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Title: Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities

Abstract

Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (F P) up to F P = 180 (average F P = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore, the measured ultra-narrow exciton linewidth (18 ueV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. Furthermore, to demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [3];  [3]; ORCiD logo [2]; ORCiD logo [1]
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  1. Stevens Institute of Technology, Hoboken, NJ (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1409304
Report Number(s):
NREL/JA-5900-68251
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; carbon nanotube; quantum yield; plasmonic; quantum computing

Citation Formats

Luo, Yue, Ahmadi, Ehsaneh D., Shayan, Kamran, Ma, Yichen, Mistry, Kevin S., Zhang, Changjian, Hone, James, Blackburn, Jeffrey L., and Strauf, Stefan. Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities. United States: N. p., 2017. Web. doi:10.1038/s41467-017-01777-w.
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Luo, Yue, Ahmadi, Ehsaneh D., Shayan, Kamran, Ma, Yichen, Mistry, Kevin S., Zhang, Changjian, Hone, James, Blackburn, Jeffrey L., & Strauf, Stefan. Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities. United States. doi:10.1038/s41467-017-01777-w.
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Luo, Yue, Ahmadi, Ehsaneh D., Shayan, Kamran, Ma, Yichen, Mistry, Kevin S., Zhang, Changjian, Hone, James, Blackburn, Jeffrey L., and Strauf, Stefan. Fri . "Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities". United States. doi:10.1038/s41467-017-01777-w. https://www.osti.gov/servlets/purl/1409304.
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@article{osti_1409304,
title = {Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities},
author = {Luo, Yue and Ahmadi, Ehsaneh D. and Shayan, Kamran and Ma, Yichen and Mistry, Kevin S. and Zhang, Changjian and Hone, James and Blackburn, Jeffrey L. and Strauf, Stefan},
abstractNote = {Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (FP) up to FP = 180 (average FP = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore, the measured ultra-narrow exciton linewidth (18 ueV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. Furthermore, to demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.},
doi = {10.1038/s41467-017-01777-w},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {11}
}
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Journal Article:
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DOI:  10.1038/s41467-017-01777-w
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Works referenced in this record:

Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna
journal, October 2009

  • Kinkhabwala, Anika; Yu, Zongfu; Fan, Shanhui
  • Nature Photonics, Vol. 3, Issue 11, p. 654-657
  • DOI: 10.1038/nphoton.2009.187
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