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Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials Matthew S. Kirschner† , Wendu Ding† , Yuxiu Li ‡§ , Craig T. Chapman† +, Aiwen Lei § , Xiao-Min Lin‡ , Lin X. Chen† , George C. Schatz † , and Richard D. Schaller*†‡ † Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States ‡ Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, United States § College of Chemistry and Molecular Sciences, Institute for Advanced Studies (IAS), Wuhan University, Wuhan 430072, People’s Republic of China Chemical Science and Engineering, Argonne National Laboratory, Lemont, Illinois 60439, United States
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Nano Lett., 2018, 18 (1), pp 442–448 DOI: 10.1021/acs.nanolett.7b04354 Publication Date (Web): December 1, 2017 Copyright © 2017 American Chemical Society *E-mail:
[email protected];
[email protected].
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We demonstrate that coherent acoustic phonons derived from plasmonic nanoparticles can Retrieve Detailed Record of this Article
modulate electronic interactions with proximal excitonic molecular species. A series of gold bipyramids with systematically varied aspect ratios and corresponding localized surface plasmon
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resonance energies, functionalized with a J-aggregated thiacarbocyanine dye molecule,
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produces two hybridized states that exhibit clear anticrossing behavior with a Rabi splitting energy of 120 meV. In metal nanoparticles, photoexcitation generates coherent acoustic
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phonons that cause oscillations in the plasmon resonance energy. In the coupled system, these
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photogenerated oscillations alter the metal nanoparticle’s energetic contribution to the hybridized system and, as a result, change the coupling between the plasmon and exciton. We demonstrate that such modulations in the hybridization are consistent across a wide range of bipyramid ensembles. We also use finite-difference time domain calculations to develop a simple
Kirschner, Matthew S.
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model describing this behavior. Such oscillatory plasmonic-excitonic nanomaterials offer a route to manipulate and dynamically tune the interactions of plasmonic/excitonic systems and unlock a
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range of potential applications. Keywords: coherent acoustic phonons; Gold nanoparticles; plasmonic-excitonic coupling; timeresolved spectroscopy
Article Views: 945 Times Received 11 October 2017 Published online 1 December 2017 Published in print 10 January 2018
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