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RESEARCH PRODUCT
TDDFT Analysis of Optical Properties of Thiol Monolayer-Protected Gold and Intermetallic Silver–Gold Au144(SR)60 and Au84Ag60(SR)60 Clusters
Hannu HäkkinenSami MalolaLauri Lehtovaarasubject
ta114ChemistryIntermetallicTime-dependent density functional theoryMolecular physicsSpectral lineSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsMetalDipoleGeneral Energyvisual_artMonolayervisual_art.visual_art_mediumDensity functional theoryPhysical and Theoretical ChemistrySurface plasmon resonanceAtomic physicsta116description
The optical absorption spectra of atomistic model structures for experimentally isolated all-gold Au144(SR)60 and intermetallic Au84Ag60(SR)60 clusters are systematically analyzed from linear-response time-dependent density functional theory (LR-TDDFT) and time-dependent density functional perturbation theory (TD-DFPT) calculations. The computed spectra, utilizing the atomistic model for Au144(SR)60 published by us in 2009, reproduce closely the experimental observations for corresponding isolated compounds, reported previously by Kumara and Dass in 2011. A collective dipole oscillation within the metal cores of the all-gold and intermetallic clusters is formed as response to light in the visible range. The weight of the oscillation and especially the screening by Au(5d) electrons are shifted gradually closer to the metal/ligand interface as the excitation energy is increased, but none of these clusters supports formation of a localized surface plasmon resonance. Based on the comparison of calculated spec...
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2014-08-13 | The Journal of Physical Chemistry C |