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29 records · Page 2

Performance optimization for hard X-ray/soft gamma-ray detectors

This paper discusses the optimization of the performance of imaging scintillation detectors used in the hard X-ray/soft gamma-ray (20-300) keV region of the spectrum. In these devices, absorption of an incident gamma-ray within an alkali halide crystal induces a scintillation light distribution which is centroided by an imaging photomultiplier tube mounted to the crystal. The ultimate imaging resolution is strongly affected by the detailed propagation of the scintillation light within the crystal and at the interface between the crystal and the phototube face plate. A number of refined techniques for preparing the scintillation crystals so as to optimize the imaging resolution have been investigated. The results indicate very good agreement with relatively simple models of the light propagation. It is shown that it is possible to achieve resolution consistent with the most optimistic models.

Harrison, Fiona A.↗

Intrinsic scintillation performance & europium concentration effects in RbSr 2 I 5 and RbSr 2 Br 5 scintillators

Scintillators play crucial roles in homeland security applications like gamma ray spectroscopy and high energy X-ray radiography. For promising new scintillators, fine-tuning the luminescent dopant concentration is one avenue to further improve their performance and tailor their properties. In this work, the effects of europium dopant concentrations on the crystal growth, luminescence and scintillation properties of RbSr 2 Br 5 and RbSr 2 I 5 crystals was investigated. Nine transparent 7 mm diameter single crystals were grown via the Vertical Bridgman method. Here, the optical band gap of RbSr 2 Br 5 was 5.9 eV and that of RbSr 2 I 5 was 4.7 eV. High scintillation performance was achieved with a relatively low europium concentration of 1 mol%. For both RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu crystals, light yield of 60–90,000 ph/MeV, energy resolution 2.8–4.0 % at 662 keV, and X-ray afterglow 0.79–1.5 % at 2 ms were obtained.

36 MATERIALS SCIENCE↗

Exploring the physics of cesium lead halide perovskite quantum dots via Bayesian inference of the photoluminescence spectra in automated experiment

The unique optoelectronic properties of metal halide perovskite quantum dots (QDs) make them promising candidates for applications in light-emitting diodes (LEDs), scintillators, and other photonic devices. The automated micropipetting synthesis platform equipped with an optical reader enables the opportunity for high throughput synthesis and photoluminescent (PL) characterization of metal halide perovskite QDs for the first time. Here, we explore the compositional dependence of the PL behavior and stability of the combinatorial library of cesium lead halide (CsPbX 3 ) perovskites QDs via the automated platform. To study the stability of synthesized QDs in the binary and ternary configurations, we study the time-dependent PL properties using previously developed machine learning analysis. Additionally, to systematically explore the PL behavior in the ternary CsPbX 3 QDs system, we introduce the Bayesian inference framework that allows the probabilistic fit of multiple models to the PL data and establishes both optimal model and model parameter robustly. Furthermore, these behaviors can be used as a control parameter for the navigation of the multidimensional compositional spaces in automated synthesis. Furthermore, this analysis shows the nonuniformity of the PL peak behavior in the ternary CsPbX 3 QDs system. Further, the analysis confirms narrow size distribution and good quality of CsPbBr 3 QDs alloyed with low concentrations of iodide and chloride. We note that Bayesian Inference fit parameters can be further used as a control signal for navigation of the chemical spaces in automated synthesis.

36 MATERIALS SCIENCE↗

Colorimetric radiation detector

A low cost, rapid, flexible radiation detector uses inorganic metal halide precursors and dyes that respond to self-quenching hybrid scintillation. Remote, high-contrast, laser sensing can be used to determine when exposure of the detector to radiation occurs (even temporally).

Boyle, Timothy J.↗

Colorimetric radiation detector

A low cost, rapid, flexible radiation detector uses inorganic metal halide precursors and dyes that respond to self-quenching hybrid scintillation. Remote, high-contrast, laser sensing can be used to determine when exposure of the detector to radiation occurs (even temporally).

