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Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials.

Matthew S Kirschner¹, Wendu Ding¹, Yuxiu Li^2,3

¹Department of Chemistry, Northwestern University , Evanston, Illinois 60208, United States.

|December 2, 2017

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Coherent acoustic phonons from plasmonic nanoparticles dynamically tune exciton interactions. This creates tunable plasmonic-excitonic nanomaterials for advanced applications.

Area of Science:

Nanophotonics and Molecular Plasmonics

Background:

Plasmonic nanoparticles exhibit localized surface plasmon resonance (LSPR) that can couple with molecular excitons.
Coherent acoustic phonons (CAPs) in metal nanoparticles can oscillate LSPR frequencies upon photoexcitation.

Purpose of the Study:

To investigate the modulation of plasmon-exciton interactions using CAPs generated in plasmonic nanoparticles.
To explore the potential of dynamically tuning these hybrid systems for novel applications.

Main Methods:

Fabrication of gold bipyramids with varying aspect ratios to tune LSPR.
Functionalization of nanoparticles with J-aggregated thiacarbocyanine dye molecules to form hybrid systems.
Spectroscopic analysis to observe anticrossing behavior and Rabi splitting.
Finite-difference time-domain (FDTD) calculations to model the observed phenomena.

Keywords:

Gold nanoparticles coherent acoustic phonons plasmonic-excitonic coupling time-resolved spectroscopy

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Main Results:

Observation of two hybridized plasmon-exciton states with clear anticrossing behavior.
Quantification of a Rabi splitting energy of 120 meV in the coupled system.
Demonstration that CAP-induced LSPR oscillations modulate the plasmon-exciton coupling.
Consistency of modulation across various bipyramid ensembles.

Conclusions:

Coherent acoustic phonons effectively modulate plasmon-exciton coupling in hybrid nanomaterials.
This dynamic tuning mechanism offers a pathway for controlling light-matter interactions.
Developed oscillatory plasmonic-excitonic nanomaterials show promise for diverse applications in nanophotonics and beyond.