Unified Finite-element Model for Transient Absorption and Raman Scattering of Vibrating Noble Metal Nanoparticles

TL;DR

This paper introduces a comprehensive finite-element modeling tool for simulating transient absorption and Raman scattering spectra of noble metal nanoparticles, accounting for geometry, composition, and vibrational effects.

Contribution

It presents a novel simulation framework that predicts spectra for various nanoparticle geometries and compositions, including local dielectric changes and vibrational amplitudes.

Findings

Successfully simulated spectra for gold and silver nanoparticles.

Able to fit experimental transient absorption amplitudes.

Predicted Raman spectra include previously neglected vibrational modes.

Abstract

Transient absorption and Raman scattering measurements on noble metal nanoparticles offer complimentary information on their vibrational modes and mechanical interactions with their surroundings. We have developed a comprehensive modeling tool for simulating both of these spectra based on COMSOL Multiphysics finite-element simulation software. This application can be used to predict the spectra for arbitrary geometries and metal compositions, takes into account local changes in dielectric function for the metals, and can model the small vibrational amplitudes of real transient absorption measurements. We present simulation results for gold and silver nanospheres, silver nanocubes, and gold truncated nanocubes, showing the ability to calculate relative peaks heights in Raman spectra and the ability to fit amplitudes of transient-absorption signals to experiment, and showing that Raman spectra can include contributions from modes often neglected due to symmetry considerations.