The recent emergence of quantum-confined nanomaterials in the field of radiation detection, in particular lead halide perovskite nanocrystals, offers scalability and performance advantages over conventional materials. This development raises fundamental questions about the mechanism of scintillation itself at the nanoscale and the role of particle size, arguably the most defining parameter of quantum dots. Understanding this is crucial for the design and optimization of future nanotechnology scintillators.
View Article and Find Full Text PDFPerovskite nanocrystal superlattices are being actively studied after reports have emerged on collective excitonic properties at cryogenic temperatures, where energetic disorder is minimized due to the frozen lattice vibrations. However, an important issue related to structural disorder of superlattices at low temperatures has received little attention to date. In this work, it is shown that CsPbBr nanocrystal superlattices undergo a reversible order-disorder transition upon cooling to 90 K.
View Article and Find Full Text PDFHybrid Organic-Inorganic Halide Perovskites (HOIHPs) represent an emerging class of semiconducting materials, widely employed in a variety of optoelectronic applications. Despite their skyrocket growth in the last decade, a detailed understanding on their structure-property relationships is still missing. In this communication, we report two unprecedented perovskite-like materials based on polyfluorinated imidazolium cations.
View Article and Find Full Text PDFPsychiatrists play a crucial role in evaluating requests and treatment indications for individuals experiencing gender incongruence, while also providing support throughout the transition process. Their work involves addressing both the psychological and somatic aspects of this journey, facilitating the profound identity changes it entails.
View Article and Find Full Text PDFLead halide perovskite nanocrystals (LHP-NCs) embedded in polymeric hosts are gaining attention as scalable and low-cost scintillation detectors for technologically relevant applications. Despite rapid progress, little is currently known about the scintillation properties and stability of LHP-NCs prepared by the ligand assisted reprecipitation (LARP) method, which allows mass scalability at room temperature unmatched by any other type of nanostructure, and the implications of incorporating LHP-NCs into polyacrylate hosts are still largely debated. Here, we show that LARP-synthesized CsPbBr NCs are comparable to particles from hot-injection routes and unravel the dual effect of polyacrylate incorporation, where the partial degradation of LHP-NCs luminescence is counterbalanced by the passivation of electron-poor defects by the host acrylic groups.
View Article and Find Full Text PDFWe report the colloidal synthesis of Bi-doped CsAgNaInCl double perovskite nanoplatelets (NPLs) exhibiting a near-unity photoluminescence quantum yield (PLQY), a record emission efficiency for nanoscale lead-free metal halides. A combination of optical spectroscopies revealed that nonradiative decay processes in the NPL were suppressed, indicating a well-passivated surface. By comparison, nanocubes with the same composition and surface ligands as the NPLs had a PLQY of only 40%.
View Article and Find Full Text PDFThe use of scintillators for the detection of ionizing radiation is a critical aspect in many fields, including medicine, nuclear monitoring, and homeland security. Recently, lead halide perovskite nanocrystals (LHP-NCs) have emerged as promising scintillator materials. However, the difficulty of affordably upscaling synthesis to the multigram level and embedding NCs in optical-grade nanocomposites without compromising their optical properties still limits their widespread use.
View Article and Find Full Text PDFLuminescent solar concentrators (LSCs) are all-photonic, semitransparent solar devices with great potential in the emerging fields of building-integrated photovoltaics and agrivoltaics. Over the past decade, particularly with the advent of quantum dot (QD) LSCs, tremendous progress has been made in terms of photovoltaic efficiency and device size by increasing solar spectral coverage and suppressing reabsorption losses. Despite these advances in LSC design, the effects of environmental conditions such as rain, dust, and dirt deposits, which are ubiquitous in both urban and agricultural environments, on LSC performance have been largely overlooked.
View Article and Find Full Text PDFOwing to outstanding optoelectronic properties, lead halide perovskite nanocrystals (PNCs) are considered promising emitters for next-generation displays. However, the development of pure blue (460-470 nm) perovskite nanocrystal light-emitting diodes (PNC-LEDs), which correspond to the requirements of Rec. 2020 standard, lag far behind that of their green and red counterparts.
View Article and Find Full Text PDFCesium lead halide perovskite nanocrystals of general formula CsPbX are having tremendous impact on a vast array of technologies requiring strong and tunable luminescence across the visible range and solutions processing. The development of plastic scintillators is just one of the many relevant applications. The syntheses are relatively simple but generally unsuitable to produce a large amount of material of reproducible quality required when moving from proof-of-concept scale to industrial applications.
View Article and Find Full Text PDFOrganic-inorganic Pb-free layered perovskites are efficient broadband emitters and thus are promising materials for lighting applications. However, their synthetic protocols require a controlled atmosphere, high temperature, and long preparation time. This hinders the potential tunability of their emission through organic cations, as is instead common practice in Pb-based structures.
