Polarization-resolved ultrafast dynamics of the complex polarizability in single gold nanoparticles

Masia, Francesco ORCID: https://orcid.org/0000-0003-4958-410X, Langbein, Wolfgang Werner ORCID: https://orcid.org/0000-0001-9786-1023 and Borri, Paola ORCID: https://orcid.org/0000-0002-7873-3314 2013. Polarization-resolved ultrafast dynamics of the complex polarizability in single gold nanoparticles. Physical Chemistry Chemical Physics 15 (12) , pp. 4226-4232. 10.1039/C2CP43451B

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Abstract

Using a phase-sensitive degenerate four-wave mixing technique in heterodyne detection we measured the ultrafast changes of the complex polarizability in single gold nanoparticles at the surface plasmon resonance. Two components in the nanoparticle nonlinear response are distinguished, depending on the linear polarization direction of pump and probe pulses and particle geometry. One component is quantitatively modeled as the variation of the complex dielectric constant induced by the initial increase in the electron gas temperature following the absorption of the pump pulse, and the subsequent electron thermalization with the lattice and the surrounding. The dependence of the measured four-wave mixing on the probe field polarization direction is well reproduced by including a deviation from spherical symmetry in the nanoparticle dielectric constant. The second component manifests as a significant increase in the measured nonlinearity when the probe field is co-polarized with the pump field at pump–probe time overlap. We attribute this component to the nonlinear response from coherent surface plasmons before dephasing into single electron excitations.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Biosciences Physics and Astronomy
Subjects:	Q Science > QC Physics
Publisher:	Royal Society of Chemistry
ISSN:	1463-9076
Funders:	BBSRC, EPSRC
Last Modified:	10 Jul 2024 19:15
URI:	https://orca.cardiff.ac.uk/id/eprint/48753

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