Colloidal lead halide perovskite (LHP) nanocrystals are of interest as photoluminescent quantum dots (QDs) whose properties depend on the size and shape. They are normally synthesized on subsecond time scales through hard-to-control ionic metathesis reactions. We report a room-temperature synthesis of monodisperse, isolable spheroidal APbBr 3 QDs (A=Cs, formamidinium, methylammonium) that are size-tunable from 3 to over 13 nanometers. The kinetics of both nucleation and growth are temporally separated and drastically slowed down by the intricate equilibrium between the precursor (PbBr 2 ) and the A[PbBr 3 ] solute, with the latter serving as a monomer. QDs of all these compositions exhibit up to four excitonic transitions in their linear absorption spectra, and we demonstrate that the size-dependent confinement energy for all transitions is independent of the A-site cation.
One of the most attractive commercial applications of semiconductor nanocrystals (NCs) is their use in lasers. Thanks to their high quantum yield, tunable optical properties, photostability, and wet-chemical processability, NCs have arisen as promising gain materials. Most of these applications, however, rely on incorporation of NCs in lasing cavities separately produced using sophisticated fabrication methods and often difficult to manipulate. Here, we present whispering gallery mode lasing in supraparticles (SPs) of self-assembled NCs. The SPs composed of NCs act as both lasing medium and cavity. Moreover, the synthesis of the SPs, based on an in-flow microfluidic device, allows precise control of the dimensions of the SPs, i.e. the size of the cavity, in the micrometer range with polydispersity as low as several percent. The SPs presented here show whispering gallery mode resonances with quality factors up to 320. Whispering gallery mode lasing is evidenced by a clear threshold behavior, coherent emission, and emission lifetime shortening due to the stimulation process.
Fast neutrons offer high penetration capabilities for both light and dense materials due to their comparatively low interaction cross sections, making them ideal for the imaging of large-scale objects such as large fossils or as-built plane turbines, for which X-rays or thermal neutrons do not provide sufficient penetration. However, inefficient fast neutron detection limits widespread application of this technique. Traditional phosphors such as ZnS:Cu embedded in plastics are utilized as scintillators in recoil proton detectors for fast neutron imaging. However, these scintillation plates exhibit significant light scattering due to the plastic−phosphor interface along with long-lived afterglow (on the order of minutes), and therefore alternative solutions are needed to increase the availability of this technique. Here, we utilize colloidal nanocrystals (NCs) in hydrogen-dense solvents for fast neutron imaging through the detection of recoil protons generated by neutron scattering, demonstrating the efficacy of nanomaterials as scintillators in this detection scheme. The light yield, spatial resolution, and neutron-vs-gamma sensitivity of several chalcogenide (CdSe and CuInS 2 )-based and perovskite halide-based NCs are determined, with only a short-lived afterglow (below the order of seconds) observed for all of these NCs. FAPbBr 3 NCs exhibit the brightest total light output at 19.3% of the commercial ZnS:Cu(PP) standard, while CsPbBrCl 2 :Mn NCs offer the best spatial resolution at ∼2.6 mm. Colloidal NCs showed significantly lower gamma sensitivity than ZnS:Cu; for example, 79% of the FAPbBr 3 light yield results from neutron-induced radioluminescence and hence the neutron-specific light yield of FAPbBr 3 is 30.4% of that of ZnS:Cu(PP). Concentration and thickness-dependent measurements highlight the importance of increasing concentrations and reducing self-absorption, yielding design principles to optimize and foster an era of NC-based scintillators for fast neutron imaging.
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