Quantum dot microdrop laser

We report single-mode and multimode lasing from isolated spherical liquid microcavities containing CdSe/ZnS nanocrystal quantum dots. Lasing is observed at densities more than 2 orders of magnitude lower than previously demonstrated or theoretically predicted, assuming a uniform nanocrystal quantum dot distribution. Charged droplets, between 10 and 40 microm in size, are electrodynamically levitated and optically pumped. Substantial laser signals at low thresholds are measured from the directional emission normal to the pump beam, owing to the high Q cavity modes.     

Excitation isotropy of single CdSe/ZnS nanocrystals

We study the dimensionality of the excitation transition dipole moment for single CdSe/ZnS core-shell nanocrystals using azimuthally and radially polarized laser modes. The comparison of measured and simulated single nanocrystal excitation patterns shows that single CdSe/ZnS quantum dots possess a spherically degenerated excitation transition dipole. We show that the dimensionality of the excitation transition dipole moment distribution is the same for all individual CdSe/ZnS nanocrystals, disregarding the difference in core size and irrespective of variations in the local environment. In contrast to the emission transition dipole moment, which is oriented in one plane, the excitation transition dipole moment of a single CdSe/ZnS quantum dots possesses an isotropy in three dimensions.     

Monolithic ZnTe-based pillar microcavities containing CdTe quantum dots

Micropillars of different diameters have been prepared by focused ion beam milling out of a planar ZnTe-based cavity. The monolithic epitaxial structure, deposited on a GaAs substrate, contains CdTe quantum dots embedded in a ZnTe λ-cavity delimited by two distributed Bragg reflectors (DBRs). The high refractive index material of the DBR structure is ZnTe, while for the low index material a short-period triple MgTe/ZnTe/MgSe superlattice is used. The CdTe quantum dots are formed by a novel Zn-induced formation process and are investigated by scanning transmission electron microscopy. Micro-photoluminescence measurements show discrete optical modes for the pillars, in good agreement with calculations based on a vectorial transfer matrix method. The measured quality factor reaches a value of 3100.     

Applications of quantum dots in optical fiber luminescent oxygen sensors

The potential applications of luminescent semiconductor nanocrystals to optical oxygen sensing are explored. The suitability of quantum dots to provide a reference signal in luminescence-based chemical sensors is addressed. A CdSe-ZnS nanocrystal, with an emission peak at 520 nm, is used to provide a reference signal. Measurements of oxygen concentration, which are based on the dynamic quenching of the luminescence of a ruthenium complex, are performed. Both the dye and the nanocrystal are immobilized in a solgel matrix and are excited by a blue LED. Experimental results show that the ratio between the reference and the sensor signals is highly insensitive to fluctuations of the excitation optical power. The use of CdTe, near-infrared quantum dots with an emission wavelength of 680 nm, in combination with a ruthenium complex to provide a new mechanism for oxygen sensing, is investigated. The possibility of creating oxygen sensitivity in different spectral regions is demonstrated. The results obtained clearly show that this technique can be applied to develop a wavelength division multiplexed system of oxygen sensors.     

Photoluminescence waveguiding in CdSe and CdTe QDs-PMMA nanocomposite films

In this paper, active planar waveguides based on the incorporation of CdSe and CdTe nanocrystal quantum dots in a polymer matrix are demonstrated. In the case of doping the polymer with both types of quantum dots, the nanocomposite film guides both emitted colors, green (550?nm, CdTe) and orange (600?nm, CdSe). The optical pumping laser can be coupled not only with a standard end-fire coupling system, but also directing the beam to the surface of the sample, indicating a good absorption cross-section and waveguide properties. To achieve these results, a study of the nanocomposite optical properties as a function of the nanocrystal concentration is presented and the optimum conditions are found for waveguiding.     

Observation of Rabi splitting from surface plasmon coupled conduction state transitions in electrically excited InAs quantum dots

We demonstrate strong coupling between a surface plasmon and intersublevel transitions in self-assembled InAs quantum dots. The surface plasmon mode exists at the interface between the semiconductor emitter structure and a periodic array of holes perforating a metallic Pd/Ge/Au film that also serves as the top electrical contact for the emitters. Spectrally narrowed quantum-dot electroluminescence was observed for devices with varying subwavelength hole spacing. Devices designed for 9, 10, and 11 μm wavelength emission also exhibit a significant spectral splitting. The association of the splitting with quantum-dot Rabi oscillation is consistent with results from a calculation of spontaneous emission from an interacting plasmonic field and quantum-dot ensemble. The fact that this Rabi oscillation can be observed in an incoherently excited, highly inhomogeneously broadened system demonstrates the utility of intersublevel transitions in quantum dots for investigations of coherent transient and quantum coherence phenomena.     

Enhanced fluorescence emission from quantum dots on a photonic crystal surface

Colloidal quantum dots display a wide range of novel optical properties that could prove useful for many applications in photonics. Here, we report the enhancement of fluorescence emission from colloidal quantum dots on the surface of two-dimensional photonic crystal slabs. The enhancement is due to a combination of high-intensity near fields and strong coherent scattering effects, which we attribute to leaky eigenmodes of the photonic crystal. By fabricating two-dimensional photonic crystal slabs that operate at visible wavelengths and engineering their leaky modes so that they overlap with the absorption and emission wavelengths of the quantum dots, we demonstrate that the fluorescence intensity can be enhanced by a factor of up to 108 compared with quantum dots on an unpatterned surface.     

