skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials

Abstract

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:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1422405
Alternate Identifier(s):
OSTI ID: 1413069
Grant/Contract Number:
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
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

Citation Formats

Kirschner, Matthew S., Ding, Wendu, Li, Yuxiu, Chapman, Craig T., Lei, Aiwen, Lin, Xiao-Min, Chen, Lin X., Schatz, George C., and Schaller, Richard D. Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b04354.
Kirschner, Matthew S., Ding, Wendu, Li, Yuxiu, Chapman, Craig T., Lei, Aiwen, Lin, Xiao-Min, Chen, Lin X., Schatz, George C., & Schaller, Richard D. Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials. United States. doi:10.1021/acs.nanolett.7b04354.
Kirschner, Matthew S., Ding, Wendu, Li, Yuxiu, Chapman, Craig T., Lei, Aiwen, Lin, Xiao-Min, Chen, Lin X., Schatz, George C., and Schaller, Richard D. Fri . "Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials". United States. doi:10.1021/acs.nanolett.7b04354.
@article{osti_1422405,
title = {Phonon-Driven Oscillatory Plasmonic Excitonic Nanomaterials},
author = {Kirschner, Matthew S. and Ding, Wendu and Li, Yuxiu and Chapman, Craig T. and Lei, Aiwen and Lin, Xiao-Min and Chen, Lin X. and Schatz, George C. and Schaller, Richard D.},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.7b04354},
journal = {Nano Letters},
number = 1,
volume = 18,
place = {United States},
year = {Fri Dec 01 00:00:00 EST 2017},
month = {Fri Dec 01 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on December 1, 2018
Publisher's Version of Record

Save / Share: