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:

Kirschner, Matthew S. ^[1]; Ding, Wendu ^[1]; Li, Yuxiu ^[2]; Chapman, Craig T. ^[1]; Lei, Aiwen  ^[3];

• Search DOE PAGES for author "Lei, Aiwen"
• Search DOE PAGES for ORCID "0000-0001-8417-3061"

Lin, Xiao-Min ^[4]; Chen, Lin X.  ^[5];

• Search DOE PAGES for author "Chen, Lin X."
• Search DOE PAGES for ORCID "0000-0002-8450-6687"

Schatz, George C.  ^[1];

• Search DOE PAGES for author "Schatz, George C."
• Search DOE PAGES for ORCID "0000-0001-5837-4740"

Schaller, Richard D.  ^[6]

• Search DOE PAGES for author "Schaller, Richard D."
• Search DOE PAGES for ORCID "0000-0001-9696-8830"

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+ Show Author Affiliations

1. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
2. 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
3. College of Chemistry and Molecular Sciences, Institute for Advanced Studies (IAS), Wuhan University, Wuhan 430072, People’s Republic of China
4. Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, United States
5. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States, Chemical Science and Engineering, Argonne National Laboratory, Lemont, Illinois 60439, United States
6. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States, Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, United States

Publication Date:

Fri Dec 01 00:00:00 EST 2017

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1413069

Alternate Identifier(s):

OSTI ID: 1422405

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Published Article

Journal Name:

Nano Letters

Additional Journal Information:

Journal Name: Nano Letters 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