I10-Beamline for Advanced Dichroism
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Peng
Chen
,
Qi
Yao
,
Junqi
Xu
,
Qiang
Sun
,
Alexander J.
Grutter
,
Patrick
Quarterman
,
Purnima P.
Balakrishnan
,
Christy J.
Kinane
,
Andrew J.
Caruana
,
Sean
Langridge
,
Ang
Li
,
Barat
Achinuq
,
Emily
Heppell
,
Yuchen
Ji
,
Shanshan
Liu
,
Baoshan
Cui
,
Jiuming
Liu
,
Puyang
Huang
,
Zhongkai
Liu
,
Guoqiang
Yu
,
Faxian
Xiu
,
Thorsten
Hesjedal
,
Jin
Zou
,
Xiaodong
Han
,
Haijun
Zhang
,
Yumeng
Yang
,
Xufeng
Kou
Diamond Proposal Number(s):
[30262]
Abstract: The intrinsic magnetic topological insulator MnBi2Te4 (MBT) provides a platform for the creation of exotic quantum phenomena. Novel properties can be created by modification of the MnBi2Te4 framework, but the design of stable magnetic structures remains challenging. Here we report ferromagnet-intercalated MnBi2Te4 superlattices with tunable magnetic exchange interactions. Using molecular beam epitaxy, we intercalate ferromagnetic MnTe layers into MnBi2Te4 to create [(MBT)(MnTe)m]N superlattices and examine their magnetic interaction properties using polarized neutron reflectometry and magnetoresistance measurements. Incorporation of the ferromagnetic spacer tunes the antiferromagnetic interlayer coupling of the MnBi2Te4 layers through the exchange-spring effect at MnBi2Te4/MnTe hetero-interfaces. The MnTe thickness can be used to modulate the relative strengths of the ferromagnetic and antiferromagnetic order, and the superlattice periodicity can tailor the spin configurations of the synthesized multilayers.
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Dec 2022
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I10-Beamline for Advanced Dichroism
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Diamond Proposal Number(s):
[23784]
Open Access
Abstract: Magnetic skyrmions (skyrmions hereafter) are magnetization configurations, whose topological robustness and nanoscale size have led to speculation that they could find use as a next-generation information carrier. Skyrmions have been observed in magnetic multilayer materials that are thin compared to the radius of a skyrmion, and chiral cubic single crystals that can be far larger than any characteristic skyrmion scale. In these single crystals, one would expect that skyrmions could exhibit interesting three-dimensional (3D) characteristics. Here, the symmetry of the micromagnetic free energy is investigated. This symmetry permits a complex 3D modulation of a skyrmion string, which we show to be a requirement of a skyrmion coexisting with the conical state. We discuss the implications of this modulation with respect to Thiele's equation and interskyrmion interactions. Further to this internal modulation, we study theoretically and show experimentally that the strings themselves must contort towards the surfaces of their confining crystals.
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Dec 2022
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I03-Macromolecular Crystallography
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Diamond Proposal Number(s):
[19915]
Abstract: Usutu virus (USUV), is a mosquito-borne flavivirus currently spreading outside the African continent producing substantial avian mortality. In contrast, infected humans could exhibit mild neurological symptoms or remain asymptomatic. As in other flaviviruses, the capped USUV genome encodes three structural and seven non-structural (NS) proteins. Among the NS proteins, NS5 plays crucial roles in virus replication, harbouring the capping and methyltransferase (MTase) activities in its N-terminal domain and the RNA-dependent RNA polymerase (RdRP) activity at the C-terminus. In this work, we present the first structural and functional characterization of the USUV MTase domain. The first structure of the USUV MTase has been determined in complex with its natural ligands (S-adenosyl-L-methionine [SAM]) and S-adenosyl-L-homocysteine [SAH]) at 2.2 Å resolution, showing a molecular dimer in the crystal asymmetric unit. One molecule is bound to the methyl donor SAM while the second is bound to the reaction by-product SAH. Both molecules are almost identical and also show a high structural similarity to the MTase domains of other flaviviruses. The structure of the USUV MTase bound to the inhibitor sinefungin at 1.8 Å resolution is also described. Careful comparisons of the interactions in the SAM-binding cavity prompt us to hypothesize about the strength and weakness of the structure-based design of antivirals directed to the SAM/SAH binding site that could be effective to deal with this threat.
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Dec 2022
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I10-Beamline for Advanced Dichroism
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Margaret R.
Mccarter
,
Kook Tae
Kim
,
Vladimir A.
Stoica
,
Sujit
Das
,
Christoph
Klewe
,
Elizabeth P.
Donoway
,
David M.
Burn
,
Padraic
Shafer
,
Fanny
Rodolakis
,
Mauro A. p.
Gonçalves
,
Fernando
Gómez-Ortiz
,
Jorge
Íñiguez
,
Pablo
García-Fernández
,
Javier
Junquera
,
Stephen W.
Lovesey
,
Gerrit
Van Der Laan
,
Se Young
Park
,
John W.
Freeland
,
Lane W.