Garzon, Fernando Henry↗

The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals

Since the initial discovery of colloidal lead halide perovskite nanocrystals, there has been significant interest placed on these semiconductors because of their remarkable optoelectronic properties, including very high photoluminescence quantum yields, narrow size- and composition-tunable emission over a wide color gamut, defect tolerance, and suppressed blinking. These material attributes have made them attractive components for next-generation solar cells, light emitting diodes, low-threshold lasers, single photon emitters, and X-ray scintillators. While a great deal of research has gone into the various applications of colloidal lead halide perovskite nanocrystals, comparatively little work has focused on the fundamental surface chemistry of these materials. While the surface chemistry of colloidal semiconductor nanocrystals is generally affected by their particle morphology, surface stoichiometry, and organic ligands that contribute to the first coordination sphere of their surface atoms, these attributes are markedly different in lead halide perovskite nanocrystals because of their ionicity. Herein, emerging work on the surface chemistry of lead halide perovskite nanocrystals is highlighted, with a particular focus placed on the most-studied composition of CsPbBr 3 . We begin with an in-depth exploration of the native surface chemistry of as-prepared, 0-D cuboidal CsPbBr 3 nanocrystals, including an atomistic description of their surface termini, vacancies, and ionic bonding with ligands. We then proceed to discuss various post-synthetic surface treatments that have been developed to increase the photoluminescence quantum yields and stability of CsPbBr 3 nanocrystals, including the use of tetraalkylammonium bromides, metal bromides, zwitterions, and phosphonic acids, and how these various ligands are known to bind to the nanocrystal surface. To underscore the effect of post-synthetic surface treatments on the application of these materials, we focus on lead halide perovskite nanocrystal-based light emitting diodes, and the positive effect of various surface treatments on external quantum efficiencies. We also discuss the current state-of-the-art in the surface chemistry of 1-D nanowires and 2-D nanoplatelets of CsPbBr 3 , which are more quantum confined than the corresponding cuboidal nanocrystals but also generally possess a higher defect density because of their increased surface area-to-volume ratios.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crystal growth and scintillation properties of new ytterbium-activated scintillators Cs 4 CaI 6 :Yb and Cs 4 SrI 6 :Yb

Yb 2+ was investigated as a potential alternative activator for Cs 4 SrI 6 and Cs 4 CaI 6 scintillators for the first time, as opposed to the previously studied Eu2+ activator. Single crystals with nominal Yb 2+ concentrations of 0.5 mol%, 1 mol%, and 3 mol% were grown in Ø7 mm ampoules using the vertical Bridgman method. Luminescence and scintillation properties were evaluated as a function of Yb 2+ concentration and host compound. Here, the 5d → 4f electronic transition of Yb 2+ was observed for both the Sr- and Ca-containing compositions. X-ray induced radioluminescence emission was centered between 449 nm and 463 nm depending on Yb 2+ concentration and host compound. Both the spin-allowed and spin-forbidden transitions were observed in photoluminescence emission spectra and were centered at 446 nm and 476 nm, respectively, for both compounds. The best scintillation performance was achieved with Cs 4 CaI 6 :Yb 1 mol%, which had a 3.5% energy resolution at 662 keV and 43,000 ph/MeV light yield. To our knowledge this is the best energy resolution ever reported for a Yb 2+ -doped scintillator. Additional Cs 4 CaI 6 :Yb 1% crystals were grown in Ø12 mm ampoules to investigate the size dependence of scintillation properties, as well as crystal homogeneity.

