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Title: Photoluminescence Enhancement of CuInS 2 Quantum Dots in Solution Coupled to Plasmonic Gold Nanocup Array

Abstract

A strong plasmonic enhancement of photoluminescence (PL) decay rate in quantum dots (QDs) coupled to an array of gold-coated nanocups is demonstrated. CuInS2 QDs that emit at a wavelength that overlaps with the extraordinary optical transmission (EOT) of the gold nanocup array are placed in the cups as solutions. Time-resolved PL reveals that the decay rate of the QDs in the plasmonically coupled system can be enhanced by more than an order of magnitude. Using finite-difference time-domain (FDTD) simulations, it is shown that this enhancement in PL decay rate results from an enhancement factor of ≈100 in electric field intensity provided by the plasmonic mode of the nanocup array, which is also responsible for the EOT. The simulated Purcell factor approaches 86 at the bottom of the nanocup and is ≈3–15 averaged over the nanocup cavity height, agreeing with the experimental enhancement result. In conclusion, this demonstration of solution-based coupling between QDs and gold nanocups opens up new possibilities for applications that would benefit from a solution environment such as biosensing.

Authors:
 [1]; ORCiD logo [2];  [2];  [2];  [1];  [2]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1396273
Report Number(s):
IS-J-9443; LA-UR-17-25520
Journal ID: ISSN 1613-6810
Grant/Contract Number:
AC52-06NA25396; NA-0003525; AC02-07CH11358; NA0003525
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 13; Journal Issue: 33; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; nanophotonics; plasmonics; Purcell enhancement; optical transmission; quantum dots; Inorganic and Physical Chemistry; Material Science; plasmonic structure, quantum dots, optical spectroscopy, photoluminescence

Citation Formats

Peer, Akshit, Hu, Zhongjian, Singh, Ajay, Hollingsworth, Jennifer A., Biswas, Rana, and Htoon, Han. Photoluminescence Enhancement of CuInS2 Quantum Dots in Solution Coupled to Plasmonic Gold Nanocup Array. United States: N. p., 2017. Web. doi:10.1002/smll.201700660.
Peer, Akshit, Hu, Zhongjian, Singh, Ajay, Hollingsworth, Jennifer A., Biswas, Rana, & Htoon, Han. Photoluminescence Enhancement of CuInS2 Quantum Dots in Solution Coupled to Plasmonic Gold Nanocup Array. United States. doi:10.1002/smll.201700660.
Peer, Akshit, Hu, Zhongjian, Singh, Ajay, Hollingsworth, Jennifer A., Biswas, Rana, and Htoon, Han. 2017. "Photoluminescence Enhancement of CuInS2 Quantum Dots in Solution Coupled to Plasmonic Gold Nanocup Array". United States. doi:10.1002/smll.201700660.
@article{osti_1396273,
title = {Photoluminescence Enhancement of CuInS2 Quantum Dots in Solution Coupled to Plasmonic Gold Nanocup Array},
author = {Peer, Akshit and Hu, Zhongjian and Singh, Ajay and Hollingsworth, Jennifer A. and Biswas, Rana and Htoon, Han},
abstractNote = {A strong plasmonic enhancement of photoluminescence (PL) decay rate in quantum dots (QDs) coupled to an array of gold-coated nanocups is demonstrated. CuInS2 QDs that emit at a wavelength that overlaps with the extraordinary optical transmission (EOT) of the gold nanocup array are placed in the cups as solutions. Time-resolved PL reveals that the decay rate of the QDs in the plasmonically coupled system can be enhanced by more than an order of magnitude. Using finite-difference time-domain (FDTD) simulations, it is shown that this enhancement in PL decay rate results from an enhancement factor of ≈100 in electric field intensity provided by the plasmonic mode of the nanocup array, which is also responsible for the EOT. The simulated Purcell factor approaches 86 at the bottom of the nanocup and is ≈3–15 averaged over the nanocup cavity height, agreeing with the experimental enhancement result. In conclusion, this demonstration of solution-based coupling between QDs and gold nanocups opens up new possibilities for applications that would benefit from a solution environment such as biosensing.},
doi = {10.1002/smll.201700660},
journal = {Small},
number = 33,
volume = 13,
place = {United States},
year = 2017,
month = 7
}

Journal Article:
Free Publicly Available Full Text
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  • The approach of optical positioning the single InAs quantum dots (QDs) was used for investigating QD photoluminescence (PL) enhancement based on plasmonic effect of nanometer-sized Au island films. It is found that the maximum increase of QD PL intensity is about thirty-eight fold after 5-nm thick Au island films are evaporated on the QD sample surface. The enhanced localized excitation field and increased QD radiative decay rate are responsible for this PL enhancement. This provides an alternative way of preparing bright single photon sources based on the plasmonic effect.
  • Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less
  • Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less