Martin
,
Dong Ryeol
Lee
,
Ramamoorthy
Ramesh
Diamond Proposal Number(s):
[24797]
Abstract: An escalating challenge in condensed-matter research is the characterization of emergent order-parameter nanostructures such as ferroelectric and ferromagnetic skyrmions. Their small length scales coupled with complex, three-dimensional polarization or spin structures makes them demanding to trace out fully. Resonant elastic x-ray scattering (REXS) has emerged as a technique to study chirality in spin textures such as skyrmions and domain walls. It has, however, been used to a considerably lesser extent to study analogous features in ferroelectrics. Here, we present a framework for modeling REXS from an arbitrary arrangement of charge quadrupole moments, which can be applied to nanostructures in materials such as ferroelectrics. With this, we demonstrate how extended reciprocal space scans using REXS with circularly polarized x rays can probe the three-dimensional structure and chirality of polar skyrmions. Measurements, bolstered by quantitative scattering calculations, show that polar skyrmions of mixed chirality coexist, and that REXS allows valuation of relative fractions of right- and left-handed skyrmions. Our quantitative analysis of the structure and chirality of polar skyrmions highlights the capability of REXS for establishing complex topological structures toward future application exploits.
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Dec 2022
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I15-1-X-ray Pair Distribution Function (XPDF)
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Diamond Proposal Number(s):
[18995]
Open Access
Abstract: The formation of stacking faults and phase interstratification disorder in layered nickel(II) hydroxides during the chemical precipitation synthesis of materials using nickel(II) nitrate and potassium hydroxide solutions has been investigated in the temperature range of 5 °C to 95 °C and time intervals from 1 hour to 1 week. Stacking faulted materials were identified by broadening of the 00l reflections, while interstratified materials were identified through the splitting of the 001 into two lines. In contrast to the disorder concepts presented in previous studies of these materials, this work has shown through vibrational spectroscopy that both the alpha-phase and beta-phase hydroxides are present in materials described with stacking fault disorder, while layered hydroxysalts were additionally present in the materials considered to be interstratified. Standard mixtures of Ni3(OH)4(NO3)2 and β-Ni(OH)2 were prepared to investigate if the intensity of particular vibrational bands could be correlated with the proportion of the particular phases in mixtures. The intensities of the C2v nitrate infrared and Raman bands at 990 cm−1 and 1315 cm−1 were shown to correlate with the amount of layered hydroxynitrate incorporated in the phase, theoretically providing a method to determine the components in mixed compositions. Since disorder and phase impurities in layered nickel hydroxide materials affect both their electroactive stability and performance as cathode materials, this work has important implications in several research fields.
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Dec 2022
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B18-Core EXAFS
I20-Scanning-X-ray spectroscopy (XAS/XES)
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Diamond Proposal Number(s):
[20872, 24074, 28515]
Open Access
Abstract: Advanced Cr-doped UO2 fuels are essential for driving safe and efficient generation of nuclear energy. Although widely deployed, little is known about their fundamental chemistry, which is a critical gap for development of new fuel materials and radioactive waste management strategies. Utilising an original approach, we directly evidence the chemistry of Cr(3+)2O3–doped U(4+)O2. Advanced high-flux, high-spectral purity X-ray absorption spectroscopy (XAS), corroborated by diffraction, Raman spectroscopy and high energy resolved fluorescence detection-XAS, is used to establish that Cr2+ directly substitutes for U4+, accompanied by U5+ and oxygen vacancy charge compensation. Extension of the analysis to heat-treated simulant nuclear fuel reveals a mixed Cr2+/3+ oxidation state, with Cr in more than one physical form, explaining the substantial discrepancies that exist in the literature. Successful demonstration of this analytical advance, and the scientific underpinning it provides, opens opportunities for an expansion in the range of dopants utilised in advanced UO2 fuels.
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Dec 2022
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Krios I-Titan Krios I at Diamond
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Matthew C.
Gaines
,
Michail N.
Isupov
,
Shamphavi
Sivabalasarma
,
Risat U. I.
Haque
,
Mathew
Mclaren
,
Clara L.
Mollat
,
Patrick
Tripp
,
Alexander
Neuhaus
,
Vicki A. M.
Gold
,
Sonja-Verena
Albers
,
Bertram
Daum
Open Access
Abstract: Pili are filamentous surface extensions that play roles in bacterial and archaeal cellular processes such as adhesion, biofilm formation, motility, cell-cell communication, DNA uptake and horizontal gene transfer. The model archaeaon Sulfolobus acidocaldarius assembles three filaments of the type-IV pilus superfamily (archaella, archaeal adhesion pili and UV-inducible pili), as well as a so-far uncharacterised fourth filament, named “thread”. Here, we report on the cryo-EM structure of the archaeal thread. The filament is highly glycosylated and consists of subunits of the protein Saci_0406, arranged in a head-to-tail manner. Saci_0406 displays structural similarity, but low sequence homology, to bacterial type-I pilins. Thread subunits are interconnected via donor strand complementation, a feature reminiscent of bacterial chaperone-usher pili. However, despite these similarities in overall architecture, archaeal threads appear to have evolved independently and are likely assembled by a distinct mechanism.
