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Title: Molecular Emission near Metal Interfaces: The Polaritonic Regime

Abstract

The strong coupling of a dense layer of molecular excitons with surface-plasmon modes in a metal gives rise to polaritons (hybrid light–matter states) called plexcitons. Surface plasmons cannot directly emit into (or be excited by) free-space photons due to the fact that energy and momentum conservation cannot be simultaneously satisfied in photoluminescence. Most plexcitons are also formally nonemissive, even though they can radiate via molecules upon localization due to disorder and decoherence. However, a fraction of them are bright even in the presence of such deleterious processes. Here in this Letter, we theoretically discuss the superradiant emission properties of these bright plexcitons, which belong to the upper energy branch and reveal huge photoluminescence enhancements compared to bare excitons, due to near-divergences in the density of photonic modes available to them. Our study generalizes the well-known problem of molecular emission next to a metal interface to the polaritonic regime.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Univ. of California, San Diego, CA (United States)
  2. Harvard Univ., Cambridge, MA (United States); Kazan Federal Univ., Kazan (Russia). Inst. of Physics
  3. City Univ. of New York (CUNY), NY (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); City Univ. of New York (CUNY), NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566535
Grant/Contract Number:  
[SC0001088; SC0017760]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
[ Journal Volume: 9; Journal Issue: 22]; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Yuen-Zhou, Joel, Saikin, Semion K., and Menon, Vinod M. Molecular Emission near Metal Interfaces: The Polaritonic Regime. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b02980.
Yuen-Zhou, Joel, Saikin, Semion K., & Menon, Vinod M. Molecular Emission near Metal Interfaces: The Polaritonic Regime. United States. doi:10.1021/acs.jpclett.8b02980.
Yuen-Zhou, Joel, Saikin, Semion K., and Menon, Vinod M. Mon . "Molecular Emission near Metal Interfaces: The Polaritonic Regime". United States. doi:10.1021/acs.jpclett.8b02980. https://www.osti.gov/servlets/purl/1566535.
@article{osti_1566535,
title = {Molecular Emission near Metal Interfaces: The Polaritonic Regime},
author = {Yuen-Zhou, Joel and Saikin, Semion K. and Menon, Vinod M.},
abstractNote = {The strong coupling of a dense layer of molecular excitons with surface-plasmon modes in a metal gives rise to polaritons (hybrid light–matter states) called plexcitons. Surface plasmons cannot directly emit into (or be excited by) free-space photons due to the fact that energy and momentum conservation cannot be simultaneously satisfied in photoluminescence. Most plexcitons are also formally nonemissive, even though they can radiate via molecules upon localization due to disorder and decoherence. However, a fraction of them are bright even in the presence of such deleterious processes. Here in this Letter, we theoretically discuss the superradiant emission properties of these bright plexcitons, which belong to the upper energy branch and reveal huge photoluminescence enhancements compared to bare excitons, due to near-divergences in the density of photonic modes available to them. Our study generalizes the well-known problem of molecular emission next to a metal interface to the polaritonic regime.},
doi = {10.1021/acs.jpclett.8b02980},
journal = {Journal of Physical Chemistry Letters},
number = [22],
volume = [9],
place = {United States},
year = {2018},
month = {10}
}

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Cited by: 8 works
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Works referencing / citing this record:

Light-emitting metasurfaces
journal, July 2019

  • Vaskin, Aleksandr; Kolkowski, Radoslaw; Koenderink, A. Femius
  • Nanophotonics, Vol. 8, Issue 7
  • DOI: 10.1515/nanoph-2019-0110