Skip to main content
  • Submit
  • About
    • Editorial Board
    • PNAS Staff
    • FAQ
    • Rights and Permissions
    • Site Map
  • Contact
  • Journal Club
  • Subscribe
    • Subscription Rates
    • Subscriptions FAQ
    • Open Access
    • Recommend PNAS to Your Librarian
  • Log in
  • My Cart

Main menu

  • Home
  • Articles
    • Current
    • Latest Articles
    • Special Features
    • Colloquia
    • Collected Articles
    • PNAS Classics
    • Archive
  • Front Matter
  • News
    • For the Press
    • Highlights from Latest Articles
    • PNAS in the News
  • Podcasts
  • Authors
    • Information for Authors
    • Purpose and Scope
    • Editorial and Journal Policies
    • Submission Procedures
    • For Reviewers
    • Author FAQ
  • Submit
  • About
    • Editorial Board
    • PNAS Staff
    • FAQ
    • Rights and Permissions
    • Site Map
  • Contact
  • Journal Club
  • Subscribe
    • Subscription Rates
    • Subscriptions FAQ
    • Open Access
    • Recommend PNAS to Your Librarian

User menu

  • Log in
  • My Cart

Search

  • Advanced search
Home
Home

Advanced Search

  • Home
  • Articles
    • Current
    • Latest Articles
    • Special Features
    • Colloquia
    • Collected Articles
    • PNAS Classics
    • Archive
  • Front Matter
  • News
    • For the Press
    • Highlights from Latest Articles
    • PNAS in the News
  • Podcasts
  • Authors
    • Information for Authors
    • Purpose and Scope
    • Editorial and Journal Policies
    • Submission Procedures
    • For Reviewers
    • Author FAQ

New Research In

Physical Sciences

Featured Portals

  • Physics
  • Chemistry
  • Sustainability Science

Articles by Topic

  • Applied Mathematics
  • Applied Physical Sciences
  • Astronomy
  • Computer Sciences
  • Earth, Atmospheric, and Planetary Sciences
  • Engineering
  • Environmental Sciences
  • Mathematics
  • Statistics

Social Sciences

Featured Portals

  • Anthropology
  • Sustainability Science

Articles by Topic

  • Economic Sciences
  • Environmental Sciences
  • Political Sciences
  • Psychological and Cognitive Sciences
  • Social Sciences

Biological Sciences

Featured Portals

  • Sustainability Science

Articles by Topic

  • Agricultural Sciences
  • Anthropology
  • Applied Biological Sciences
  • Biochemistry
  • Biophysics and Computational Biology
  • Cell Biology
  • Developmental Biology
  • Ecology
  • Environmental Sciences
  • Evolution
  • Genetics
  • Immunology and Inflammation
  • Medical Sciences
  • Microbiology
  • Neuroscience
  • Pharmacology
  • Physiology
  • Plant Biology
  • Population Biology
  • Psychological and Cognitive Sciences
  • Sustainability Science
  • Systems Biology

Lifetime dynamics of plasmons in the few-atom limit

Kyle D. Chapkin, Luca Bursi, Grant J. Stec, Adam Lauchner, Nathaniel J. Hogan, Yao Cui, Peter Nordlander, and Naomi J. Halas
PNAS September 11, 2018 115 (37) 9134-9139; published ahead of print August 27, 2018 https://doi.org/10.1073/pnas.1805357115
Kyle D. Chapkin
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Luca Bursi
bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;cDepartment of Physics and Astronomy, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Grant J. Stec
bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;dDepartment of Chemistry, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Adam Lauchner
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Nathaniel J. Hogan
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Yao Cui
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Peter Nordlander
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;cDepartment of Physics and Astronomy, Rice University, Houston, TX 77005;eDepartment of Material Science and Nanoengineering, Rice University, Houston, TX 77005
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
  • ORCID record for Peter Nordlander
Naomi J. Halas
aDepartment of Electrical and Computer Engineering, Rice University, Houston, TX 77005;bLaboratory for Nanophotonics, Rice University, Houston, TX 77005;cDepartment of Physics and Astronomy, Rice University, Houston, TX 77005;dDepartment of Chemistry, Rice University, Houston, TX 77005;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
  • For correspondence: halas@rice.edu
  1. Contributed by Naomi J. Halas, July 24, 2018 (sent for review March 28, 2018; reviewed by Christine M. Aikens and Dmitri N. Basov)

  • Article
  • Figures & SI
  • Info & Metrics
  • PDF
Loading

This article requires a subscription to view the full text. If you have a subscription you may use the login form below to view the article. Access to this article can also be purchased.

