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American Chemical Society, ACS Nano, 3(10), p. 3835-3842, 2016

DOI: 10.1021/acsnano.6b00715

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Dissecting the Few-Femtosecond Dephasing Time of Dipole and Quadrupole Modes in Gold Nanoparticles Using Polarized Photoemission Electron Microscopy

Journal article published in 2016 by Quan Sun ORCID, Han Yu, Kosei Ueno, Atsushi Kubo, Yasutaka Matsuo, Hiroaki Misawa
This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

Dipole and quadrupole modes are the two lowest orders of localized surface plasmon resonance (LSPR) eigenmodes in metallic nanoparticles. Of these two modes, the quadrupole mode is forbidden for symmetric metallic nanoparticles excited by linearly polarized light at normal incidence. Here, we demonstrate excitation of the quadrupole mode in symmetrical gold (Au) nanoblocks shined with s-polarized light at oblique incidence. In particular, we probe the nearfield LSPR in Au nanoblocks using photoemission electron microscopy (PEEM) and find that at oblique incidence, the dipole and quadrupole modes can be selectively excited, in terms of nearfield enhancement, by manipulating the light polarization state. More importantly, by timeresolved PEEM measurements, we experimentally demonstrate that the quadrupole mode in symmetrical Au nanoblocks has longer dephasing time than that of the dipole mode.