View Article and Find Full Text PDFMulticomponent systems consisting of lead halide perovskite nanocrystals (CsPbX-NCs, X = Br, I) grown inside mesoporous silica nanospheres (NSs) with selectively sealed pores combine intense scintillation and strong interaction with ionizing radiation of CsPbX NCs with the chemical robustness in aqueous environment of silica particles, offering potentially promising candidates for enhanced radiotherapy and radio-imaging strategies. We demonstrate that CsPbX NCs boost the generation of singlet oxygen species (O) in water under X-ray irradiation and that the encapsulation into sealed SiO NSs guarantees perfect preservation of the inner NCs after prolonged storage in harsh conditions. We find that the O production is triggered by the electromagnetic shower released by the CsPbX NCs with a striking correlation with the halide composition (I > I Br > Br).
View Article and Find Full Text PDFColloidal CdTe nanoplatelets featuring a large absorption coefficient and ultrafast tunable luminescence coupled with heavy-metal-based composition present themselves as highly desirable candidates for radiation detection technologies. Historically, however, these nanoplatelets have suffered from poor emission efficiency, hindering progress in exploring their technological potential. Here, we report the synthesis of CdTe nanoplatelets possessing a record emission efficiency of 9%.
View Article and Find Full Text PDFIn this work, we report the hot-injection synthesis of CsZnCl colloidal nanocrystals (NCs) with tunable amounts of Cu and Mn substituent cations. All the samples had a rodlike morphology, with a diameter of ∼14 nm and a length of ∼30-100 nm. Alloying did not alter the crystal structure of the host CsZnCl NCs, and Cu ions were mainly introduced in the oxidation state +1 according to X-ray photoelectron and electron paramagnetic resonance spectroscopies.
View Article and Find Full Text PDFColloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed.
View Article and Find Full Text PDFSimultaneously achieving both broad absorption and sharp emission in the near-infrared (NIR) is challenging. Coupling of an efficient absorber such as lead halide perovskites to lanthanide emissive species is a promising way to meet the demands for visible-to-NIR spectral conversion. However, lead-based perovskite sensitizers suffer from relatively narrow absorption in the visible range, poor stability, and toxicity.
View Article and Find Full Text PDFIn June 2021, the Swiss parliament accepted a legislative proposal calling for the introduction of a fee to fight emergency department (ED) overcrowding. Although this issue remains a major challenge for health policies, the introduction of such a fee raises many questions, notably regarding health equity. However, other more equitable solutions exist: improving the case management of ED frequent users and improving coordination between ED and primary care.
View Article and Find Full Text PDFWe synthesize colloidal nanocrystals (NCs) of RbInCl, composed of isolated metal halide octahedra ("0D"), and of CsNaInCl and CsKInCl double perovskites, where all octahedra share corners and are interconnected ("3D"), with the aim to elucidate and compare their optical features once doped with Sb ions. Our optical and computational analyses evidence that the photoluminescence quantum yield (PLQY) of all these systems is consistently lower than that of the corresponding bulk materials due to the presence of deep surface traps from under-coordinated halide ions. Also, Sb-doped "0D" RbInCl NCs exhibit a higher PLQY than Sb-doped "3D" CsNaInCl and CsKInCl NCs, most likely because excitons responsible for the PL emission migrate to the surface faster in 3D NCs than in 0D NCs.
View Article and Find Full Text PDFColloidal semiconductor nanoplatelets (NPLs) are a subgroup of quantum confined materials that have recently emerged as promising active materials for solution processed light-emitting diodes (LEDs) thanks to their peculiar structural and electronic properties as well as their reduced dimensionality. Nowadays, the conventional structure for NPL-based LEDs makes use of poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) as a hole transporting layer (HTL). This is a well-known conjugated conductive polymer because it leads to high LED efficiency, though it has limited stability in air due to its intrinsic acidity and hygroscopicity.
View Article and Find Full Text PDFWe report here the synthesis of undoped and Cu-doped CsZnCl nanocrystals (NCs) in which we could tune the concentration of Cu from 0.7 to 7.5%.
View Article and Find Full Text PDFWe report the synthesis of colloidal CsPbX-PbSBr (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr-PbSBr nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments.
View Article and Find Full Text PDFWe devised a hot-injection synthesis to prepare colloidal double-perovskite CsNaBiCl nanocrystals (NCs). We also examined the effects of replacing Na with Ag cations by preparing and characterizing CsNa Ag BiCl alloy NCs with ranging from 0 to 1. Whereas CsNaBiCl NCs were not emissive, CsNa Ag BiCl NCs featured a broad photoluminescence band at ∼690 nm, Stokes-shifted from the respective absorption by ≥1.
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