I14-Hard X-ray Nanoprobe
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Ian
Byrnes
,
Lisa Magdalena
Rossbach
,
Jakub
Jaroszewicz
,
Daniel
Grolimund
,
Dario
Ferreira Sanchez
,
Miguel A.
Gomez-Gonzalez
,
Gert
Nuyts
,
Estela
Reinoso-Maset
,
Koen
Janssens
,
Brit
Salbu
,
Dag Anders
Brede
,
Ole Christian
Lind
Diamond Proposal Number(s):
[27615]
Open Access
Abstract: Micro- and nanoscopic X-ray techniques were used to investigate the relationship between uranium (U) tissue distributions and adverse effects to the digestive tract of aquatic model organism Daphnia magna following uranium nanoparticle (UNP) exposure. X-ray absorption computed tomography measurements of intact daphnids exposed to sublethal concentrations of UNPs or a U reference solution (URef) showed adverse morphological changes to the midgut and the hepatic ceca. Histological analyses of exposed organisms revealed a high proportion of abnormal and irregularly shaped intestinal epithelial cells. Disruption of the hepatic ceca and midgut epithelial tissues implied digestive functions and intestinal barriers were compromised. Synchrotron-based micro X-ray fluorescence (XRF) elemental mapping identified U co-localized with morphological changes, with substantial accumulation of U in the lumen as well as in the epithelial tissues. Utilizing high-resolution nano-XRF, 400–1000 nm sized U particulates could be identified throughout the midgut and within hepatic ceca cells, coinciding with tissue damages. The results highlight disruption of intestinal function as an important mode of action of acute U toxicity in D. magna and that midgut epithelial cells as well as the hepatic ceca are key target organs.
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Jan 2023
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I14-Hard X-ray Nanoprobe
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Takaaki
Noguchi
,
Toru
Matsumoto
,
Akira
Miyake
,
Yohei
Igami
,
Mitsutaka
Haruta
,
Hikaru
Saito
,
Satoshi
Hata
,
Yusuke
Seto
,
Masaaki
Miyahara
,
Naotaka
Tomioka
,
Hope A.
Ishii
,
John P.
Bradley
,
Kenta K.
Ohtaki
,
Elena
Dobrică
,
Hugues
Leroux
,
Corentin
Le Guillou
,
Damien
Jacob
,
Francisco
De La Peña
,
Sylvain
Laforet
,
Maya
Marinova
,
Falko
Langenhorst
,
Dennis
Harries
,
Pierre
Beck
,
Thi H. V.
Phan
,
Rolando
Rebois
,
Neyda M.
Abreu
,
Jennifer
Gray
,
Thomas
Zega
,
Pierre-M.
Zanetta
,
Michelle S.
Thompson
,
Rhonda
Stroud
,
Kate
Burgess
,
Brittany A.
Cymes
,
John C.
Bridges
,
Leon
Hicks
,
Martin R.
Lee
,
Luke
Daly
,
Phil A.
Bland
,
Michael E.
Zolensky
,
David R.
Frank
,
James
Martinez
,
Akira
Tsuchiyama
,
Masahiro
Yasutake
,
Junya
Matsuno
,
Shota
Okumura
,
Itaru
Mitsukawa
,
Kentaro
Uesugi
,
Masayuki
Uesugi
,
Akihisa
Takeuchi
,
Mingqi
Sun
,
Satomi
Enju
,
Aki
Takigawa
,
Tatsuhiro
Michikami
,
Tomoki
Nakamura
,
Megumi
Matsumoto
,
Yusuke
Nakauchi
,
Masanao
Abe
,
Masahiko
Arakawa
,
Atsushi
Fujii
,
Masahiko
Hayakawa
,
Naru
Hirata
,
Naoyuki
Hirata
,
Rie
Honda
,
Chikatoshi
Honda
,
Satoshi
Hosoda
,
Yu-Ichi
Iijima
,
Hitoshi
Ikeda
,
Masateru
Ishiguro
,
Yoshiaki
Ishihara
,
Takahiro
Iwata
,
Kousuke
Kawahara
,
Shota
Kikuchi
,
Kohei
Kitazato
,
Koji
Matsumoto
,
Moe
Matsuoka
,
Yuya
Mimasu
,
Akira
Miura
,
Tomokatsu
Morota
,
Satoru
Nakazawa
,
Noriyuki
Namiki
,
Hirotomo
Noda
,
Rina
Noguchi
,
Naoko
Ogawa
,
Kazunori
Ogawa
,
Tatsuaki
Okada
,
Chisato
Okamoto
,
Go
Ono
,
Masanobu
Ozaki
,
Takanao
Saiki
,
Naoya
Sakatani
,
Hirotaka
Sawada
,
Hiroki
Senshu
,
Yuri
Shimaki
,
Kei
Shirai
,
Seiji
Sugita
,
Yuto
Takei
,
Hiroshi
Takeuchi
,
Satoshi
Tanaka
,
Eri
Tatsumi
,
Fuyuto
Terui
,
Ryudo
Tsukizaki
,
Koji
Wada
,
Manabu
Yamada
,
Tetsuya
Yamada
,
Yukio
Yamamoto
,
Hajime
Yano
,
Yasuhiro
Yokota
,
Keisuke
Yoshihara
,
Makoto
Yoshikawa
,
Kent
Yoshikawa
,
Ryohta
Fukai
,
Shizuho
Furuya
,
Kentaro
Hatakeda
,
Tasuku
Hayashi
,
Yuya
Hitomi
,
Kazuya
Kumagai
,
Akiko
Miyazaki
,
Aiko
Nakato
,
Masahiro
Nishimura
,
Hiromichi
Soejima
,
Ayako I.
