I13-2-Diamond Manchester Imaging
I14-Hard X-ray Nanoprobe
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Kamila
Iskhakova
,
Hanna
Cwieka
,
Svenja
Meers
,
Heike
Helmholz
,
Anton
Davydok
,
Malte
Storm
,
Ivo Matteo
Baltruschat
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Silvia
Galli
,
Daniel
Pröfrock
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Olga
Will
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Mirko
Gerle
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Timo
Damm
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Sandra
Sefa
,
Weilue
He
,
Keith
Macrenaris
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Malte
Soujon
,
Felix
Beckmann
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Julian
Moosmann
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Thomas
O'Hallaran
,
Roger J.
Guillory
,
D. C. Florian
Wieland
,
Berit
Zeller-Plumhoff
,
Regine
Willumeit-Römer
Diamond Proposal Number(s):
[25078]
Open Access
Abstract: Magnesium (Mg) – based alloys are becoming attractive materials for medical applications as temporary bone implants for support of fracture healing, e.g. as a suture anchor. Due to their mechanical properties and biocompatibility, they may replace titanium or stainless-steel implants, commonly used in orthopedic field. Nevertheless, patient safety has to be assured by finding a long-term balance between metal degradation, osseointegration, bone ultrastructure adaptation and element distribution in organs. In order to determine the implant behavior and its influence on bone and tissues, we investigated two Mg alloys with gadolinium contents of 5 and 10 wt percent in comparison to permanent materials titanium and polyether ether ketone. The implants were present in rat tibia for 10, 20 and 32 weeks before sacrifice of the animal. Synchrotron radiation-based micro computed tomography enables the distinction of features like residual metal, degradation layer and bone structure. Additionally, X-ray diffraction and X-ray fluorescence yield information on parameters describing the bone ultrastructure and elemental composition at the bone-to-implant interface. Finally, with element specific mass spectrometry, the elements and their accumulation in the main organs and tissues are traced. The results show that Mg-xGd implants degrade in vivo under the formation of a stable degradation layer with bone remodeling similar to that of Ti after 10 weeks. No accumulation of Mg and Gd was observed in selected organs, except for the interfacial bone after 8 months of healing. Thus, we confirm that Mg-5Gd and Mg-10Gd are suitable material choices for bone implants.
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Nov 2024
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[33049]
Open Access
Abstract: Increasing municipal solid waste (MSW) production poses challenges for sustainable urban development. Modern energy-from-waste (EfW) facilities incinerate MSW, reducing mass and recovering energy. In the UK, MSW incineration bottom ash (MSW IBA) is primarily reused in civil engineering applications. This study characterizes UK-produced MSW IBA, examining its pH-dependent leaching behaviour and response to environmental lixiviants. Results show predominant components include a melt phase, primary glass and fine ash aggregations, and a chemical composition dominated by SiO2 (30–50 %), CaO (∼15 %), Fe2O3 (∼10 %), and Al2O3 (∼8%). X-ray absorption near edge structure (XANES) analysis shows that Zn and Cu are most likely oxygen-bound (adsorbed to oxy-hydroxides and as oxides) with some sulphur bound. Polychlorinated biphenyls (PCBs) and polychlorinated dibenzodioxins/furans (PCDD/Fs) are well below regulatory limits, and polycyclic aromatic hydrocarbons (PAHs) were undetectable. Leaching tests indicate trace elements mobilize at pHs ≤ 6. With a natural pH of 11.3 and high buffering capacity, significant acid inputs to the MSW IBA are required to reach this pH, which are improbable in the environment. Wood chip additions increase leachate’s dissolved organic carbon (DOC) and reduce pH, but had minimal impact on metal-leaching behaviour. Synthetic plant exudate solutions minimally affect metal leaching at realistic concentrations, only enhancing leaching at ≥ 1500 mg l−1 DOC. This work supports MSW IBA’s low-risk in specified civil engineering applications.
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Oct 2024
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[33825]
Abstract: Septins are cytoskeletal proteins and their interaction with membranes is crucial for their role in various cellular processes. Septins have polybasic regions (PB1 and PB2) which are important for lipid interaction. Earlier, we and others have highlighted the role of the septin C-terminal domain (CTD) to membrane interaction. However, detailed information on residues/group of residues important for such feature is lacking. In this study, we investigate the lipid-binding profile of Schistosoma mansoni Septin10 (SmSEPT10) using PIP strip and Langmuir monolayer adsorption assays. Our findings highlight the CTD as the primary domain responsible for lipid interaction in SmSEPT10, showing binding to phosphatidylinositol phosphates. SmSEPT10 CTD contains a conserved polybasic region (PB3) present in both animals and fungi septins, and a Lys (K367) within its putative amphipathic helix (AH) that we demonstrate as important for lipid binding. PB3 deletion or mutation of this Lys (K367A) strongly impairs lipid interaction. Remarkably, we observe that the AH within a construct lacking the final 43 amino acid residues is insufficient for lipid binding. Furthermore, we investigate the homocomplex formed by SmSEPT10 CTD in solution by cross-linking experiments, CD spectroscopy, SEC-MALS and SEC-SAXS. Taken together, our studies define the lipid-binding region in SmSEPT10 and offer insights into the molecular basis of septin-membrane binding. This information is particularly relevant for less-studied non-human septins, such as SmSEPT10.
