Localized surface plasmon resonance in silver nanoparticles: Atomistic first-principles time-dependent density-functional theory calculations

Abstract

We observe using ab initio methods that localized surface plasmon resonances in icosahedral silver nanoparticles enter the asymptotic region already between diameters of 1 and 2 nm, converging close to the classical quasistatic limit around 3.4 eV. We base the observation on time-dependent density-functional theory simulations of the icosahedral silver clusters Ag${}_{55}$ (1.06 nm), Ag${}_{147}$ (1.60 nm), Ag${}_{309}$ (2.14 nm), and Ag${}_{561}$ (2.68 nm). The simulation method combines the adiabatic GLLB-SC exchange-correlation functional with real time propagation in an atomic orbital basis set using the projector-augmented wave method. The method has been implemented for the electron structure code GPAW within the scope of this work. We obtain good agreement with experimental data and modeled results, including photoemission and plasmon resonance. Moreover, we can extrapolate the ab initio results to the classical quasistatically modeled icosahedral clusters.

8 pages, 5 figures

References in corpus (10)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Localized atomic basis set in the projector augmented wave method
• Kohn-Sham potential with discontinuity for band gap materials
• Symmetry and Electronic Structure of Noble Metal Nanoparticles and the Role of Relativity
• Optical response of small silver clusters
• Conventional and Acoustic Surface Plasmons on Noble Metal Surfaces: A Time-dependent Density Functional Theory Study
• Electronic shell structure and chemisorption on gold nanoparticles
• Photoabsorption by Volume Plasmons in Metal Nanoclusters
• Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets

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