B16-Test Beamline
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Diamond Proposal Number(s):
[28395]
Open Access
Abstract: Carbon fibre composites are widely used in low specific stiffness and high strength structures such as airframes. Compressive loading of these assemblies can lead to buckling and localised deformation around defects and imperfections that can hinder performance and lead to overengineering via excessive safety factors. Synchrotron X-Ray Diffraction (SXRD) has recently been shown to be capable of performing lattice strain mapping within carbon fibre composites at the microscale, a previously unprecedented resolution. In this study SXRD and radiography was performed on carbon fibre composite columns produced via two different methods (standard lamination and half square) at a range of different load states: unbuckled, one-third of the buckling load and post buckling. The results provide quantitative insights into the impact of these different production methods on lattice strain and fibre orientation, as well as the influence these factors have on reducing buckling load (by up to 22%). As well as being the first use of SXRD on industrially representative full-size carbon fibre samples, these insights provide invaluable detail into the factors which limit performance and the origins of column failure; crucial factors required to optimise structural design, production and loading capability.
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Nov 2023
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I24-Microfocus Macromolecular Crystallography
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James
Birch
,
Tristan O. C.
Kwan
,
Peter J.
Judge
,
Danny
Axford
,
Pierre
Aller
,
Agata
Butryn
,
Rosana
Reis
,
Juan F.
Bada Juarez
,
Javier
Vinals
,
Robin L.
Owen
,
Eriko
Nango
,
Rie
Tanaka
,
Kensuke
Tono
,
Yasumasa
Joti
,
Tomoyuki
Tanaka
,
Shigeki
Owada
,
Michihiro
Sugahara
,
So
Iwata
,
Allen M.
Orville
,
Anthony
Watts
,
Isabel
Moraes
Diamond Proposal Number(s):
[19152]
Open Access
Abstract: Serial crystallography has emerged as an important tool for structural studies of integral membrane proteins. The ability to collect data from micrometre-sized weakly diffracting crystals at room temperature with minimal radiation damage has opened many new opportunities in time-resolved studies and drug discovery. However, the production of integral membrane protein microcrystals in lipidic cubic phase at the desired crystal density and quantity is challenging. This paper introduces VIALS (versatile approach to high-density microcrystals in lipidic cubic phase for serial crystallography), a simple, fast and efficient method for preparing hundreds of microlitres of high-density microcrystals suitable for serial X-ray diffraction experiments at both synchrotron and free-electron laser sources. The method is also of great benefit for rational structure-based drug design as it facilitates in situ crystal soaking and rapid determination of many co-crystal structures. Using the VIALS approach, room-temperature structures are reported of (i) the archaerhodopsin-3 protein in its dark-adapted state and 110 ns photocycle intermediate, determined to 2.2 and 1.7 Å, respectively, and (ii) the human A2A adenosine receptor in complex with two different ligands determined to a resolution of 3.5 Å.
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Oct 2023
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DIAD-Dual Imaging and Diffraction Beamline
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Abstract: Purpose / Aim: Dentine hypersensitivity (DH) is a commonly occurring dental condition where sharp pain derived from exposed dentine in response to stimuli that cannot be ascribed to any other dental diseases. It is highly prevalent affecting up to 69% of the UK population and has a significant impact on the quality of life. Bioactive glasses that degrade in oral environment and form apatite are thought to be beneficial in occluding the exposed open dentine tubules and have been introduced to toothpastes, e.g. Novamin® (45S5 Bioglass) for Sensodyne by GSK, fluoride containing bioactive glass for BioMin® F by BioMin Technologies Ltd. Post-mortem characterisations evidenced tubule occlusion (Fig.1) but failed in providing dynamic history. Therefore, this study aimed to monitor dentine tubule occlusion with bioactive glasses using an operando time-lapse X-ray diffraction tomography experiment. Materials & Methods: Disinfected Teeth (collected under REC reference 16/SW/0220) were sectioned mesio-distally into discs approximately 500 μm thick using a precision diamond saw, polished down to 300 μm manually. Matchstick specimens (5 mm length x 3 mm width) prepared were brushed for 2 mins with bioactive glasses pastes, housed in a modified Eppendorf tube and positioned on the tomography stage of the Dual Imaging and