Significance

In this work, we study collective electronic excitations—plasmons—in the few-atom limit in charged polycyclic aromatic hydrocarbon (PAH) molecules. These systems are the zero-dimensional limit of graphene, consisting of only a few fused aromatic carbon rings where the perimeter atoms are bonded to hydrogen. As systems identified as supporting plasmons, established by the transfer of a single electron to or from the neutral PAH molecule, they are perhaps the most optimal examples where a clear distinction between plasmons and single electron–hole pair excitations can be rigorously made. Here, we study the lifetime dynamics of charged versus neutral PAH molecules to characterize the relaxation channels in these quantum plasmon systems.

Abstract

Polycyclic aromatic hydrocarbon (PAH) molecules are essentially graphene in the subnanometer limit, typically consisting of 50 or fewer atoms. With the addition or removal of a single electron, these molecules can support molecular plasmon (collective) resonances in the visible region of the spectrum. Here, we probe the plasmon dynamics in these quantum systems by measuring the excited-state lifetime of three negatively charged PAH molecules: anthanthrene, benzo[ghi]perylene, and perylene. In contrast to the molecules in their neutral state, these three systems exhibit far more rapid decay dynamics due to the deexcitation of multiple electron–hole pairs through molecular plasmon “dephasing” and vibrational relaxation. This study provides a look into the distinction between collective and single-electron excitation dynamics in the purely quantum limit and introduces a conceptual framework with which to visualize molecular plasmon decay.

  • plasmonics
  • excited-state dynamics
  • molecular plasmons
  • plasmonicity
  • lifetime

Footnotes

  • ↵1To whom correspondence should be addressed. Email: halas{at}rice.edu.
  • Author contributions: P.N. and N. J. Halas designed research; K.D.C., L.B., G.J.S., A.L., N. J. Hogan, and Y.C. performed research; K.D.C., L.B., and N. J. Hogan analyzed data; and K.D.C., L.B., P.N., and N. J. Halas wrote the paper.

  • Reviewers: C.M.A., Kansas State University; and D.N.B., Columbia University.

  • The authors declare no conflict of interest.

  • This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1805357115/-/DCSupplemental.

Published under the PNAS license.

View Full Text

Log in using your username and password

Forgot your user name or password?

Purchase access

You may purchase access to this article. This will require you to create an account if you don't already have one.

Subscribers, for more details, please visit our Subscriptions FAQ.

Please click here to log into the PNAS submission website.

PreviousNext
Back to top
Article Alerts
Email Article

Thank you for your interest in spreading the word on PNAS.

NOTE: We only request your email address so that the person you are recommending the page to knows that you wanted them to see it, and that it is not junk mail. We do not capture any email address.

Enter multiple addresses on separate lines or separate them with commas.
Lifetime dynamics of plasmons in the few-atom limit
(Your Name) has sent you a message from PNAS
(Your Name) thought you would like to see the PNAS web site.
Citation Tools
Lifetime dynamics of plasmons in the few-atom limit
Kyle D. Chapkin, Luca Bursi, Grant J. Stec, Adam Lauchner, Nathaniel J. Hogan, Yao Cui, Peter Nordlander, Naomi J. Halas
Proceedings of the National Academy of Sciences Sep 2018, 115 (37) 9134-9139; DOI: 10.1073/pnas.1805357115

