Coupling single quantum dots to plasmonic nanocones: optical properties (original) (raw)
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Nanoscale, 2015
Hybrid structures of few or single quantum dots (QDs) coupled to single optical antennas are of prime interest for nano-optical research. The photoluminescence (PL) signal from single nanoemitters, such as QDs, can be enhanced, and their emission characteristics modified, by coupling them to plasmonic nanostructures. Here, a self-aligned technique for placing nanoscale QDs with about 10 nm lateral accuracy and well-defined molecular distances to the tips of individual nanocones is reported. This way the QDs are positioned exactly in the high near-field region that can be created near the cone apex. The cones are excited in the focus of a radially polarized laser beam and the PL signal of few or single QDs on the cone tips is spectrally detected.
Nano Letters, 2010
We demonstrate how the controlled positioning of a plasmonic nanoparticle modifies the photoluminescence of a single epitaxial GaAs quantum dot. The antenna particle leads to an increase of the luminescence intensity by about a factor of eight. Spectrally and temporally resolved photoluminescence measurements prove an increase of the quantum dot's excitation rate. The combination of stable epitaxial quantum emitters and plasmonic nanostructures promises to be highly beneficial for nanoscience and quantum optics.
Scientific reports, 2017
Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other nonradiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60 and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.
Journal of the American Chemical Society, 2016
New approaches in molecular nanoscopy are greatly desired for interrogation of biological, organic, and inorganic objects with sizes below the diffraction limit. Our current work investigates emergent monolayer protected gold quantum dots (nanoclusters) composed of 25gold by utilizing two-photon excited fluorescence (TPEF) near-field scanning optical microscopy (NSOM) at single nanocluster concentrations. Here, we demonstrate an approach to synthesize and to obtain isolated single nanoclusters on solid glass substrates. Their subsequent investigation using TPEF NSOM reveals that even when they are separated by several tens-of-nanometer distances we can excite and interrogate single nanoclusters individually. Interestingly, we observe an enhanced two-photon absorption cross section for single Au 25 NCs that can be attributed to few-atom local field effects and to local-field induced microscopic cascading (LFIMC), indicating their potential to be used in ultrasensitive sensing, disease diagnostics, cancer cell therapy, and molecular computers. Finally, we report room temperature aperture-based TPEF NSOM imaging of these nanoclusters (NCs) for the first time at 30 nm point resolution which is a ~5-fold improvement compared to the previous best result for the same technique. This report unveils the employment of the unique combination of unusually large two-photon absorption cross section and high photo stability of the gold-nanoclusters to (non-destructively) investigate stable isolated
Manipulating Coupling between a Single Semiconductor Quantum Dot and Single Gold Nanoparticle
Nano Letters, 2011
Using atomic force microscopy nanomanipulation, we position a single Au nanoparticle near a CdSe/ZnS quantum dot to construct a hybrid nanostructure with variable geometry. The coupling between the two particles is varied in a systematic and reversible manner. The photoluminescence lifetime and blinking of the same quantum dot are measured before and after assembly of the structure. In some hybrid structures, the total lifetime is reduced from about 30 ns to well below 1 ns. This dramatic change in lifetime is accompanied by the disappearance of blinking as the nonradiative energy transfer from the CdSe/ZnS quantum dot to the Au nanoparticle becomes the dominant decay channel. Both total lifetime and photoluminescence intensity changes are well described by simple analytical calculations.
Temperature dependence of quantum dot fluorescence assisted by plasmonic nanoantennas
Physical Review B, 2015
Optical antennas based on noble metal nanoparticles can increase the photoluminescence of quantum dots, but the exact strength of this enhancement depends on the brightness (i.e., the intrinsic quantum yield η i) of the emitters. Here we perform temperature-dependent measurements on a system of PbS colloidal quantum dots coupled with Au ring arrays that bring quantitative insight into this phenomenon. We show that although the boost in photoluminescence is lower at cryogenic temperatures where the nanocrystals become very bright emitters, the spectral signature of this enhancement is remarkably independent of η i. These observations remain true even at wavelengths where the losses by absorption in the metal nanoparticles considerably increase due to the excitation of localized plasmon resonances, in contradiction with standard theory that treats the emitters as a collection of two-level systems. We propose a mechanism in which the quantum dots are modeled as multilevel and inhomogeneously broadened emitters to account for these findings.
Resonant Plasmonic Enhancement of Single-Molecule Fluorescence by Individual Gold Nanorods
ACS Nano, 2014
Enhancing the fluorescence of a weak emitter is important to further extend the reach of single-molecule fluorescence imaging to many unexplored systems. Here we study fluorescence enhancement by isolated gold nanorods and explore the role of the surface plasmon resonance (SPR) on the observed enhancements. Gold nanorods can be cheaply synthesized in large volumes yet we find similar fluorescence enhancements as literature reports on lithographically fabricated nanoparticle assemblies. The fluorescence of a weak emitter, crystal violet, can be enhanced more than 1000-fold by a single nanorod with its SPR at 629 nm excited at 633 nm. This strong enhancement results from both an excitation rate enhancement of ~130 and an effective emission enhancement of ~9. The fluorescence enhancement, however, decreases sharply when the SPR wavelength moves away from the excitation laser wavelength or when the SPR has only a partial overlap with the emission spectrum of the fluorophore. The reported measurements of fluorescence enhancement by 11 nanorods with varying SPR wavelengths are consistent with numerical simulations.
Enhanced localized fluorescence in plasmonic nanoantennae
Applied Physics Letters, 2008
Pairs of gold elliptical nanoparticles form antennae, resonant in the visible. A dye, embedded in a dielectric host, coats the antennae; its emission excites plasmon resonances in the antennae and is enhanced. Far-field excitation of the dye-nanoantenna system shows a wavelength-dependent increase in fluorescence that reaches 100 times enhancement. Near-field excitation shows enhanced fluorescence from a single nanoantenna localized in a subwavelength area of ∼0.15μm2. The polarization of enhanced emission is along the main antenna axis. These observed experimental results are important for increasing light extraction from emitters localized around antennae and for potential development of a subwavelength sized laser.
Nature Communications, 2020
Hybrid plasmonic nano-emitters based on the combination of quantum dot emitters (QD) and plasmonic nanoantennas open up new perspectives in the control of light. However, precise positioning of any active medium at the nanoscale constitutes a challenge. Here, we report on the optimal overlap of antenna’s near-field and active medium whose spatial distribution is controlled via a plasmon-triggered 2-photon polymerization of a photosensitive formulation containing QDs. Au nanoparticles of various geometries are considered. The response of these hybrid nano-emitters is shown to be highly sensitive to the light polarization. Different light emission states are evidenced by photoluminescence measurements. These states correspond to polarization-sensitive nanoscale overlap between the exciting local field and the active medium distribution. The decrease of the QD concentration within the monomer formulation allows trapping of a single quantum dot in the vicinity of the Au particle. The la...