Optical response of silver clusters and their hollow shells from linear-response TDDFT
MARCHESIN, Federico
Donostia International Physics Center [DIPC]
Centro de Fisica de Materiales [CFM]
Leer más >
Donostia International Physics Center [DIPC]
Centro de Fisica de Materiales [CFM]
MARCHESIN, Federico
Donostia International Physics Center [DIPC]
Centro de Fisica de Materiales [CFM]
Donostia International Physics Center [DIPC]
Centro de Fisica de Materiales [CFM]
SÁNCHEZ-PORTAL, Daniel
Centro de Fisica de Materiales [CFM]
Donostia International Physics Center [DIPC]
< Leer menos
Centro de Fisica de Materiales [CFM]
Donostia International Physics Center [DIPC]
Idioma
en
Article de revue
Este ítem está publicado en
Journal of Physics: Condensed Matter. 2016-06-05, vol. 28, n° 21, p. 214001 (1-21)
IOP Publishing
Resumen en inglés
We present a study of the optical response of compact and hollow icosahedral clusters containing up to 868 silver atoms by means of time-dependent density functional theory. We have studied the dependence on size and ...Leer más >
We present a study of the optical response of compact and hollow icosahedral clusters containing up to 868 silver atoms by means of time-dependent density functional theory. We have studied the dependence on size and morphology of both the sharp plasmonic resonance at 3-4 eV (originated mainly from $sp$-electrons), and the less studied broader feature appearing in the 6-7 eV range (interband transitions). An analysis of the effect of structural relaxations, as well as the choice of exchange correlation functional (local density versus generalized gradient approximations) both in the ground state and optical response calculations is also presented. We have further analysed the role of the different atom layers (surface versus inner layers) and the different orbital symmetries on the absorption cross-section for energies up to 8 eV. We have also studied the dependence on the number of atom layers in hollow structures. Shells formed by a single layer of atoms show a pronounced red shift of the main plasmon resonances that, however, rapidly converge to those of the compact structures as the number of layers is increased. The methods used to obtain these results are also carefully discussed. Our methodology is based on the use of localized basis (atomic orbitals, and atom-centered- and dominant- product functions), which bring several computational advantages related to their relatively small size and the sparsity of the resulting matrices. Furthermore, the use of basis sets of atomic orbitals also brings the possibility to extend some of the standard population analysis tools (e.g., Mulliken population analysis) to the realm of optical excitations. Some examples of these analyses are described in the present work.< Leer menos
Palabras clave en inglés
TDDFT
atomic orbitals
product basis
silver clusters
silver shells
GGA kernel
response function
Proyecto ANR
Prédiction par calcul numérique intensif du potentiel à circuit ouvert au sein de cellules photovoltaïques organiques.
Orígen
Importado de HalCentros de investigación