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Title: Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials

In this study, we demonstrate that coherent acoustic phonons derived from plasmonic nanoparticles can modulate electronic interactions with proximal excitonic molecular species. A series of gold bipyramids with systematically varied aspect ratios and corresponding localized surface plasmon resonance energies, functionalized with a J-aggregated thiacarbocyanine dye molecule, produce two hybridized states that exhibit clear anti-crossing behavior with a Rabi splitting energy of 120 meV. In metal nanoparticles, photoexcitation generates coherent acoustic phonons that cause oscillations in the plasmon resonance energy. In the coupled system, these photo-generated 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 is consistent across a wide range of bipyramid ensembles. We also use Finite-Difference Time Domain calculations to develop a simple model describing this behavior. Lastly, such oscillatory plasmonic-excitonic nanomaterials (OPENs) offer a route to manipulate and dynamically-tune the interactions of plasmonic/excitonic systems and unlock a range of potential applications.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ; ORCiD logo [3] ;  [4] ; ORCiD logo [5] ; ORCiD logo [1] ; ORCiD logo [6]
  1. Northwestern Univ., Evanston, IL (United States). Department of Chemistry
  2. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Wuhan University (China). College of Chemistry and Molecular Sciences, Institute for Advanced Studies (IAS)
  3. Wuhan University (China). College of Chemistry and Molecular Sciences, Institute for Advanced Studies (IAS)
  4. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  5. Northwestern Univ., Evanston, IL (United States). Department of Chemistry; Argonne National Lab. (ANL), Lemont, IL (United States). Chemical Science and Engineering
  6. Northwestern Univ., Evanston, IL (United States). Department of Chemistry; Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; coherent acoustic phonons; Gold nanoparticles; plasmonic-excitonic coupling; time-resolved spectroscopy
OSTI Identifier:
1422405
Alternate Identifier(s):
OSTI ID: 1413069