Photoabsorption Spectra of Na_n+ clusters: Thermal Line-Broadening Mechanisms

Abstract

Photoabsorption cross sections of small sodium cluster cations (Na${}_n^{+}$, n=3,5,7 and 9) were calculated at various temperatures with the time-dependent local-density-approximation (TDLDA) in conjunction with ab initio molecular dynamics simulations, yielding spectra that agree with measured ones without ad-hoc line broadening or renormalization. Three thermal line-broadening mechanisms are revealed: (I) lifting of level degeneracies caused by symmetry-breaking ionic motions, (II) oscillatory shifts of the entire spectrum caused by breathing vibrations, and (III) cluster structural isomerizations.

4 pages,2 figures, to appear in Phys. Rev. Lett

References in corpus (1)

• Fragmentation of the photoabsorption strength in neutral and charged metal microclusters

Cited by in corpus (12)

• Light scattering and surface plasmons on small spherical particles
• Calculation of the optical response of C60 and Na8 using time-dependent density functional theory and local orbitals
• Photoelectron spectra of anionic sodium clusters from time-dependent density-functional theory in real-time
• Dynamics of clusters and molecules in contact with an environment
• On the premelting features in sodium clusters
• Optical absorption by magnesia-supported gold clusters and nanocatalysts: effects from the support, cluster and adsorbants
• Theoretical study of finite temperature spectroscopy in van der Waals clusters. II Time-dependent absorption spectra
• Theoretical study of finite temperature spectroscopy in van der Waals clusters. I. Probing phase changes in CaAr_n
• Absolute absorption spectroscopy based on molecule interferometry
• Optical response of small closed-shell sodium clusters
• Photoabsorption in Sodium Clusters: First Principles Configuration Interaction Calculations
• Electron--phonon coupling and anharmonic effects in metal clusters