Temporal Dynamics of Localized Exciton-Polaritons in Composite Organic-Plasmonic Metasurfaces

Elad Eizner; Katherine Akulov; Tal Schwartz; Tal Ellenbogen

doi:10.1021/acs.nanolett.7b03751

Temporal Dynamics of Localized Exciton-Polaritons in Composite Organic-Plasmonic Metasurfaces

Elad Eizner^*, Katherine Akulov, Tal Schwartz, Tal Ellenbogen

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton-plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton-plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.

Original language	English
Pages (from-to)	7675-7683
Number of pages	9
Journal	Nano Letters
Volume	17
Issue number	12
DOIs	https://doi.org/10.1021/acs.nanolett.7b03751
State	Published - 13 Dec 2017

Keywords

Plasmonics
aluminum nanoantennas
organic polaritons
strong coupling
temporal dynamics
ultrafast photonics

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10.1021/acs.nanolett.7b03751

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title = "Temporal Dynamics of Localized Exciton-Polaritons in Composite Organic-Plasmonic Metasurfaces",

abstract = "We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton-plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton-plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.",

keywords = "Plasmonics, aluminum nanoantennas, organic polaritons, strong coupling, temporal dynamics, ultrafast photonics",

author = "Elad Eizner and Katherine Akulov and Tal Schwartz and Tal Ellenbogen",

note = "Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

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doi = "10.1021/acs.nanolett.7b03751",

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AU - Eizner, Elad

AU - Akulov, Katherine

AU - Schwartz, Tal

AU - Ellenbogen, Tal

PY - 2017/12/13

Y1 - 2017/12/13

N2 - We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton-plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton-plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.

AB - We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton-plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton-plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.

KW - Plasmonics

KW - aluminum nanoantennas

KW - organic polaritons

KW - strong coupling

KW - temporal dynamics

KW - ultrafast photonics

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JO - Nano Letters

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Temporal Dynamics of Localized Exciton-Polaritons in Composite Organic-Plasmonic Metasurfaces

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Keywords

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