Suzuki
,
Tomohiro
Usui
,
Toru
Yada
,
Daiki
Yamamoto
,
Kasumi
Yogata
,
Miwa
Yoshitake
,
Harold C.
Connolly
,
Dante S.
Lauretta
,
Hisayoshi
Yurimoto
,
Kazuhide
Nagashima
,
Noriyuki
Kawasaki
,
Naoya
Sakamoto
,
Ryuji
Okazaki
,
Hikaru
Yabuta
,
Hiroshi
Naraoka
,
Kanako
Sakamoto
,
Shogo
Tachibana
,
Sei-Ichiro
Watanabe
,
Yuichi
Tsuda
Open Access
Abstract: Without a protective atmosphere, space-exposed surfaces of airless Solar System bodies gradually experience an alteration in composition, structure and optical properties through a collective process called space weathering. The return of samples from near-Earth asteroid (162173) Ryugu by Hayabusa2 provides the first opportunity for laboratory study of space-weathering signatures on the most abundant type of inner solar system body: a C-type asteroid, composed of materials largely unchanged since the formation of the Solar System. Weathered Ryugu grains show areas of surface amorphization and partial melting of phyllosilicates, in which reduction from Fe3+ to Fe2+ and dehydration developed. Space weathering probably contributed to dehydration by dehydroxylation of Ryugu surface phyllosilicates that had already lost interlayer water molecules and to weakening of the 2.7 µm hydroxyl (–OH) band in reflectance spectra. For C-type asteroids in general, this indicates that a weak 2.7 µm band can signify space-weathering-induced surface dehydration, rather than bulk volatile loss.
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Dec 2022
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I14-Hard X-ray Nanoprobe
I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[12477, 29965]
Open Access
Abstract: Synchrotron radiation (SR) techniques, which use high-energy photon beams to create high-resolution images and spectra of a sample, are valuable analytical methods that have long benefited physical, geological, and biochemical research. Recent developments in synchrotron infrastructure have allowed SR techniques to become a more accessible resource for studying ecological and evolutionary phenomena at the micro- or nanoscale. Here we provide a synthesis to SR techniques, how they compare with other analytical techniques, how they have been used, and then discuss how this technology has significant potential for future applications within ecology and evolution research. A literature review demonstrates the growing use of SR techniques within environmental and ecological research communities, alongside the variety of organisms and target elements that have been prioritized since 2000. Clear gaps still exist within the imaging of lighter, biologically relevant elements (e.g., C, N, and P) for assessing their cycling within organisms, and also in the study of a wider range of microbial, vertebrate, and invertebrate species. While different organism types and target elements may require different sample preparation strategies, the selection of an appropriate elemental fixation method (chemical or cryogenic), embedding material, sample thickness, and mounting material is particularly important. We demonstrate the opportunities that SR techniques present to those in the fields of environmental biology, ecology, and evolutionary science who may be unfamiliar, while demystifying the caveats and sample preparation considerations that must be addressed to acquire high-quality data. While these techniques are currently mainly employed within the context of environmental pollution and ecotoxicology studies, we argue that elemental imaging, X-ray microscopy and spectroscopic analysis have a huge, largely untapped potential within agri-ecology, paleoclimatology, and comparative and functional morphology studies.
