Molecular dynamics in shape space and femtosecond vibrational spectroscopy of metal clusters

TL;DR

This paper presents a novel molecular dynamics method in shape space for metal clusters, utilizing a deformable jellium model and shell correction, to explore ultrafast vibrational spectroscopy via femtosecond laser pulses.

Contribution

It introduces a new shape space molecular dynamics approach for metal clusters, combining a deformable jellium model with shell correction to study vibrational spectra.

Findings

Simulated Ag_14 cluster dynamics at finite temperature.

Demonstrated potential of ultrashort laser pulses for spectroscopy.

Showed shape vibrations can be probed with pump-probe techniques.

Abstract

We introduce a method of molecular dynamics in shape space aimed at metal clusters. The ionic degrees of freedom are described via a dynamically deformable jellium with inertia parameters derived from an incompressible, irrotational flow. The shell correction method is used to calculate the electronic potential energy surface underlying the dynamics. Our finite temperature simulations of Ag_14 and its ions, following the negative to neutral to positive scheme, demonstrate the potential of pump and probe ultrashort laser pulses as a spectroscopy of cluster shape vibrations.