Citation Manager Formats

  • BibTeX
  • Bookends
  • EasyBib
  • EndNote (tagged)
  • EndNote 8 (xml)
  • Medlars
  • Mendeley
  • Papers
  • RefWorks Tagged
  • Ref Manager
  • RIS
  • Zotero
Request Permissions
Share
Lifetime dynamics of plasmons in the few-atom limit
Kyle D. Chapkin, Luca Bursi, Grant J. Stec, Adam Lauchner, Nathaniel J. Hogan, Yao Cui, Peter Nordlander, Naomi J. Halas
Proceedings of the National Academy of Sciences Sep 2018, 115 (37) 9134-9139; DOI: 10.1073/pnas.1805357115
del.icio.us logo Digg logo Reddit logo Twitter logo CiteULike logo Facebook logo Google logo Mendeley logo
  • Tweet Widget
  • Facebook Like
  • Mendeley logo Mendeley
Proceedings of the National Academy of Sciences: 116 (7)
Current Issue

Submit

Sign up for Article Alerts

Jump to section

  • Article
    • Abstract
    • Materials and Methods
    • Acknowledgments
    • Footnotes
    • References
  • Figures & SI
  • Info & Metrics
  • PDF

You May Also be Interested in

Several aspects of the proposal, which aims to expand open access, require serious discussion and, in some cases, a rethink.
Opinion: “Plan S” falls short for society publishers—and for the researchers they serve
Several aspects of the proposal, which aims to expand open access, require serious discussion and, in some cases, a rethink.
Image credit: Dave Cutler (artist).
Several large or long-lived animals seem strangely resistant to developing cancer. Elucidating the reasons why could lead to promising cancer-fighting strategies in humans.
Core Concept: Solving Peto’s Paradox to better understand cancer
Several large or long-lived animals seem strangely resistant to developing cancer. Elucidating the reasons why could lead to promising cancer-fighting strategies in humans.
Image credit: Shutterstock.com/ronnybas frimages.
Featured Profile
PNAS Profile of NAS member and biochemist Hao Wu
 Nonmonogamous strawberry poison frog (Oophaga pumilio).  Image courtesy of Yusan Yang (University of Pittsburgh, Pittsburgh).
Putative signature of monogamy
A study suggests a putative gene-expression hallmark common to monogamous male vertebrates of some species, namely cichlid fishes, dendrobatid frogs, passeroid songbirds, common voles, and deer mice, and identifies 24 candidate genes potentially associated with monogamy.
Image courtesy of Yusan Yang (University of Pittsburgh, Pittsburgh).
Active lifestyles. Image courtesy of Pixabay/MabelAmber.
Meaningful life tied to healthy aging
Physical and social well-being in old age are linked to self-assessments of life worth, and a spectrum of behavioral, economic, health, and social variables may influence whether aging individuals believe they are leading meaningful lives.
Image courtesy of Pixabay/MabelAmber.

More Articles of This Classification

Physical Sciences

  • Deep elastic strain engineering of bandgap through machine learning
  • Single-molecule excitation–emission spectroscopy
  • Microscopic description of acid–base equilibrium
Show more

Physics

  • Unraveling materials Berry curvature and Chern numbers from real-time evolution of Bloch states
  • Opinion: “Plan S” falls short for society publishers—and for the researchers they serve
  • Limits of multifunctionality in tunable networks
Show more

Related Content

  • No related articles found.
  • Scopus
  • PubMed
  • Google Scholar

Cited by...

  • No citing articles found.
  • Google Scholar

Similar Articles

Site Logo
Powered by HighWire
  • Submit Manuscript
  • Twitter
  • Facebook
  • RSS Feeds
  • Email Alerts

Articles

  • Current Issue
  • Latest Articles
  • Archive

PNAS Portals

  • Classics
  • Front Matter
  • Teaching Resources
  • Anthropology
  • Chemistry
  • Physics
  • Sustainability Science

Information

  • Authors
  • Editorial Board
  • Reviewers
  • Press
  • Site Map

Feedback    Privacy/Legal

Copyright © 2019 National Academy of Sciences. Online ISSN 1091-6490