Abstract

AbstractThe nonlinear scattering of a laser pulse off spherical nanoclusters with free electrons and with a diffuse surface is examined in the collisionless hydrodynamics approximation in the framework of perturbation theory with respect to the laser pulse intensity, as well as of the steady‐state approximation. In a previous publication [S.V. Fomichev and W. Becker, Phys. Rev. A 81, 063201 (2010)] we reported the full nonlinear hydrodynamic model of forced collective electron motion confined to a cluster with diffuse surface and introduced two different perturbation theories corresponding to different laser intensity regimes. In the current paper, in the framework of this hydrodynamic model we focus on the properties of plasmon resonance‐enhanced third‐harmonic generation in a spherical cluster and its dependence on the shape of its diffuse surface whose role increases for nonlinear processes. At the same time, the quadrupole second‐harmonic generation in a spherical cluster is also inspected as a necessary intermediate step. Both cold metal clusters in vacuum or in a dielectric surrounding and hot laser‐heated and laser‐ionized clusters are considered within the same approach for a wide range of the fundamental laser frequency. Nonlinear laser excitation of the dipole plasmon Mie resonance in spherical clusters, as well as of other respective multipole plasmon resonances is investigated analytically and numerically in detail (position, width, and strength) versus the cluster‐surface diffuseness, the outer ionization degree in charged clusters, the electron‐density diffuseness, and their interplay. Under certain conditions, depending on the various cluster parameters, different secondary nonlinear resonances are found. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Talk to us

Join us for a 30 min session where you can share your feedback and ask us any queries you have

Schedule a call

Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.