Solution-phase spectroelectrochemistry was used to study electron injection into colloidal CdSe quantum dots (QDs) with sizes ranging from 3.4 to 11.1 nm in tetrahydrofuran (THF). The absorbance and photoluminescence of the QDs were monitored in response to both charging and discharging cycles, and the optical changes were reversible on a timescale of minutes. Bleaching of the QD 1S 3/2h 1S e exciton state was used to determine the conduction band energy levels. We found that the negative trion state was stable in THF for hours under an applied cathodic potential. Both the degree of bleaching and the recovery of the exciton state depended on the applied potential. Based on the current and charge measurements, we found that between 10 and 150 electrons were injected into the QDs, depending on the electrode potential and QD size. Most of the electron injection occurred below the band edge and led to quenching of the QD photoluminescence. The potential at which injection into QDs occurred depended on the nature of the QD ligands.
Controlled nanocrystal assembly is a pre‐requisite for incorporation of these materials into solid state devices. Many assembly methods have been investigated which target precise nanocrystal positioning, high process controllability, scalability, and universality. However, most methods are unable to achieve all of these goals. Here, surface templated electrophoretic deposition (STED) is presented as a potential assembly method for a wide variety of nanocrystals. Controlled positioning and deposition of a wide range of nanocrystals into arbitrary spatial arrangements − including gold nanocrystals of different shapes and sizes, magnetic nanocrystals, fluorescent organic nanoparticles, and semiconductor quantum dots − is demonstrated. Nanoparticles with diameters <10 nm are unable to be deposited due to their low surface charge and strong Brownian motion (low Péclet number). It is shown that this limit can be circumvented by forming clusters of nanocrystals or by silica coating nanocrystals to increase their effective size.
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.
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 × 10 9 and 1.6 × 10 11 cm Hz 1/2 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.
The first examples of neutral and cationic bismuth complexes bearing β-ketoiminato ligands were isolated by employing salt metathesis route. BiCl 3 reacts with [O=C(Me)]CH[C(Me)N(K)Ar] (1) resulting in a homoleptic β-ketoiminato bismuth complex Bi[{O=
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