Diffraction (DIAD) beamline at Diamond Light Source (UK’s national synchrotron). A baseline X-ray tomography (pink beam, 0-180°, detector exposure of 0.01 and 5,000 projections) and X-ray diffraction mapping (matrix scan with 10x10 points, 20 s exposure) were collected before artificial saliva was introduced. Time-lapse X-ray tomography and X-ray diffraction mapping using the same parameters as baseline scan were carried out consecutively for 8 h allowing the visualisation of tubule occlusion and changes of mineral density as well as monitor the phase evolution from glass to apatite. Artificial saliva was manually replenished. Monochromatic beam with an energy of 20 keV was used and calibrations were performed. Results: The collected tomography data allow visualisation of dentine tubule occlusion showing improved occlusion with time. 2D XRD data provide qualitative and quantitative information relates to glass dissolution and apatite formation as a function of time. Conclusions: The Dual Imaging and Diffraction (DIAD) beamline correlates X-ray tomography and X-ray diffraction mapping offers the opportunity to study dentine occlusion by bioactive glasses in a time evolving manner that is not available via other techniques. Although in vitro but clinically relevant. The results will potentially provide a guidance for optimising and designing products for dentine tubule occlusion/treating dentine hypersensitivity – one of the most prevalent global diseases with healthy ageing.
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Oct 2023
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B18-Core EXAFS
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Diamond Proposal Number(s):
[24523]
Abstract: Aggregation modulates the photochemical and photophysical properties of methylene blue (MB+). MB+ adsorbed by the anionic polymer Chelex® 100 was characterized by UV–visible absorption spectroscopy and sulfur K-edge X-ray absorption near edge structure (XANES) as H- and J-aggregates. Nuclear magnetic resonance (NMR) indicates that dye molecules bind to the unprotonated carboxylic groups of the polymer via electrostatic interactions and are bridged by water molecules. MB+ also stacks with phenyl rings appended in the Chelex® 100 chain, leading to a gain in the mobility of ordered water displaced around the aromatic rings. Like the blue bottle experiment, MB+ in Chelex® 100 was entirely photoconverted for the leuco form (LMB) by visible and red light and reoxidized by molecular oxygen. Electron paramagnetic resonance (EPR) of MB+ in Chelex® 100 demonstrated the formation of a sulfur-centered free radical during photobleaching. The free radical involvement in MB+ photobleaching is consistent with a type I mechanism in which the stabilization of the products MB2+• and MB• in dye aggregates allows the formation of LMB by MB• dismutation or a second electron abstraction. Chelex® 100 beds loaded with MB+ solutions prepared in H2O and D2O produce H2O2 and D2O2, respectively, after successive cycles of photobleaching and recycling by O2 dissolved in the liquid phase. The formation of hydrogen peroxide is attributed to spontaneous superoxide ion disproportionation in the microenvironment of the polymer lattice. The LMB produced in Chelex® 100 was also able to act as a reducing agent for the synthesis of anisotropic iridescent gold nanoparticles (GNPs). The LMB/Chelex system allows the modulation of the shape and size of GNPs using different dye/Au3+ ratios. GNPs produced using LMB as a reducing agent are also efficient cell delivery systems. The specific properties of LMB confined in solid hosts LMB/Chelex also have potential applications in new solid-state optoelectronic devices such as sensing and imaging.
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Oct 2023
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I22-Small angle scattering & Diffraction
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Abstract: In situations where the stereoregularity of the polymer chains permits, crystals can form in synthetic or natural polymers. These crystals have an immense impact on the properties of the polymeric material. Typically polymers crystallized from a quiescent melt form spherulites, but where the melt exhibits a level of anisotropy, the crystalline morphology, is quite different to the spherulitic structure, although it may well contain chain-folded lamellar crystals. We consider a number of different systems in which the anisotropy has developed in different ways. Despite these differences, there are strong features in common within the semi-crystalline polymer morphology. We consider the strain-induced crystallization in deformed natural rubber, in sheared melts containing both self-assembling nanoparticles and engineered nanoparticles, and during extrusion as part of fused granular deposition-based 3D printing.
