Temporal dynamics of strongly coupled exciton-localized surface plasmons beyond Rabi oscillations

Elad Eizner, Katherine Akulov, Tal Schwartz, Tal Ellenbogen

Research output: Chapter in Book/Report/Conference proceedingConference contributionpeer-review

Abstract

Strong coupling between excitons and light leads to the formation of hybrid states with mixed properties of light and matter. As a result, interesting physical phenomena have been observed at room temperature, e.g. Bose-Einstein condensation and superfluidity, and novel applications are emerging, such as low threshold lasers and quantum devices. Recently it was shown that metasurfaces of aluminum nanoantennas coated with molecular J-aggregates can provide an excellent platform for the formation of strongly coupled exciton-localized surface plasmons (X-LSPs). However, their optical nonlinearities and temporal dynamics are still not well understood. In this work, we use femtosecond pump-probe spectroscopy to study X-LSPs in such composite Al/molecular metasurfaces on time scales that are longer than their Rabi oscillation period. We study the linear and nonlinear optical properties of the uncoupled and hybrid systems and find that the nanoscale plasmonic confinement in metallic nanoparticle cavities introduces intriguing new ultrafast phenomena in the strong coupling regime. These include modifications of the hybrid system due to femtosecond changes in the molecular environment, picosecond oscillations due to acoustic breathing modes of the nanoantennas, and long relaxation times of the nonlinear perturbation at the upper X-LSPs frequency band.

Original languageEnglish
Title of host publicationNanophotonics VII
EditorsDavid L. Andrews, Andreas Ostendorf, Angus J. Bain, Jean-Michel Nunzi
PublisherSPIE
ISBN (Electronic)9781510618701
DOIs
StatePublished - 2018
EventNanophotonics VII 2018 - Strasbourg, France
Duration: 22 Apr 201826 Apr 2018

Publication series

NameProceedings of SPIE - The International Society for Optical Engineering
Volume10672
ISSN (Print)0277-786X
ISSN (Electronic)1996-756X

Conference

ConferenceNanophotonics VII 2018
Country/TerritoryFrance
CityStrasbourg
Period22/04/1826/04/18

Keywords

  • Aluminum Nanoantennas
  • Organic Polaritons
  • Plasmonics
  • Strong Coupling
  • Temporal Dynamics
  • Ultrafast Photonics

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