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Abstract Over the past decade, lead halide perovskites have gained significant interest for ionizing radiation detection, owing to their exceptional performance, and cost-effective fabrication in a wide range of form factors, from thick films to large single crystals. However, the toxicity of lead, limited environmental and thermal stability of these materials, as well as dark current drift due to ionic conductivity, have prompted the development of alternative materials that can address these challenges. Bismuth-based compounds (including perovskite derivatives and nonperovskite materials) have similarly high atomic numbers, leading to strong X-ray attenuation, but have lower toxicity, tend to be more environmentally stable, and can have lower ionic conductivity, especially in low-dimensional materials. These materials are also advantageous over commercial direct X-ray detectors by being able to detect lower dose rates of X-rays than amorphous selenium by at least two orders of magnitude, are potentially more cost-effective to mass produce than cadmium zinc telluride, and can operate at room temperature (unlike high-purity Ge). Given the strong interest in this area, we here discuss recent advances in the development of bismuth-based perovskite derivatives (with 3D, 2D and 0D structural dimensionality), and other bismuth-based perovskite-inspired materials for direct X-ray detection. We discuss the critical properties of these materials that underpin the strong performances achieved, particularly the ability to detect low-dose rates of X-rays. We cover key strategies for enhancing the performance of these materials, as well as the challenges that need to be overcome to commercialize these emerging technologies. Graphical abstractmore » « less
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Abstract In this study, we demonstrate a novel approach for synthesizing free‐standing and transferable polycrystalline diamond membranes (PCDm) to overcome these constraints, thus enabling a much wider spectrum of applications. Two types of PCDm cantilevers —Top‐Surface‐Up (TSU) and Bottom‐Surface‐Up (BSU) are fabricated, each with two different sets of dimensions: 150 µm (width) × 1200 µm (length) and 300 µm (width) × 2000 µm (length). Their mechanical and electrical properties are systematically investigated. Atomic Force Microscopy (AFM) analysis revealed that TSU‐PCDm has a higher elastic modulus than BSU‐PCDm, attributed to differences in grain size and defect distribution. Despite these differences, all PCDms in our work exhibit consistently high modulus values with minimal mechanical degradation across various cantilever geometries. Bandgap measurements using X‐ray Photoelectron Spectroscopy (XPS) and UV–vis absorption spectroscopy indicated a lower bandgap for TSU‐PCDm due to boron incorporation, while BSU‐PCDm exhibited a higher bandgap due to increased hydrogen content. Electrical characterization showed that the sheet resistance of TSU‐PCDm decreases under strain, whereas BSU‐PCDm maintains stable resistance. These findings unveil the material properties of PCDm and their potential usage for myriad diamond‐based electronic applications.more » « less
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As the energy demand is expected to double over the next 30 years, there has been a major initiative towards advancing the technology of both energy harvesting and storage for renewable energy. In this work, we explore a subset class of dielectrics for energy storage since ferroelectrics offer a unique combination of characteristics needed for energy storage devices. We investigate ferroelectric lead-free 0.5[Ba(Ti0.8Zr0.2)O3]-0.5(Ba0.7Ca0.3)TiO3 epitaxial thin films with different crystallographic orientations grown by pulsed laser deposition. We focus our attention on the influence of the crystallographic orientation on the microstructure, ferroelectric, and dielectric properties. Our results indicate an enhancement of the polarization and strong anisotropy in the dielectric response for the (001)-oriented film. The enhanced ferroelectric, energy storage, and dielectric properties of the (001)-oriented film is explained by the coexistence of orthorhombic-tetragonal phase, where the disordered local structure is in its free energy minimum.more » « less
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The prototypical chalcogenide perovskite, BaZrS3 (BZS), with its direct bandgap of 1.7–1.8 eV, high chemical stability, and strong light–matter interactions, has garnered significant interest over the past few years. So far, attempts to grow BaZrS3 films have been limited mainly to physical vapor deposition techniques. Here, we report the fabrication of BZS thin films via a facile aqueous solution route of polymer-assisted deposition (PAD), where the polymer-chelated cation precursor films were sulfurized in a mixed CS2 and Ar atmosphere. The formation of a single-phase polycrystalline BZS thin film at a processing temperature of 900 °C was confirmed by X-ray diffraction and Raman spectroscopy. The stoichiometry of the films was verified by Rutherford Backscattering spectrometry and energy-dispersive X-ray spectroscopy. The BZS films showed a photoluminescence peak at around 1.8 eV and exhibited a photogenerated current under light illumination at a wavelength of 530 nm. Temperature-dependent resistivity analysis revealed that the conduction of BaZrS3 films under the dark condition could be described by the Efros–Shklovskii variable range hopping model in the temperature range of 60–300 K, with an activation energy of about 44 meV.more » « less
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Perovskite offers a framework that boasts various functionalities and physical properties of interest such as ferroelectricity, magnetic orderings, multiferroicity, superconductivity, semiconductor, and optoelectronic properties owing to their rich compositional diversity. These properties are also uniquely tied to their crystal distortion which is directly affected by lattice strain. Therefore, many important properties of perovskite can be further tuned through strain engineering which can be accomplished by chemical doping or simply element substitution, interface engineering in epitaxial thin films, and special architectures such as nanocomposites. In this review, we focus on and highlight the structure–property relationships of perovskite metal oxide films and elucidate the principles to manipulate the functionalities through different modalities of strain engineering approaches.more » « less
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Abstract Multiferroic materials have generated great interest due to their potential as functional device materials. Nanocomposites have been increasingly used to design and generate new functionalities by pairing dissimilar ferroic materials, though the combination often introduces new complexity and challenges unforeseeable in single-phase counterparts. The recently developed approaches to fabricate 3D super-nanocomposites (3D‐sNC) open new avenues to control and enhance functional properties. In this work, we developed a new 3D‐sNC with CoFe2O4 (CFO) short nanopillar arrays embedded in BaTiO3 (BTO) film matrix via microstructure engineering by alternatively depositing BTO:CFO vertically-aligned nanocomposite layers and single-phase BTO layers. This microstructure engineering method allows encapsulating the relative conducting CFO phase by the insulating BTO phase, which suppress the leakage current and enhance the polarization. Our results have demonstrated that microstructure engineering in 3D‐sNC offers a new bottom–up method of fabricating advanced nanostructures with a wide range of possible configurations for applications where the functional properties need to be systematically modified.more » « less
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