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Dec 2022
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I09-Surface and Interface Structural Analysis
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Leanne A. H.
Jones
,
Zongda
Xing
,
Jack E. N.
Swallow
,
Huw
Shiel
,
Thomas J.
Featherstone
,
Matthew J.
Smiles
,
Nicole
Fleck
,
Pardeep K.
Thakur
,
Tien-Lin
Lee
,
Laurence J.
Hardwick
,
David O.
Scanlon
,
Anna
Regoutz
,
Tim D.
Veal
,
Vinod R.
Dhanak
Diamond Proposal Number(s):
[25980]
Open Access
Abstract: A comprehensive study of bulk molybdenum dichalcogenides is presented with the use of soft and hard X-ray photoelectron (SXPS and HAXPES) spectroscopy combined with hybrid density functional theory (DFT). The main core levels of MoS2, MoSe2, and MoTe2 are explored. Laboratory-based X-ray photoelectron spectroscopy (XPS) is used to determine the ionization potential (IP) values of the MoX2 series as 5.86, 5.40, and 5.00 eV for MoSe2, MoSe2, and MoTe2, respectively, enabling the band alignment of the series to be established. Finally, the valence band measurements are compared with the calculated density of states which shows the role of p-d hybridization in these materials. Down the group, an increase in the p-d hybridization from the sulfide to the telluride is observed, explained by the configuration energy of the chalcogen p orbitals becoming closer to that of the valence Mo 4d orbitals. This pushes the valence band maximum closer to the vacuum level, explaining the decreasing IP down the series. High-resolution SXPS and HAXPES core-level spectra address the shortcomings of the XPS analysis in the literature. Furthermore, the experimentally determined band alignment can be used to inform future device work.
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Dec 2022
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B21-High Throughput SAXS
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Elisabetta
Esposito
,
Laura
Calderan
,
Andrea
Galvan
,
Enrica
Cappellozza
,
Markus
Drechsler
,
Paolo
Mariani
,
Alessia
Pepe
,
Maddalena
Sguizzato
,
Enrico
Vigato
,
Edoardo
Dalla Pozza
,
Manuela
Malatesta
Diamond Proposal Number(s):
[21035]
Open Access
Abstract: In this study, the transdermal fate of vesicular nanosystems was investigated. Particularly, ethosomes based on phosphatidylcholine 0.9% w/w and transethosomes based on phosphatidylcholine 0.9 or 2.7% w/w plus polysorbate 80 0.3% w/w as an edge activator were prepared and characterized. The vesicle mean size, morphology and deformability were influenced by both phosphatidylcholine and polysorbate 80. Indeed, the mean diameters of ethosome were around 200 nm, while transethosome’s mean diameters were 146 or 350 nm in the case of phosphatidylcholine 0.9 or 2.7%, w/w, respectively. The highest deformability was achieved by transethosomes based on phosphatidylcholine 0.9%, w/w. The three types of vesicular nanosystems were applied on explanted human skin maintained in a bioreactor. Transmission electron microscopy demonstrated that all vesicles were able to enter the skin, keeping their structural integrity. Notably, the vesicle penetration capability was influenced by their physical-chemical features. Indeed, ethosomes reached keratinocytes and even the dermis, phosphatidylcholine 0.9% transethosomes were found in keratinocytes and phosphatidylcholine 2.7% transethosomes were found only in corneocytes of the outer layer. These findings open interesting perspectives for a differentiated application of these vesicles for transdermal drug delivery as a function of the cutaneous pathology to be addressed.
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Dec 2022
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I13-2-Diamond Manchester Imaging
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Diamond Proposal Number(s):
[16205]
Open Access
Abstract: Methane (CH4) hydrate dissociation and CH4 release are potential geohazards currently investigated using X-ray computed tomography (XCT). Image segmentation is an important data processing step for this type of research. However, it is often time consuming, computing resource-intensive, operator-dependent, and tailored for each XCT dataset due to differences in greyscale contrast. In this paper, an investigation is carried out using U-Nets, a class of Convolutional Neural Network, to segment synchrotron XCT images of CH4-bearing sand during hydrate formation, and extract porosity and CH4 gas saturation. Three U-Net deployments previously untried for this task are assessed: (1) a bespoke 3D hierarchical method, (2) a 2D multi-label, multi-axis method and (3) RootPainter, a 2D U-Net application with interactive corrections. U-Nets are trained using small, targeted hand-annotated datasets to reduce operator time. It was found that the segmentation accuracy of all three methods surpass mainstream watershed and thresholding techniques. Accuracy slightly reduces in low-contrast data, which affects volume fraction measurements, but errors are small compared with gravimetric methods. Moreover, U-Net models trained on low-contrast images can be used to segment higher-contrast datasets, without further training. This demonstrates model portability, which can expedite the segmentation of large datasets over short timespans.
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Dec 2022
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