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Efficient Emission Enhancement of Single CdSe/CdS/PMMA Quantum Dots through Controlled Near-Field Coupling to Plasmonic Bullseye Resonators

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https://doi.org/10.1021/acs.nanolett.8b01533
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Nano Letters. 2018, 18(9), pp. 5396-5400. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.8b01533

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A strong increase of spontaneous radiative emission from colloidally synthesized CdSe/CdS/PMMA hybrid particles is achieved when manipulated into plasmonic bullseye resonators with the tip of an atomic force microscope (AFM). This type of antenna provides a broadband resonance, which may be precisely matched to the exciton ground state energy in the inorganic cores. Statistically analyzing the spectral photoluminescence (PL) of a large number of individual coupled and uncoupled CdSe/CdS/PMMA quantum dots, we find an order of magnitude of intensity enhancement due to the Purcell effect. Time-resolved PL shows a commensurate increase of the spontaneous emission rate with radiative lifetimes below 230 ps for the bright exciton transition. The combination of AFM and PL imaging allows for sub-200 nm localization of the particle position inside the plasmonic antenna. This capability unveils a different coupling behavior of dark excitonic states: even stronger PL enhancement occurs at positions with maximum spatial gradient of the nearfield, effectively adding a dipolar component to original quadrupole transitions. The broadband maximization of light-matter interaction provided by our nanoengineered compound systems enables an attractive class of future experiments in ultrafast quantum optics.

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530 Physik

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Colloidal quantum dots; light-matter coupling; near-field enhancement; Purcell factor; time-domain quantum physics

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ISO 690WERSCHLER, Florian, Benjamin LINDNER, Christopher HINZ, Frieder CONRADT, Pascal GUMBSHEIMER, Carla NEGELE, Tjaard DE ROO, Stefan MECKING, Alfred LEITENSTORFER, Denis V. SELETSKIY, 2018. Efficient Emission Enhancement of Single CdSe/CdS/PMMA Quantum Dots through Controlled Near-Field Coupling to Plasmonic Bullseye Resonators. In: Nano Letters. 2018, 18(9), pp. 5396-5400. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.8b01533
BibTex
@article{Werschler2018-08-09Effic-44569,
  year={2018},
  doi={10.1021/acs.nanolett.8b01533},
  title={Efficient Emission Enhancement of Single CdSe/CdS/PMMA Quantum Dots through Controlled Near-Field Coupling to Plasmonic Bullseye Resonators},
  number={9},
  volume={18},
  issn={1530-6984},
  journal={Nano Letters},
  pages={5396--5400},
  author={Werschler, Florian and Lindner, Benjamin and Hinz, Christopher and Conradt, Frieder and Gumbsheimer, Pascal and Negele, Carla and de Roo, Tjaard and Mecking, Stefan and Leitenstorfer, Alfred and Seletskiy, Denis V.}
}
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