Scalable Route to Colloidal Ni x Co 3– x S 4 Nanoparticles with Low Dispersity Using Amino Acids
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Two-dimensional cadmium selenide nanoplatelets (NPLs) exhibit large absorption cross sections and homogeneously broadened band-edge transitions that offer utility in wide-ranging optoelectronic applications. Here, we examine the temperature-dependence of amplified spontaneous emission (ASE) in 4- and 5-monolayer thick NPLs and show that the threshold for close-packed (neat) films decreases with decreasing temperature by a factor of 2-10 relative to ambient temperature owing to extrinsic (trapping) and intrinsic (phonon-derived line width) factors. Interestingly, for pump intensities that exceed the ASE threshold, we find development of intense emission to lower energy in particular provided that the film temperature is <= 200 K. For NPLs diluted in an inert polymer, both biexcitonic ASE and low-energy emission are suppressed, suggesting that described neat-film observables rely upon high chromophore density and rapid, collective processes. Transient emission spectra reveal ultrafast red-shifting with the time of the lower energy emission. Taken together, these findings indicate a previously unreported process of amplified stimulated emission from polyexciton states that is consistent with quantum droplets and constitutes a form of exciton condensate. For studied samples, quantum droplets form provided that roughly 17 meV or less of thermal energy is available, which we hypothesize relates to polyexciton binding energy. Polyexciton ASE can produce pump-fluence-tunable red-shifted ASE even 120 meV lower in energy than biexciton ASE. Finally, our findings convey the importance of biexciton and polyexciton populations in nanoplatelets and show that quantum droplets can exhibit light amplification at significantly lower photon energies than biexcitonic ASE.
We demonstrate nearly a microsecond of spin coherence in Er 3+ ions doped in cerium dioxide nanocrystal hosts, despite a large gyromagnetic ratio and nanometric proximity of the spin defect to the nanocrystal surface. The long spin coherence is enabled by reducing the dopant density below the instantaneous diffusion limit in a nuclear spin-free host material, reaching the limit of a single erbium spin defect per nanocrystal. We observe a large Orbach energy in a highly symmetric cubic site, further protecting the coherence in a qubit that would otherwise rapidly decohere. Spatially correlated electron spectroscopy measurements reveal the presence of Ce 3+ at the nanocrystal surface, which likely acts as extraneous paramagnetic spin noise. Even with these factors, defect-embedded nanocrystal hosts show tremendous promise for quantum sensing and quantum communication applications, with multiple avenues, including core-shell fabrication, redox tuning of oxygen vacancies, and organic surfactant modification, available to further enhance their spin coherence and functionality in the future.
Photocatalytic materials for hydrogen generation are typically categorized into UV-absorbing metal oxides and visible-range semiconductors such as chalcogenides or perovskites, which often incorporate toxic elements. To address environmental concerns of the latter group, indium phosphide (InP)-based quantum dots (QDs) have recently emerged as a less toxic alternative. These nanocrystals (NCs) benefit from a broadband and tunable absorption spectrum, which is well matched for solar photochemistry, and offer suitable electronic characteristics to drive photoinduced charge separation. This perspective provides a comprehensive summary of the recent advancements in developing InP-based NCs with a focus on photocatalytic hydrogen production. We discuss synthetic strategies that enhance the catalytic activity of these materials and highlight key challenges that must be addressed to enhance their performance. Finally, we explore future research directions aimed at improving photocatalytic efficiency and integrating InP-based QDs into practical solar-to-fuel conversion systems.
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