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Oct 2024
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Open Access
Abstract: Short range order of a ternary Mg82Ca8Au10 biodegradable amorphous alloy was studied by combining diffraction datasets and Au L3 edge EXAFS data by the Reverse Monte Carlo simulation technique. It was found that while the Mg–Mg bond length agrees well with the empirical atomic diameter of Mg, both the Mg–Ca and Mg–Au mean interatomic distances are ∼9 % shorter than the sum of the corresponding atomic radii. The Ca–Au bond length exhibits ∼14 % shortening. The linear expansion coefficients of the glass determined from the temperature induced shift of the first peak of the structure factor and the reduced pair distribution function are ∼3.7 × 10−5 K−1 and ∼3.1 × 10−5 K−1, respectively. During devitrification, two crystalline phases emerge from the amorphous alloy: hexagonal AuMg3 and the solid solution of Ca in hexagonal close packed Mg. The thermal expansion behaviour of the AuMg3 unit cell was also determined using diffraction data.
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Oct 2024
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Mingyuan
Ye
,
Ziqi
Zhao
,
Liying
Liu
,
Li
Shao
,
Li
Liu
,
Xiaorui
Hao
,
Jiaqi
Lv
,
Peng-Fei
Wang
,
Yu-Han
Zhang
,
Fa-Nian
Shi
,
Yuhan
Wu
Abstract: In this work, Cu1.04Mn0.96O2 nanosheets were synthesized via a simple hydrothermal method, and their electrochemical lithium storage properties and reaction mechanisms were investigated. The nanosheet structure effectively promotes electron transfer and shortens the transport path. Additionally, the partial substitution of Cu for Mn decreases the Jahn-Teller distortion of the MnO6 octahedron. Employing as an anode for Li-ion batteries, the specific capacity reached 610.91 mAh g−1 after 100 cycles at a current density of 100 mA g−1.
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Oct 2024
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Open Access
Abstract: Over the last three decades, the technology that makes it possible to follow chemical processes in the solid state in real time has grown enormously. These studies have important implications for the design of new functional materials for applications in optoelectronics and sensors. Light–matter interactions are of particular importance, and photocrystallography has proved to be an important tool for studying these interactions. In this technique, the three-dimensional structures of light-activated molecules, in their excited states, are determined using single-crystal X-ray crystallography. With advances in the design of high-power lasers, pulsed LEDs and time-gated X-ray detectors, the increased availability of synchrotron facilities, and most recently, the development of XFELs, it is now possible to determine the structures of molecules with lifetimes ranging from minutes down to picoseconds, within a single crystal, using the photocrystallographic technique. This review discusses the procedures for conducting successful photocrystallographic studies and outlines the different methodologies that have been developed to study structures with specific lifetime ranges. The complexity of the methods required increases considerably as the lifetime of the excited state shortens. The discussion is supported by examples of successful photocrystallographic studies across a range of timescales and emphasises the importance of the use of complementary analytical techniques in order to understand the solid-state processes fully.
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Oct 2024
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I06-Nanoscience (XPEEM)
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Raul
Lopez-Martin
,
Chris
Binns
,
Benito
Santos Burgos
,
Peter S.
Normile
,
Jose A.
De Toro
,
Andrew
Pratt
,
Toby
Bird
,
Maha
Alotaibi
,
Jack
Pearce
,
David
Hesp
,
Connor
Fields
,
Shengfu
Yang
,
Hanqing
Liu
,
Larissa S. I.
Veiga
,
Sarnjeet S.
Dhesi
Diamond Proposal Number(s):
[33064]
Open Access
Abstract: Nanostructured FeCo films comprising small (2.1 nm mean diameter) Co nanoparticles deposited into an Fe matrix are investigated by magnetometry, transmission electron microscopy and X-ray Magnetic Circular Dichroism (XMCD). Similar films were previously reported to possess a saturation magnetisation of up to 3 µB/atom, thus exceeding the Slater-Pauling limit by a significant margin. The present work confirms the previous findings by magnetometry and demonstrates that the Co nanoparticles maintain their particulate identity within the film while adopting the crystallographic structure of the Fe matrix. The films show no evidence for voids or porosity (they exhibit the bulk density). An important factor in the high magnetisation in the films is an enhanced magnetic moment on the Co atoms, which XMCD indicates to be at least 2.21 µB, i.e., 30 % larger than the bulk value for metallic cobalt.