硫化铜量子点的研究进展

硫化铜量子点作为一种p型半导体纳米晶,具有很强的表面等离子体共振效应、低的毒性以及独特的光学和电学性能,在光催化、生物技术、光电转换材料领域受到了极大关注。由于单分散的硫化铜量子点的制备过程复杂,效率较低,并且纯的硫化铜量子点电导率较低,这极大地限制了其在能量存储器件方面的应用。此外,由于硫化铜量子点复杂的能带结构和独特的p型半导体特性,针对硫化铜量子点的光学性能调控尚不成熟。基于此,本文综述了硫化铜量子点在制备方面的研究现状与取得的进展,介绍了硫化铜量子点的能带结构、晶体结构,及其在量子点敏化太阳能电池、光催化降解污染物、肿瘤细胞诊断与治疗等方面的研究进展,并对硫化铜量子点或Cu系量子点更进一步的研究、开发应用提出了几点建议。     

Imaging of resonant quenching of surface plasmons by quantum dots

In scanning tunneling microscopy (STM), confinement of surface plasmons to the optical cavity formed at the metallic tunneling gap stimulates the emission of light. We demonstrate that quantum dots (QDs) found in such a cavity give rise to discrete, observable transitions in the tunneling luminescence spectrum due to the resonant extinction of the plasmon. The observed resonances represent a fingerprint of the QD and occur at the optical band gap owing to the nearly simultaneous transfer of carriers from both sides of the tunneling gap to the QD. The resonant quenching of surface plasmons enables a new imaging technique, dubbed plasmon resonance imaging, with a spatial resolution potentially similar to that of STM and the energy resolution of optical spectroscopies. This detection and imaging strategy is not restricted to QDs, being of great interest to an entire spectrum of nanostructures, from molecular assemblies and biomolecules to carbon nanotubes.     

Optical forces in hybrid plasmonic waveguides

We demonstrate that in a hybrid plasmonic system the optical force exerted on a dielectric waveguide by a metallic substrate is enhanced by more than 1 order of magnitude compared to the force between a photonic waveguide and a dielectric substrate. A nanoscale gap between the dielectric waveguide and the metallic substrate leads to deep subwavelength optical energy confinement with ultralow mode propagation loss and hence results in the enhanced optical forces at low input optical power, as numerically demonstrated by both Maxwell's stress tensor formalism and the coupled mode theory analysis. Moreover, the hybridization between the surface plasmon modes and waveguide modes allows efficient optical trapping of single dielectric nanoparticle with size of only several nanometers in the gap region, manifesting various optomechanical applications such as nanoscale optical tweezers.     

Quantum dot/plasmonic nanoparticle metachromophores with quantum yields that vary with excitation wavelength

Coupled plasmonic/chromophore systems are of interest in applications ranging from fluorescent biosensors to solar photovoltaics and photoelectrochemical cells because near-field coupling to metal nanostructures can dramatically alter the optical performance of nearby materials. We show that CdSe quantum dots (QDs) near single silver nanoprisms can exhibit photoluminescence lifetimes and quantum yields that depend on the excitation wavelength, in apparent violation of the Kasha-Vavilov rule. We attribute the variation in QD lifetime with excitation wavelength to the wavelength-dependent coupling of higher-order plasmon modes to different spatial subpopulations of nearby QDs. At the QD emission wavelength, these subpopulations are coupled to far-field radiation with varying efficiency by the nanoprism dipolar resonance. These results offer an easily accessible new route to design metachromophores with tailored optical properties.     

Exciplex kinetics in nanocrystal organic light-emitting diodes

We studied the exciplex kinetics in nanocrystal organic light-emitting diodes (NC-OLEDs) where the emissive layer of inorganic nanocrystal quantum dots is sandwiched between the electron and hole transport layers of organic semiconductors at the organic–organic interface. We modeled exciplex generation, diffusion, recombination, and capture by nanocrystals via the Förster mechanism in NC-OLEDs. The exciplex kinetics determines the NC-OLED operation characterized by the quantum yield efficiency and emission intensity and it can be optimized by controlling the nanocrystal separation in the NC-OLED.     

One- and two-dimensional photonic crystal microcavities in single crystal diamond

Diamond is an attractive material for photonic quantum technologies because its colour centres have a number of outstanding properties, including bright single photon emission and long spin coherence times. To take advantage of these properties it is favourable to directly fabricate optical microcavities in high-quality diamond samples. Such microcavities could be used to control the photons emitted by the colour centres or to couple widely separated spins. Here, we present a method for the fabrication of one- and two-dimensional photonic crystal microcavities with quality factors of up to 700 in single crystal diamond. Using a post-processing etching technique, we tune the cavity modes into resonance with the zero phonon line of an ensemble of silicon-vacancy colour centres, and we measure an intensity enhancement factor of 2.8. The controlled coupling of colour centres to photonic crystal microcavities could pave the way to larger-scale photonic quantum devices based on single crystal diamond.     

