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Nonlinear plasmon-exciton coupling enhances sum-frequency generation from a hybrid metal/semiconductor nanostructure

Zhong, Jin Hui ; Vogelsang, Jan LU ; Yi, Jue Min ; Wang, Dong ; Wittenbecher, Lukas LU ; Mikaelsson, Sara LU ; Korte, Anke ; Chimeh, Abbas ; Arnold, Cord L. LU and Schaaf, Peter , et al. (2020) In Nature Communications 11(1).
Abstract

The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The ultrafast optical dynamics of such hybrid plasmon–emitter systems have rarely been explored. Here, we study those dynamics by interferometrically probing nonlinear optical emission from individual porous gold nanosponges infiltrated with zinc oxide (ZnO) emitters. Few-femtosecond time-resolved photoelectron emission microscopy reveals multiple long-lived localized plasmonic hot spot modes, at the surface of the randomly disordered nanosponges, that are resonant in a... (More)

The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The ultrafast optical dynamics of such hybrid plasmon–emitter systems have rarely been explored. Here, we study those dynamics by interferometrically probing nonlinear optical emission from individual porous gold nanosponges infiltrated with zinc oxide (ZnO) emitters. Few-femtosecond time-resolved photoelectron emission microscopy reveals multiple long-lived localized plasmonic hot spot modes, at the surface of the randomly disordered nanosponges, that are resonant in a broad spectral range. The locally enhanced plasmonic near-field couples to the ZnO excitons, enhancing sum-frequency generation from individual hot spots and boosting resonant excitonic emission. The quantum pathways of the coupling are uncovered from a two-dimensional spectrum correlating fundamental plasmonic excitations to nonlinearly driven excitonic emissions. Our results offer new opportunities for enhancing and coherently controlling optical nonlinearities by exploiting nonlinear plasmon-quantum emitter coupling.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
11
issue
1
article number
1464
publisher
Nature Publishing Group
external identifiers
  • pmid:32193407
  • scopus:85082066134
ISSN
2041-1723
DOI
10.1038/s41467-020-15232-w
language
English
LU publication?
yes
id
257a7e44-bdcd-4c1c-8913-b575b3c4ed1c
date added to LUP
2020-04-02 12:42:46
date last changed
2024-03-20 06:44:36
@article{257a7e44-bdcd-4c1c-8913-b575b3c4ed1c,
  abstract     = {{<p>The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The ultrafast optical dynamics of such hybrid plasmon–emitter systems have rarely been explored. Here, we study those dynamics by interferometrically probing nonlinear optical emission from individual porous gold nanosponges infiltrated with zinc oxide (ZnO) emitters. Few-femtosecond time-resolved photoelectron emission microscopy reveals multiple long-lived localized plasmonic hot spot modes, at the surface of the randomly disordered nanosponges, that are resonant in a broad spectral range. The locally enhanced plasmonic near-field couples to the ZnO excitons, enhancing sum-frequency generation from individual hot spots and boosting resonant excitonic emission. The quantum pathways of the coupling are uncovered from a two-dimensional spectrum correlating fundamental plasmonic excitations to nonlinearly driven excitonic emissions. Our results offer new opportunities for enhancing and coherently controlling optical nonlinearities by exploiting nonlinear plasmon-quantum emitter coupling.</p>}},
  author       = {{Zhong, Jin Hui and Vogelsang, Jan and Yi, Jue Min and Wang, Dong and Wittenbecher, Lukas and Mikaelsson, Sara and Korte, Anke and Chimeh, Abbas and Arnold, Cord L. and Schaaf, Peter and Runge, Erich and Huillier, Anne L’ and Mikkelsen, Anders and Lienau, Christoph}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Nonlinear plasmon-exciton coupling enhances sum-frequency generation from a hybrid metal/semiconductor nanostructure}},
  url          = {{http://dx.doi.org/10.1038/s41467-020-15232-w}},
  doi          = {{10.1038/s41467-020-15232-w}},
  volume       = {{11}},
  year         = {{2020}},
}