width does not increase with decreasing cluster size as is commonly found (or assumed) for typical cluster shape distributions.

Original languageEnglish
Pages (from-to)11272-11279
Number of pages8
JournalJournal of Physical Chemistry C
Volume112
Issue number30
DOIs
Publication statusPublished - Jul 31 2008

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Plasmons
Electrodynamics
Electronic states
plasmons
Silver
Light absorption
Density functional theory
Absorption spectra
optical absorption
Ions
electronics
closing
electrodynamics
optical spectrum
silver
density functional theory
continuums
absorption spectra
ions

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

From discrete electronic states to plasmons : TDDFT optical absorption properties of Agn (n = 10, 20, 35, 56, 84, 120) tetrahedral clusters. / Aikens, Christine M.; Li, Shuzhou; Schatz, George C.

In: Journal of Physical Chemistry C, Vol. 112, No. 30, 31.07.2008, p. 11272-11279.

Research output: Contribution to journalArticle

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