Second‐Harmonic Generation from a Single Core/Shell Quantum Dot

Nanoparticles emitting two‐photon luminescence are broadly used as photostable emitters for nonlinear microscopy. Second‐harmonic generation (SHG) as another two‐photon mechanism offers complementary optical properties but the reported sizes of nanoparticles are still large, of a few tens of nanometers. Herein, coherent SHG from single core/shell CdTe/CdS nanocrystals with a diameter of 10 to 15 nm is reported. The nanocrystal excitation spectrum reveals resonances in the nonlinear efficiency with an overall maximum at about 970 nm. Polarization analysis of the second‐harmonic emission confirms the expected zinc blende symmetry, and allows extraction of the three‐dimensional nanocrystal orientation. The small size of these nonlinearly active quantum dots, together with the intrinsic coherence and orientation sensitivity of the SHG process, are well adapted for ultrafast probing of optical near‐fields with high resolution as well as for orientation tracking for bioimaging applications.     

Vertical growth and resonator properties of hexagonally shaped zinc oxide nanonails

We synthesized vertically aligned nail-shaped ZnO nanocrystal arrays on silicon substrates via a combination of a carbothermal reduction method and textured ZnO seeding layers that were precoated on silicon substrates by thermally decomposing zinc acetate, and studied their optical properties using cathodoluminescence (CL) and photoluminescence techniques. The ZnO nanonails show a sharp band-gap edge UV emission and a defect-related broad green emission. Monochromatic CL images of an individual ZnO nanonail show variations in spatial distributions of respective CL bands that had different origins. We attribute the spatial variation of CL images to an uneven distribution of luminescent defects and/or a structure-related light out-coupling from hexagonal ZnO nanostructures. The most distinct CL feature from the hexagonal head of an individual ZnO nanonail was the occurrence of a series of distinct resonant peaks within the visible wavelength range. It appeared that the head of a nanonail played the role of a hexagonal cavity so that polarization-dependent whispering gallery modes were stimulated by electron beam excitation.     

Exciplex kinetics in nanocrystal organic light-emitting diodes

We studied the exciplex kinetics in nanocrystal organic light-emitting diodes (NC-OLEDs) where the emissive layer of inorganic nanocrystal quantum dots is sandwiched between the electron and hole transport layers of organic semiconductors at the organic–organic interface. We modeled exciplex generation, diffusion, recombination, and capture by nanocrystals via the F?rster mechanism in NC-OLEDs. The exciplex kinetics determines the NC-OLED operation characterized by the quantum yield efficiency and emission intensity and it can be optimized by controlling the nanocrystal separation in the NC-OLED.     

Hybrid Frenkel-Wannier-Mott excitons at interfaces and in microcavities

We discuss the linear and nonlinear optical properties of organic-inorganic nanostructures (quantum wells and superlattices) brought about by resonance interactions between Frenkel excitons in organic QWs and Wannier-Mott excitons in semiconductor QWs. We show that such a coupling (Coulomb dipole-dipole at an interface and through the cavity photons in a microcavity) is responsible for the appearance of mixed Frenkel-Wannier excitations. We demonstrate that the new hybrid states and their dispersion curves can be tailored to engineer the enhancement of resonant optical nonlinearity, fluorescence efficiency and relaxation processes.     

Plasmonic antennas for directional sorting of fluorescence emission

Spontaneous emission of fluorescent molecules or quantum dots is radiated along all directions when emitters are diluted in a liquid solution, which severely limits the amount of collected light. Besides, the emission direction does not carry any useful information and cannot be used to sort different molecules. To go beyond these limits, optical antennas have been recently introduced as conceptual tools to control the radiation properties for nanoemitters fixed on a substrate. Despite intense recent research, controlling the luminescence directivity remains a challenge for emitters with random positions and orientations, which is a key for several biomolecular screening applications. Here, we present full directional control of the fluorescence emission from molecules in water solution by an optical antenna made of a nanoaperture surrounded by a periodic set of shallow grooves in a gold film. For each emission wavelength, the fluorescence beam can be directed along a specific direction with a given angular width, hereby realizing a micrometer-size dispersive antenna. We demonstrate the fluorescence beaming results from an interference phenomenon and provide physical optics guidelines to control the fluorescence directivity by tuning the groove-nanoaperture distance. This photon-sorting capability provides a new approach for high-sensitivity screening of molecular species in solution.     

Size selective excitonic transition energies in strongly confined CdSe quantum dots

We report on the synthesis of CdSe nanocrystal quantum dots (QDs) of different radii (R). Size dependent optical properties like increase in the confinement energy with decreasing radius for different excitonic transitions are studied. Different excitonic transitions are calculated from the second derivative of UV-vis absorption spectra of as synthesized CdSe QDs. The transitions are assigned to specific states by calculating the transition energies using effective mass approximation. A close matching of the transition energies with the experiment suggesting that the second derivative of the absorption spectra could provide a direct knowledge of the electronic transition for the direct band gap semiconductor quantum dots.