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Title: Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Abstract

Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  2. Purdue Univ., West Lafayette, IN (United States). Dept. of Chemistry
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1418662
Grant/Contract Number:
SC0016356
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; Localized surface plasmons; metal nanoparticle arrays; plasmon lasing; transient absorption microscopy; lattice plasmons

Citation Formats

Deeb, Claire, Guo, Zhi, Yang, Ankun, Huang, Libai, and Odom, Teri W. Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.7b05223.
Deeb, Claire, Guo, Zhi, Yang, Ankun, Huang, Libai, & Odom, Teri W. Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays. United States. doi:10.1021/acs.nanolett.7b05223.
Deeb, Claire, Guo, Zhi, Yang, Ankun, Huang, Libai, and Odom, Teri W. Thu . "Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays". United States. doi:10.1021/acs.nanolett.7b05223.
@article{osti_1418662,
title = {Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays},
author = {Deeb, Claire and Guo, Zhi and Yang, Ankun and Huang, Libai and Odom, Teri W.},
abstractNote = {Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.},
doi = {10.1021/acs.nanolett.7b05223},
journal = {Nano Letters},
number = 2,
volume = 18,
place = {United States},
year = {Thu Jan 25 00:00:00 EST 2018},
month = {Thu Jan 25 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on January 25, 2019
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