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Oct 2023
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I05-ARPES
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Kevin P.
Kramer
,
Rina
Tazai
,
Karin
Von Arx
,
Masafumi
Horio
,
Julia
Küspert
,
Qisi
Wang
,
Yasmine
Sassa
,
Timur K.
Kim
,
Cephise
Cacho
,
Julien E.
Rault
,
Patrick
Le Fèvre
,
François
Bertran
,
Marc
Janoschek
,
Nicolas
Gauthier
,
Daniel
Mazzone
,
Ramzy
Daou
,
Johan
Chang
Open Access
Abstract: We present a resonant angle-resolved photoemission spectroscopy (ARPES) study of the electronic band structure and heavy fermion quasiparticles in CeRu2Si2. Using light polarization analysis, considerations of the crystal field environment and hybridization between conduction and f electronic states, we identify the d-electronic orbital character of conduction bands crossing the Fermi level. Resonant ARPES spectra suggest that the localized Ce f states hybridize with eg and t2g states around the zone center. In this fashion, we reveal the orbital structure of the heavy fermion quasiparticles in CeRu2Si2 and discuss its implications for metamagnetism and superconductivity in the related compound CeCu2Si2.
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Oct 2023
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B07-B-Versatile Soft X-ray beamline: High Throughput
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Álvaro
Tolosana-Moranchel
,
Alvaro
Garcia
,
Álvaro
García-Corral
,
José F.
Marco
,
Laura
Pascual
,
Dalia
Liuzzi
,
Mohamed A.
Salam
,
Pilar
Ferrer
,
Jorge
Torrero
,
David C.
Grinter
,
Georg
Held
,
Daniel
García Sánchez
,
K. Andreas
Friedrich
,
Maria
Retuerto
,
Sergio
Rojas
Diamond Proposal Number(s):
[30338]
Open Access
Abstract: The overall performance of proton exchange membrane fuel cells is limited by the sluggish kinetics of the oxygen-reduction reaction (ORR). Among the most active PGM-free ORR electrocatalysts are metal-nitrogen-carbon (M-N-C), such as Fe–N–C. The Fe–N4 ensembles in these PGM-free catalysts, present in different configurations, are proposed to be the active sites for the ORR in acid. In this work, we have synthesized a Fe/N/C catalyst via thermal treatment of a polymeric CxNy precursor obtained by the wet-polymerization of melamine (a nitrogen rich molecule) and terephthaldehyde. The materials obtained (Im-FeNC-1HT and Im-FeNC-2HT) display high ORR activity in acid electrolyte compared to other Fe–N–C catalysts prepared with precursors different than 2-methylimidazole or ZIF-8. Characterization data indicate the formation of high- and low-spin Fe-Nx ensembles, with a site density of 4.4·1019 sitesFe·g−1 estimated by electrochemical stripping of NO. The ORR activity was evaluated in a RRDE configuration in 0.1 M HClO4 and in MEA configuration in a single cell.
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Sep 2023
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I03-Macromolecular Crystallography
I04-Macromolecular Crystallography
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Andrew
Chancellor
,
Robert A.
Simmons
,
Rahul C.
Khanolkar
,
Vladimir
Nosi
,
Aisha
Beshirova
,
Giuliano
Berloffa
,
Rodrigo
Colombo
,
Vijaykumar
Karuppiah
,
Johanne M.
Pentier
,
Vanessa
Tubb
,
Hemza
Ghadbane
,
Richard J.
Suckling
,
Keith
Page
,
Rory M.
Crean
,
Alessandro
Vacchini
,
Corinne
De Gregorio
,
Verena
Schaefer
,
Daniel
Constantin
,
Thomas
Gligoris
,
Angharad
Lloyd
,
Miriam
Hock
,
Velupillai
Srikannathasan
,
Ross A.
Robinson
,
Gurdyal S.
Besra
,
Marc W.
Van Der Kamp
,
Lucia
Mori
,
Raffaele
Calogero
,
David K.