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Dec 2022
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[23705]
Abstract: Background: Contrast agents (CA) are administered in magnetic resonance imaging (MRI) clinical exams to measure tissue perfusion, enhance image contrast between adjacent tissues, or provide additional biochemical information in molecular MRI. The efficacy of a CA is determined by the tissue distribution of the agent and its concentration in the extracellular space of all tissues. Methods: In this work, micro-synchrotron radiation x-ray fluorescence (µ-SRXRF) was used to examine and characterize a gadolinium-based zinc-sensitive agent (GdL2) currently under development for detection of prostate cancer (PCa) by MRI. Prostate tissue samples were collected from control mice and mice with known PCa after an MRI exam that included injection of GdL2. The samples were raster scanned to investigate trends in Zn, Gd, Cu, Fe, S, P, and Ca. Results: Significant Zn and Gd co-localization was observed in both healthy and malignant tissues. In addition, a marked decrease in Zn was found in the lateral lobe of the prostate obtained from mice with PCa. Conclusion: We demonstrate here that µ-SRXRF is a useful tool for monitoring the distribution of several elements including Zn and Gd in animal models of cancer. The optimized procedures for tissue preparation, processing, data collection, and analysis are described.
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Dec 2022
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I18-Microfocus Spectroscopy
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Abstract: In this work, x-ray and optical techniques were utilized to analyze tissue for two main applications in cancer: intraoperative breast cancer margin assessment and contrast agent development for prostate cancer magnetic resonance imaging (MRI). A clinically compatible combined time-resolved fluorescence and diffuse reflectance (TRF-DR) spectroscopy system was used to measure breast tissue from 80 patients with invasive ductal carcinoma (IDC). A procedure was developed to compare extracted optical parameters with histological analysis. Trends in optical parameters between breast tumor, adipose, and fibroglandular tissue were investigated. Optical parameters that showed statistically significant differences between tissue groups were used in multivariate analysis and tissue modelling. Tissue classification using the combined system resulted in tumor detection sensitivity and specificity of 83.9% and 96.2%, respectively. Further work studying more fibroglandular tissue and tissue of mixed composition would develop this system for intraoperative use for tumor margin detection. In addition, micro-synchrotron radiation x-ray fluorescence (μ-SRXRF) was used to determine the efficacy of a novel gadolinium-based contrast agent for zinc-targeting in prostate cancer imaging. Trends in elements of interest such as Gd, Zn, Fe, Cu, and S between mice with prostate cancer, castrate-resistant prostate cancer, and normal mice were observed. Raster scans were collected of large regions of the prostate as well as within the lateral lobe specifically. Significant Zn and Gd co-localization was observed in both healthy and malignant tissues. Also, a marked decrease in Zn was found in the lateral lobe of the prostate obtained from mice with prostate cancer. The sample preparation and processing procedure outlined in this work provide a feasible and effective method of assessing the efficacy of MRI contrast agents in vivo. With the ability to use a beam as small as 5μm × 5μm, this optimized technique also lends itself to the investigation of other elements and contrast agents in biological tissue.
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Dec 2022
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I14-Hard X-ray Nanoprobe
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Abstract: Biomineralization relies on the regulation of localized environments to control how minerals are formed. Through the use of confinement and specific additives, the organism is able to change the energy landscape of nucleation and growth to build single crystals with unusual morphologies. In order to better understand the environments in which biomineralization occurs, it is important to understand both the effects of specific factors on crystallization and how those factors may show up in the final mineralized tissue. Biominerals formed in intracellular vesicles have the highest level of organism-directed regulation and 2 of these types of systems are explored in this work: calcium carbonate, with which sea urchins build their skeletal components, and strontium sulfate, a rare biomineral found in the endoskeletons of marine plankton called Acantharia. In the first part of this work, the role of confinement on the crystallization is explored in the calcium carbonate system. A microfluidic assay was used to measure volume scaling of the crystallization rate in droplets filled with supersaturated calcium carbonate solution. This volume scaling predicts that on the size scale of intracellular vesicles, calcium carbonate crystallization is exceeding slow, with a 1% probability of crystallization after ~1 million years. This suggests an accelerant must be present during sea urchin embryo spiculogenesis to build their calcite skeletal components. An extension of this work to the system of barium calcium carbonate is made in the second chapter of this thesis where model selection is combined with survival analysis to make inferences in a system with a time-dependent crystallization rate. In the next section of this work, characterization of the mineralized tissue is performed in sea urchin and Acantharia spicules. In sea urchin spicule cross section, nanoscale X-ray diffraction mapping is used to measure distortions in the lattice at high resolution and sensitivity in 2 species of sea urchins which produce different types of spicules. The measured changes in d-spacing correlate with low-Z inclusions previously observed in TEM and the change in d-spacing could not be explained by fluctuations in magnesium content alone. In Acantharia, for which relatively little is known compared to sea urchins, both composition and d-spacing were characterized. X-ray fluorescence (XRF) mapping revealed compositional gradients in trace elements barium, calcium and potassium in spicule cross sections, which diffract as single crystals. D-spacing maps show features similar to those in XRF maps and TEM images. A more detailed look at composition was performed with atom probe tomography (APT) which showed even higher concentrations of sodium (on the order of 1 at%) as compared to the other trace elements. Clustering of sodium, water, and some ambiguous ion species were also observed in APT tips and implications for whether organic inclusions are present in these spicules is discussed. Biological compartments in which mineralized tissues are formed are key components to understanding crystallization pathways in biominerals and can leave traces of themselves within the mineral itself. Through the study of crystallization in confinement and characterization of features within these single crystals a clearer picture of these environments can be formed. This can provide inspiration for fabricating better and more sustainable materials as well as expand our knowledge about complex crystallization processes.