36 MATERIALS SCIENCE↗

Optimized Photoemission from Organic Molecules in 2D Layered Halide Perovskites

In recent years, hybrid organic−inorganic metal halides have been at the forefront of materials research. Typically, the functional (e.g., optoelectronic) properties of hybrid halides are derived from the inorganic structural part, whereas the organic structural units can add extra advantages in terms of stability, rigidity, and processability. Here, we report the design, synthesis, and characterization of two new hybrid materials in which the outstanding photophysical properties originate from the organic structural part. The new compounds, (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , have 2D layered Ruddlesden−Poppertype perovskite structures. These hybrids are blue-white light emitters just like their corresponding pure organic salts, but with much improved emission efficiencies. Optical spectroscopy and density functional theory (DFT) studies confirm that photoemission comes from the trans-stilbene organic cations. The photoluminescence quantum yield (PLQY) values of these new materials are among the highest known, 50.83% and 26.60% for (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , respectively. This is up to a 5-fold increase as compared to the light emission efficiency of the precursor salt C 15 H 16 NCl (PLQY of 10.33%). Alongside their outstanding optical properties, their environmental and thermal stability allow their consideration for potential practical applications such as radiation detection. This work shows that hybrid metal halides can be compositionally and structurally engineered to have highly efficient photoemission originating from the organic components for fast scintillation applications.

Halogens↗

The Path to Enlightenment: Progress and Opportunities in High Efficiency Halide Perovskite Light-Emitting Devices

Besides the flourishment in photovoltaics, halide perovskites hold great promise to compete with leading contenders among solution-processed emitters, such as organics and semiconductor colloidal nanocrystals, in the field of light emission. Halide perovskites exhibit outstanding optoelectronic properties, including high photoluminescence quantum yields, facile bandgap tunability, narrow emission line widths, and respectable carrier mobilities, promoting them to thrive in versatile light-emitting applications such as light-emitting diodes, lasers, X-ray scintillators, and circularly polarized light sources. Herein, we discuss the underlying physics of light emission in state-of-the-art perovskite light-emitting devices and focus on promising strategies for further improvement of device performance.

42 ENGINEERING↗

Structural Changes in Molten Salt Fuel and/or Waste Stream Compounds Cs 2 UCl 6 and Cs 2 UO 2 Cl 4 from Room Temperature to Melting and Related Materials [Slides]

Perovskite phases have been explored in recent literature as waste forms for long term storage of radioactive waste from molten salt reactors specifically. Synthesis of new halide perovskite phases can inform these efforts as well as molten salt reactor chemistry in general. Inorganic perovskites have also shown promise as new scintillating materials for detection of X-rays and gamma rays. Modifying the structure and chemistry of these compounds, perhaps with organic components, could be used to synthesize new scintillating compounds or modify the properties of existing ones. Both U 6+ and U 4+ readily form compounds with a striking similarity to vacancy ordered perovskites (Cs 2 UO 2 Cl 4 and Cs 2 UCl 6 ). Each of these compounds is relevant to molten salt reactor chemistry and/or waste streams. These phases could from in uranium chloride salt systems or waste streams: Cs being a fission product.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Eutectic Processing of Semiconductor Colloidal Nanocrystals for Energy Applications

Colloidal semiconductor nanocrystals (NCs) offer a costeffective platform for light-energy conversion in X-ray scintillators, photovoltaics, lasers, and display technologies. Yet, device-relevant NCs often require complex heterostructured compositions, where lattice imperfections compromise the efficiency and stability of photoconversion processes. Here, we show that a simple synthetic detour through a eutectic state of II−VI semiconductor NCs (e.g., CdSe, ZnSe) with halide salts (e.g., CdCl 2 , ZnCl 2 ) overcomes this limitation by melting and reconstructing NC lattices into defect-free alloyed and core/shell architectures. Applied to ternary CdSeTe NCs, this process produces downconverters with record brightness and minimal line widths, delivering a 3-fold increase in film-side external quantum efficiency of commercial CdTe photovoltaic modules (First Solar Inc.). Meanwhile, eutectic processing of CdSe-based core/shell emitters yields an 8-fold enhancement in their photoluminescence stability under backlight operation, addressing the reliability bottleneck for display technologies. Together, these findings establish eutectic NC processing as a scalable route to efficient, durable photoconversion materials for energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