Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons

Chang Hee Cho; Carlos O. Aspetti; Michael E. Turk; James M. Kikkawa; Sung Wook Nam; Ritesh Agarwal

doi:10.1038/nmat3067

Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons

Chang Hee Cho
, Carlos O. Aspetti
, Michael E. Turk
, James M. Kikkawa
, Sung Wook Nam
, Ritesh Agarwal

Department of Physics and Chemistry

University of Pennsylvania

Research output: Contribution to journal › Article › peer-review

142 Scopus citations

Abstract

The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10-50, producing emission mostly from thermalizedexcitons. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS-SiO 2-Ag core-shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >10 3 and sub-picosecond lifetimes. Core-shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon-exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.

Original language	English
Pages (from-to)	669-675
Number of pages	7
Journal	Nature Materials
Volume	10
Issue number	9
DOIs	https://doi.org/10.1038/nmat3067
State	Published - Sep 2011

Bibliographical note

Funding Information:
We thank N. Engheta for discussions and A. Exarhos for helping to build the optical Kerr gate system. Time-resolved photoluminescence work was supported by the Department of Energy BES under Award No. DESC0002158. The remaining work was supported by the US Army Research Office under Grant No. W911NF-09-1-0477, National Institutes of Health through the NIH Director’s New Innovator Award Program, 1-DP2-7251-01, and the Nano/Bio Interface Center through NSF-NSEC-DMR08-32802. C.O.A. is supported by the NBIC through the NSF IGERT DGE02-21664.

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title = "Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons",

abstract = "The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10-50, producing emission mostly from thermalizedexcitons. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS-SiO 2-Ag core-shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >10 3 and sub-picosecond lifetimes. Core-shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon-exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.",

author = "Cho, \{Chang Hee\} and Aspetti, \{Carlos O.\} and Turk, \{Michael E.\} and Kikkawa, \{James M.\} and Nam, \{Sung Wook\} and Ritesh Agarwal",

note = "Funding Information: We thank N. Engheta for discussions and A. Exarhos for helping to build the optical Kerr gate system. Time-resolved photoluminescence work was supported by the Department of Energy BES under Award No. DESC0002158. The remaining work was supported by the US Army Research Office under Grant No. W911NF-09-1-0477, National Institutes of Health through the NIH Director{\textquoteright}s New Innovator Award Program, 1-DP2-7251-01, and the Nano/Bio Interface Center through NSF-NSEC-DMR08-32802. C.O.A. is supported by the NBIC through the NSF IGERT DGE02-21664.",

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AU - Kikkawa, James M.

AU - Nam, Sung Wook

AU - Agarwal, Ritesh

N1 - Funding Information: We thank N. Engheta for discussions and A. Exarhos for helping to build the optical Kerr gate system. Time-resolved photoluminescence work was supported by the Department of Energy BES under Award No. DESC0002158. The remaining work was supported by the US Army Research Office under Grant No. W911NF-09-1-0477, National Institutes of Health through the NIH Director’s New Innovator Award Program, 1-DP2-7251-01, and the Nano/Bio Interface Center through NSF-NSEC-DMR08-32802. C.O.A. is supported by the NBIC through the NSF IGERT DGE02-21664.

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N2 - The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10-50, producing emission mostly from thermalizedexcitons. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS-SiO 2-Ag core-shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >10 3 and sub-picosecond lifetimes. Core-shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon-exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.

AB - The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10-50, producing emission mostly from thermalizedexcitons. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS-SiO 2-Ag core-shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >10 3 and sub-picosecond lifetimes. Core-shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon-exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.

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Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons

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