Journal
NANO LETTERS
Volume 18, Issue 9, Pages 5396-5400Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b01533
Keywords
Colloidal quantum dots; near-field enhancement; light-matter coupling; Purcell factor; time-domain quantum physics
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [SFB767]
- DFG [283908774]
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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 D 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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