Cole
,
Gennaro
De Libero
,
Marco
Lepore
Diamond Proposal Number(s):
[22870, 28224]
Abstract: Mucosal-associated invariant T (MAIT) cells use canonical semi-invariant T cell receptors (TCR) to recognize microbial riboflavin precursors displayed by the antigen-presenting molecule MR1. The extent of MAIT TCR crossreactivity toward physiological, microbially unrelated antigens remains underexplored. We describe MAIT TCRs endowed with MR1-dependent reactivity to tumor and healthy cells in the absence of microbial metabolites. MAIT cells bearing TCRs crossreactive toward self are rare but commonly found within healthy donors and display T-helper-like functions in vitro. Experiments with MR1-tetramers loaded with distinct ligands revealed significant crossreactivity among MAIT TCRs both ex vivo and upon in vitro expansion. A canonical MAIT TCR was selected on the basis of extremely promiscuous MR1 recognition. Structural and molecular dynamic analyses associated promiscuity to unique TCRβ-chain features that were enriched within self-reactive MAIT cells of healthy individuals. Thus, self-reactive recognition of MR1 represents a functionally relevant indication of MAIT TCR crossreactivity, suggesting a potentially broader role of MAIT cells in immune homeostasis and diseases, beyond microbial immunosurveillance.
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Sep 2023
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I22-Small angle scattering & Diffraction
Detectors
Diagnostics
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Open Access
Abstract: Single-crystal chemical vapour deposition (CVD) diamond detectors are an established transmissive synchrotron beamline diagnostic instrument used for beam position and beam intensity monitoring. A recently commercialized alternative is silicon carbide (4H-SiC) devices. These have the potential to provide the same diagnostic information as commercially available single-crystal CVD diamond X-ray beam position monitors, but with a much larger transmissive aperture. At Diamond Light Source an experimental comparison of the performance of single-crystal CVD diamond and 4H-SiC X-ray beam position monitors has been carried out. A quantitative comparison of their performance is presented in this paper. The single-crystal diamond and 4H-SiC beam position monitors were installed in-line along the synchrotron X-ray beam path enabling synchronous measurements at kilohertz rates of the beam motion from both devices. The results of several tests of the two position monitors' performance are presented: comparing signal uniformity across the surface of the detectors, comparing kHz intensity measurements, and comparing kHz beam position measurements from the detectors. Each test is performed with a range of applied external bias voltages. A discussion of the benefits and limitations of 4H-SiC and single-crystal CVD diamond detectors is included.
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Sep 2023
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I04-Macromolecular Crystallography
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Sibusiso B.
Maseko
,
Yasmine
Brammerloo
,
Inge
Van Molle
,
Adria
Sogues
,
Charlotte
Martin
,
Christoph
Gorgulla
,
Estelle
Plant
,
Julien
Olivet
,
Jeremy
Blavier
,
Thandokuhle
Ntombela
,
Frank
Delvigne
,
Haribabu
Arthanari
,
Hiba
El Hajj
,
Ali
Bazarbachi
,
Carine
Van Lint
,
Kourosh
Salehi-Ashtiani
,
Han
Remaut
,
Steven
Ballet
,
Alexander N.
Volkov
,
Jean-Claude
Twizere
Abstract: Human T-cell leukemia virus type-1 (HTLV-1) is the first pathogenic retrovirus discovered in human. Although HTLV-1-induced diseases are well-characterized and linked to the encoded Tax-1 oncoprotein, there is currently no strategy to target Tax-1 functions with small molecules. Here, we analyzed the binding of Tax-1 to the human homolog of the drosophila discs large tumor suppressor (hDLG1/SAP97), a multi-domain scaffolding protein involved in Tax-1-transformation ability. We have solved the structures of the PDZ binding motif (PBM) of Tax-1 in complex with the PDZ1 and PDZ2 domains of hDLG1 and assessed the binding of 10 million molecules by virtual screening. Among the 19 experimentally confirmed compounds, one systematically inhibited the Tax-1-hDLG1 interaction in different biophysical and cellular assays, as well as HTLV-1 cell-to-cell transmission in a T-cell model. Thus, our work demonstrates that interactions involving Tax-1 PDZ-domains are amenable to small-molecule inhibition, which provides a framework for the design of targeted therapies for HTLV-1-induced diseases.
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Sep 2023
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