We studied the chemical, optical and catalytic properties of metal (Pt, Pd, Ag, Au)-Cu 2 O core-shell nanoparticles grown via a simple and reproducible approach which utilizes aqueous-phase reactions at room temperature. We were able to control the thickness of the Cu 2 O shell and examine the effect of the core's shape and size on the structure and properties of the hybrid nanocrystals. We also studied the optical properties of the hybrid nanocrystals, in particular the effect of the Cu 2 O shell thickness on the frequency of the plasmon of gold nanorods. In addition, the catalytic activity of the hybrid nanostructures was examined by testing the reduction reaction of 4-nitrophenol with NaBH 4 . Finally, the hybrid metal-Cu 2 O nanostructures were used as templates to form the yolk-shell of metal-Cu 2 S materials. The interface and the crystalline structures of the four hybrid nanostructures were extensively characterized by high resolution transmission electron microscopy (HRTEM), energy-filtered TEM (EFTRM) and X-ray diffraction (XRD).

We optimized the performance of quantum confined Stark effect (QCSE)-based voltage nanosensors. A high-throughput approach for single-particle QCSE characterization was developed and utilized to screen a library of such nanosensors. Type-II ZnSe/CdS seeded nanorods were found to have the best performance among the different nanosensors evaluated in this work.The degree of correlation between intensity changes and spectral changes of the exciton's emission under applied field was characterized. An upper limit for the temporal response of individual ZnSe/CdS nanorods to voltage modulation was characterized by high-throughput, high-temporal resolution intensity measurements using a novel photon-counting camera. The measured 3.5 μs response time is limited by the voltage modulation electronics and represents ~ x 30 times higher bandwidth than needed for recording an action potential in a neuron.

ConspectusPairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots.The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole–dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs).One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion.This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

Solution-processed core/multishell semiconductor quantum dots (QDs) could be tailored to facilitate the carrier separation, promotion, and recombination mechanisms necessary to implement photon upconversion. In contrast to other upconversion schemes, upconverting QDs combine the stability of an inorganic crystalline structure with the spectral tunability afforded by quantum confinement. Nevertheless, their upconversion quantum yield (UCQY) is fairly low. Here, design rules are uncovered that enable to significantly enhance the performance of double QD upconversion systems, and these findings are leveraged to fabricate upconverting QDs with increased photon upconversion efficiency and reduced saturation intensities under pulsed excitation. The role of the intra-QD band alignment is exemplified by comparing the upconversion process in PbS/CdS/ZnSe QDs with that of PbS/CdS/CdSe ones with variable CdSe shell thicknesses. It is shown that electron delocalization into the shell leads to a longer-lived intermediate state in the QDs, facilitating further absorption of photons, and enhancing the upconversion process. The performance of these upconversion QDs under pulsed excitation versus continuous pumping is also compared; the reasons for the significant differences between these two regimes are discussed. The results show how one can overcome some of the limitations of previous upconverting QDs, with potential applications in biophotonics and infrared detection.

We investigated the effect of cation exchange on the anionic framework of lightly doped CdSe:Te/CdS nanorods. In contrast with previously studied core/shell systems, the Te dopant, located in the center of the CdSe core, provides an extremely sensitive indicator for any structural changes of the anionic framework that may occur as a result of the cation exchange process. We first optimized the cation exchange procedure in order to retain the fluorescence properties of the CdSe:Te/ CdS nanorods after exchange of Cd 2+ for Cu + and back to Cd 2+ . Next, using multiexciton spectroscopy, we were able to probe the magnitude of the exciton−exciton repulsion interaction and use that to assess the degree of crystal structure conservation. Our findings provide a much stronger proof that the anion framework is indeed rigid, showing no evidence of significant migration of the anionic dopant.