Electrophoretic Deposition of Single Nanoparticles.

The controlled assembly of colloid particles on a solid substrate has always been a major challenge in colloid and surface science. Here we provide an overview of electrophoretic deposition (EPD) of single charge-stabilized nanoparticles. We demonstrate that surface templated EPD (STEPD) assembly, which combines EPD with top-down nanofabrication, allows a wide range of nanoparticles to be built up into arbitrary structures with high speed, scalability, and excellent fidelity. We will also discuss some of the current colloid chemical limitations and challenges in STEPD assembly for sub-10 nm nanoparticles and for the fabrication of densely packed single particle arrays.

Temperature Dependence of the CdS Bandgap in the Extreme Confinement Regime.

A non-empirical equation describing the effect of size on the temperature dependence of the optical bandgap of CdS (dEg/dT) is obtained on the basis of the Brus equation. Intriguingly, we find that dEg/dT diverges strongly from bulk values only within the "extreme confinement" (EC) regime. We conducted both experimental and theoretical investigations of the absorption spectra of CdS clusters and quantum dots as a function of temperature above room temperature. Our results show that the value of dEg/dT obtained from absorption spectra in the EC regime is 2.5 times higher than in the strong confinement regime. Notable ligand sensitivities are also observed for dEg/dT in the case of CdS clusters. Ab initio molecular dynamics simulations and density functional theory calculations reveal that thermal fluctuations are the crucial factor influencing the bandgap temperature coefficient. Our results help resolve some long-standing debates regarding the dEg/dT behavior of semiconductor quantum dots.

Room Temperature Bias-Selectable, Dual-Band Infrared Detectors Based on Lead Sulfide Colloidal Quantum Dots and Black Phosphorus.

A single photodetector capable of switching its peak spectral photoresponse between two wavelength bands is highly useful, particularly for the infrared (IR) bands in applications such as remote sensing, object identification, and chemical sensing. Technologies exist for achieving dual-band IR detection with bulk III-V and II-VI materials, but the high cost and complexity as well as the necessity for active cooling associated with some of these technologies preclude their widespread adoption. In this study, we leverage the advantages of low-dimensional materials to demonstrate a bias-selectable dual-band IR detector that operates at room temperature by using lead sulfide colloidal quantum dots and black phosphorus nanosheets. By switching between zero and forward bias, these detectors switch peak photosensitive ranges between the mid- and short-wave IR bands with room temperature detectivities of 5 × 109 and 1.6 × 1011 cm Hz1/2 W-1, respectively. To the best of our knowledge, these are the highest reported room temperature values for low-dimensional material dual-band IR detectors to date. Unlike conventional bias-selectable detectors, which utilize a set of back-to-back photodiodes, we demonstrate that under zero/forward bias conditions the device's operation mode instead changes between a photodiode and a phototransistor, allowing additional functionalities that the conventional structure cannot provide.

Spectroelectrochemistry of CdSe/CdxZn1-xS Nanoplatelets.

We report an unexpected enhancement of photoluminescence (PL) in CdSe-based core/shell nanoplatelets (NPLs) upon electrochemical hole injection. Moderate hole doping densities induce an enhancement of more than 50% in PL intensity. This is accompanied by a narrowing and blue-shift of the PL spectrum. Simultaneous, time-resolved PL experiments reveal a slower luminescence decay. Such hole-induced PL brightening in NPLs is in stark contrast to the usual observation of PL quenching of CdSe-based quantum dots following hole injection. We propose that hole injection removes surface traps responsible for the formation of negative trions, thereby blocking nonradiative Auger processes. Continuous photoexcitation causes the enhanced PL intensity to decrease back to its initial level, indicating that photocharging is a key step leading to loss of PL luminescence during normal aging. Modulating the potential can be used to reversibly enhance or quench the PL, which enables electro-optical switching.