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1.
Int J Mol Sci ; 24(17)2023 Aug 25.
Artículo en Inglés | MEDLINE | ID: mdl-37686007

RESUMEN

The calcium-binding protein S100A9 is recognized as an important component of the brain neuroinflammatory response to the onset and development of neurodegenerative disease. S100A9 is intrinsically amyloidogenic and in vivo co-aggregates with amyloid-ß peptide and α-synuclein in Alzheimer's and Parkinson's diseases, respectively. It is widely accepted that calcium dyshomeostasis plays an important role in the onset and development of these diseases, and studies have shown that elevated levels of calcium limit the potential for S100A9 to adopt a fibrillar structure. The exact mechanism by which calcium exerts its influence on the aggregation process remains unclear. Here we demonstrate that despite S100A9 exhibiting α-helical secondary structure in the absence of calcium, the protein exhibits significant plasticity with interconversion between different conformational states occurring on the micro- to milli-second timescale. This plasticity allows the population of conformational states that favour the onset of fibril formation. Magic-angle spinning solid-state NMR studies of the resulting S100A9 fibrils reveal that the S100A9 adopts a single structurally well-defined rigid fibrillar core surrounded by a shell of approximately 15-20 mobile residues, a structure that persists even when fibrils are produced in the presence of calcium ions. These studies highlight how the dysregulation of metal ion concentrations can influence the conformational equilibria of this important neuroinflammatory protein to influence the rate and nature of the amyloid deposits formed.


Asunto(s)
Calcio , Enfermedades Neurodegenerativas , Humanos , Amiloide , Resonancia Magnética Nuclear Biomolecular , Calcio de la Dieta , Calgranulina B
2.
Nano Lett ; 18(1): 424-433, 2018 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-29210586

RESUMEN

All-inorganic lead halide perovskite nanowires have been the focus of increasing interest since they exhibit improved stability compared to their hybrid organic-inorganic counterparts, while retaining their interesting optical and optoelectronic properties. Arrays of surface-guided nanowires with controlled orientations and morphology are promising as building blocks for various applications and for systematic research. We report the horizontal and aligned growth of CsPbBr3 nanowires with a uniform crystallographic orientation on flat and faceted sapphire surfaces to form arrays with 6-fold and 2-fold symmetries, respectively, along specific directions of the sapphire substrate. We observed waveguiding behavior and diameter-dependent photoluminescence emission well beyond the quantum confinement regime. The arrays were easily integrated into multiple devices, displaying p-type behavior and photoconductivity. Photodetectors based on those nanowires exhibit the fastest rise and decay times for any CsPbBr3-based photodetectors reported so far. One-dimensional arrays of halide perovskite nanowires are a promising platform for investigating the intriguing properties and potential applications of these unique materials.

3.
ACS Appl Mater Interfaces ; 16(2): 2637-2648, 2024 Jan 17.
Artículo en Inglés | MEDLINE | ID: mdl-38174359

RESUMEN

Infrared photodetectors are essential devices for telecommunication and night vision technologies. Two frequently used materials groups for this technology are III-V and II-VI semiconductors, notably, mercury-cadmium-telluride alloys (MCT). However, growing them usually requires expensive substrates that can only be provided on small scales, and their large-scale production as crystalline nanostructures is challenging. In this paper, we present a two-stage process for creating aligned MCT nanowires (NWs). First, we report the growth of planar CdTe nanowires with controlled orientations on flat and faceted sapphire substrates via the vapor-liquid-solid (VLS) mechanism. We utilize this guided growth approach to parallelly integrate the NWs into fast near-infrared photodetectors with characteristic rise and fall times of ∼100 µs at room temperature. An epitaxial effect of the planar growth and the unique structure of the NWs, including size and composition, are suggested to explain the high performance of the devices. In the second stage, we show that cation exchange with mercury can be applied, resulting in a band gap narrowing of up to 55 meV, corresponding to an exchange of 2% Cd with Hg. This work opens new opportunities for creating small, fast, and sensitive infrared detectors with an engineered band gap operating at room temperature.

4.
ACS Nano ; 16(6): 9086-9094, 2022 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-35584237

RESUMEN

Optoelectronic micro- and nanostructures have a vast parameter space to explore for modification and optimization of their functional performance. This paper reports on a data-led approach using high-throughput single nanostructure spectroscopy to probe >8000 structures, allowing for holistic analysis of multiple material and optoelectronic parameters with statistical confidence. The methodology is applied to surface-guided CsPbBr3 nanowires, which have complex and interrelated geometric, structural, and electronic properties. Photoluminescence-based measurements, studying both the surface and embedded interfaces, exploits the natural inter nanowire geometric variation to show that increasing the nanowire width reduces the optical bandgap, increases the recombination rate in the nanowire bulk, and reduces the rate at the surface interface. A model of carrier recombination and diffusion ascribes these trends to carrier density and strain effects at the interfaces and self-consistently retrieves values for carrier mobility, trap densities, bandgap, diffusion length, and internal quantum efficiency. The model predicts parameter trends, such as the variation of internal quantum efficiency with width, which is confirmed by experimental verification. As this approach requires minimal a priori information, it is widely applicable to nano- and microscale materials.

5.
ACS Nano ; 15(10): 16130-16138, 2021 Oct 26.
Artículo en Inglés | MEDLINE | ID: mdl-34546712

RESUMEN

Metal halide perovskites (MHPs) have unique characteristics and hold great potential for next-generation optoelectronic technologies. Recently, the importance of lattice strain in MHPs has been gaining recognition as a significant optimization parameter for device performance. While the effect of strain on the fundamental properties of MHPs has been at the center of interest, its combined effect with an external electric field has been largely overlooked. Here we perform an electric-field-dependent photoluminescence study on heteroepitaxially strained surface-guided CsPbBr3 nanowires. We reveal an unexpected strong linear dependence of the photoluminescence intensity on the alternating field amplitude, stemming from an induced internal dipole. Using low-frequency polarized-Raman spectroscopy, we reveal structural modifications in the nanowires under an external field, associated with the observed polarity. These results reflect the important interplay between strain and an external field in MHPs and offer opportunities for the design of MHP-based optoelectronic nanodevices.

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