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Oct 2024
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Open Access
Abstract: Accurate analysis of the rich information contained within X-ray spectra usually calls for detailed electronic structure theory simulations. However, density functional theory (DFT), time-dependent DFT and many-body perturbation theory calculations increasingly require the use of advanced codes running on high-performance computing (HPC) facilities. Consequently, many researchers who would like to augment their experimental work with such simulations are hampered by the compounding of nontrivial knowledge requirements, specialist training and significant time investment. To this end, we present Web-CONEXS, an intuitive graphical web application for democratizing electronic structure theory simulations. Web-CONEXS generates and submits simulation workflows for theoretical X-ray absorption and X-ray emission spectroscopy to a remote computing cluster. In the present form, Web-CONEXS interfaces with three software packages: ORCA, FDMNES and Quantum ESPRESSO, and an extensive materials database courtesy of the Materials Project API. These software packages have been selected to model diverse materials and properties. Web-CONEXS has been conceived with the novice user in mind; job submission is limited to a subset of simulation parameters. This ensures that much of the simulation complexity is lifted and preliminary theoretical results are generated faster. Web-CONEXS can be leveraged to support beam time proposals and serve as a platform for preliminary analysis of experimental data.
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Sep 2024
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DIAD-Dual Imaging and Diffraction Beamline
I11-High Resolution Powder Diffraction
I12-JEEP: Joint Engineering, Environmental and Processing
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Open Access
Abstract: The plumes of Enceladus contain a non-ice component that originates from aqueous processes occurring within the interior 1,2. The ocean of Enceladus is thought to be connected to the surface across a range of time scales. These processes range from the rapid eruption of cryovolcanic plumes to slow crustal convection on geological timescales3,4. In every case, the system will have a temperature and geochemical evolution as it freezes, with the history of evolution recorded in the sequence of mineral precipitation. Analogously to igneous and metamorphic petrology, we can explore the mineralogy and its context to reconstruct the history of that sample. Most importantly, for astrobiological investigations, the formation and cryo-petrological study of inorganic salts can be used to identify sites of recent exposure on the surface.
Synchrotron X-ray techniques allow fast, high-resolution probing of these systems with X-ray light. By exploring large, multi-component samples with multiple techniques, with variable temperature over time we can reveal many emergent processes that may not be predictable with simple phase diagrams.
We use a combination of synchrotron powder X-ray diffraction (PXRD) and X-ray microtomography (µCT) across multiple beamlines at Diamond Light Source (I11, I12 and DIAD). Using a multi-modal approach, we present an in-situ study of the low-temperature phase behaviour of Na-Cl-HCO3 fluids. We employ K11-DIAD (Dual Imaging and Diffraction) to carry out ‘image-guided diffraction’ on an Enceladus-type sample frozen in real-time. DIAD’s unique capabilities allow us not only to study microstructure down to 1 µm but also to carry out spatially resolved XRD and identify solid phases present.
We present, for the first time, the use of dual imaging and diffraction of a Na-Cl-CO₃ solution frozen in real time in 3 dimensions [Figure 1]. DIAD’s imaged guided diffraction provides spatially-resolved XRD, allowing us to probe different regions of our sample and identify the formation of Na2CO₃ hydrates. We show the influence of carbonate chemistry on the sequence of cryogenic precipitation and the development of complex microstructures. These results provide insights into crustal transport processes and will help with interpreting observational data from upcoming Galilean missions.
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Sep 2024
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I13-2-Diamond Manchester Imaging
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Carlos
Navarrete-Leon
,
P. Stephen
Patrick
,
Adam
Doherty
,
Harry
Allan
,
Silvia
Cipiccia
,
Shashidhara
Marathe
,
Kaz
Wanelik
,
Michela
Esposito
,
Charlotte K.
Hagen
,
Alessandro
Olivo
,
Marco
Endrizzi
Diamond Proposal Number(s):
[30748]
Open Access
Abstract: Two-directional beam-tracking (2DBT) is a method for phase-contrast imaging and tomography that uses an intensity modulator to structure the X-ray beam into an array of independent circular beamlets that are resolved by a high-resolution detector. It features isotropic spatial resolution, provides two-dimensional phase sensitivity, and enables the three-dimensional reconstructions of the refractive index decrement, δ, and the attenuation coefficient, μ. In this work, the angular sensitivity and the spatial resolution of 2DBT images in a synchrotron-based implementation is reported. In its best configuration, angular sensitivities of ∼20 nrad and spatial resolution of at least 6.25 µm in phase-contrast images were obtained. Exemplar application to the three-dimensional imaging of soft tissue samples, including a mouse liver and a decellularized porcine dermis, is also demonstrated.
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Sep 2024
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