Effect of chemical composition on luminescence of thiol-stabilized CdTe nanocrystals

Judicious selection of the amount of surfactant during synthesis enables a drastic increase in the photoluminescence efficiency of aqueous CdTe nanocrystals (NCs) stabilized by thioglycolic acid (TGA). Elemental determination of the NCs was undertaken to identify the origin of this effect. The molar ratio of (Te + S) to Cd approached unity when the optimum amount of TGA was used during synthesis, whereas the number of S atoms originating from TGA molecules in one NC (2.6 nm of diameter) remained unchanged at 90 ± 3. This indicates that the core lattice composition at the beginning of synthesis, rather than the surface conditions, affects the photoluminescence efficiency of the NCs even after prolonged refluxing

Archimedean-like colloidal tilings on substrates with decagonal and tetradecagonal symmetry

Two-dimensional colloidal suspensions subject to laser interference patterns with decagonal symmetry can form an Archimedean-like tiling phase where rows of squares and triangles order aperiodically along one direction [J. Mikhael et al., Nature 454, 501 (2008)]. In experiments as well as in Monte-Carlo and Brownian dynamics simulations, we identify a similar phase when the laser field possesses tetradecagonal symmetry. We characterize the structure of both Archimedean-like tilings in detail and point out how the tilings differ from each other. Furthermore, we also estimate specific particle densities where the Archimedean-like tiling phases occur. Finally, using Brownian dynamics simulations we demonstrate how phasonic distortions of the decagonal laser field influence the Archimedean-like tiling. In particular, the domain size of the tiling can be enlarged by phasonic drifts and constant gradients in the phasonic displacement. We demonstrate that the latter occurs when the interfering laser beams are not adjusted properly

Multiband tight-binding theory of disordered ABC semiconductor quantum dots: Application to the optical properties of alloyed CdZnSe nanocrystals

Zero-dimensional nanocrystals, as obtained by chemical synthesis, offer a broad range of applications, as their spectrum and thus their excitation gap can be tailored by variation of their size. Additionally, nanocrystals of the type ABC can be realized by alloying of two pure compound semiconductor materials AC and BC, which allows for a continuous tuning of their absorption and emission spectrum with the concentration x. We use the single-particle energies and wave functions calculated from a multiband sp^3 empirical tight-binding model in combination with the configuration interaction scheme to calculate the optical properties of CdZnSe nanocrystals with a spherical shape. In contrast to common mean-field approaches like the virtual crystal approximation (VCA), we treat the disorder on a microscopic level by taking into account a finite number of realizations for each size and concentration. We then compare the results for the optical properties with recent experimental data and calculate the optical bowing coefficient for further sizes

The Role of Intrinsic and Surface States on the Emission Properties of Colloidal CdSe and CdSe/ZnS Quantum Dots

Time Resolved Photoluminescence (TRPL) measurements on the picosecond time scale (temporal resolution of 17 ps) on colloidal CdSe and CdSe/ZnS Quantum Dots (QDs) were performed. Transient PL spectra reveal three emission peaks with different lifetimes (60 ps, 460 ps and 9–10 ns, from the bluest to the reddest peak). By considering the characteristic decay times and by comparing the energetic separations among the states with those theoretically expected, we attribute the two higher energy peaks to ± 1Uand ± 1L bright states of the fine structure picture of spherical CdSe QDs, and the third one to surface states emission. We show that the contribution of surface emission to the PL results to be different for the two samples studied (67% in the CdSe QDs and 32% in CdSe/ZnS QDs), confirming the decisive role of the ZnS shell in the improvement of the surface passivation

Quantum dots coordinated with conjugated organic ligands: new nanomaterials with novel photophysics

CdSe quantum dots functionalized with oligo-(phenylene vinylene) (OPV) ligands (CdSe-OPV nanostructures) represent a new class of composite nanomaterials with significantly modified photophysics relative to bulk blends or isolated components. Single-molecule spectroscopy on these species have revealed novel photophysics such as enhanced energy transfer, spectral stability, and strongly modified excited state lifetimes and blinking statistics. Here, we review the role of ligands in quantum dot applications and summarize some of our recent efforts probing energy and charge transfer in hybrid CdSe-OPV composite nanostructures

The surface science of nanocrystals

All nanomaterials share a common feature of large surface-to-volume ratio, making their surfaces the dominant player in many physical and chemical processes. Surface ligands-molecules that bind to the surface-are an essential component of nanomaterial synthesis, processing and application. Understanding the structure and properties of nanoscale interfaces requires an intricate mix of concepts and techniques borrowed from surface science and coordination chemistry. Our Review elaborates these connections and discusses the bonding, electronic structure and chemical transformations at nanomaterial surfaces. We specifically focus on the role of surface ligands in tuning and rationally designing properties of functional nanomaterials. Given their importance for biomedical (imaging, diagnostics and therapeutics) and optoelectronic (light-emitting devices, transistors, solar cells) applications, we end with an assessment of application-targeted surface engineering. © 2016 Macmillan Publishers Limited. All rights reserved32233

Photocurrent enhancement in hybrid nanocrystal quantum-dot p-i-n photovoltaic devices

We fabricate a hybrid nanocrystal quantum-dot patterned p-i-n structure that utilizes nonradiative energy transfer from highly absorbing colloidal nanocrystal quantum dots to a patterned semiconductor slab to demonstrate a sixfold increase of the photocurrent conversion efficiency compared to the bare p-i-n semiconductor device.<br/