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Dec 2022
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I14-Hard X-ray Nanoprobe
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Mandar
Bandekar
,
Fazel
Abdolahpur Monikh
,
Jukka
Kekäläinen
,
Teemu
Tahvanainen
,
Raine
Kortet
,
Peng
Zhang
,
Zhiling
Guo
,
Jarkko
Akkanen
,
Jari T. T.
Leskinen
,
Miguel A.
Gomez-Gonzalez
,
Gopala
Krishna Darbha
,
Hans-Peter
Grossart
,
Eugenia
Valsami-Jones
,
Jussi V. K.
Kukkonen
Diamond Proposal Number(s):
[30433]
Open Access
Abstract: The smallest fraction of plastic pollution, submicron plastics (SMPs <1 μm) are expected to be ubiquitous in the environment. No information is available about SMPs in peatlands, which have a key role in sequestering carbon in terrestrial ecosystems. It is unknown how these plastic particles might behave and interact with (micro)organisms in these ecosystems. Here, we show that the chemical composition of polystyrene (PS) and poly(vinyl chloride) (PVC)-SMPs influenced their adsorption to peat. Consequently, this influenced the accumualtion of SMPs by Sphagnum moss and the composition and diversity of the microbial communities in peatland. Natural organic matter (NOM), which adsorbs from the surrounding water to the surface of SMPs, decreased the adsorption of the particles to peat and their accumulation by Sphagnum moss. However, the presence of NOM on SMPs significantly altered the bacterial community structure compared to SMPs without NOM. Our findings show that peatland ecosystems can potentially adsorb plastic particles. This can not only impact mosses themselves but also change the local microbial communities.
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Nov 2022
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I08-Scanning X-ray Microscopy beamline (SXM)
I14-Hard X-ray Nanoprobe
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Cyril
Besnard
,
Ali
Marie
,
Sisini
Sasidharan
,
Petr
Buček
,
Jessica
Walker
,
Julia E.
Parker
,
Thomas E. J.
Moxham
,
Benedikt
Daurer
,
Burkhard
Kaulich
,
Majid
Kazemian
,
Richard M.
Shelton
,
Gabriel
Landini
,
Alexander M.
Korsunsky
Diamond Proposal Number(s):
[30684, 31005]
Open Access
Abstract: This study reports the characterisation of human dental enamel caries using synchrotron nanoscale correlative ptychography and spectroscopic mapping in combination with scanning electron microscopy. A lamella ̴2.4 µm thick was extracted from a carious enamel region of a tooth using focused ion beam-scanning electron microscopy and transferred to two synchrotron beamlines to perform hard X-ray nano-fluorescence spectroscopy simultaneously with differential phase contrast mapping at a beam size of 50 nm. Soft X-ray ptychography data was then reconstructed with a pixel size of 8 nm. The two dimensional variation in chemistry and structure of carious enamel was revealed at the nanoscale, namely, the organisation of hydroxyapatite nano-crystals within enamel rods was imaged together with the inter-rod region. Correlative use of electron and X-ray scanning microscopies for the same sample allowed visualisation of the connection between structure and composition as presented in a compound image where colour indicates the relative calcium concentration in the sample, as indicated by the calcium Kα fluorescence intensity and grey scale shows the nanostructure. This highlights the importance of advanced correlative imaging to investigate the complex structure-composition relationships in nanomaterials of natural or artificial origin.
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Oct 2022
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[25932]
Open Access
Abstract: The doping of functionalized graphene oxide (GO) in the membranes becomes a promising method for improving the performance of high-temperature proton exchange membrane fuel cells (HT-PEMFC). Phosphonated graphene oxide (PGO) with a P/O ratio of 8.5% was quickly synthesised by one-step electrochemical exfoliation based on a 3D printed reactor and natural graphite flakes. Compared with the GO prepared by the two-step electrochemical exfoliation method, the PGO synthesized by the one-step electrochemical exfoliation can better improve the performance of the membrane-electrode-assembly (MEA) based on the Polybenzimidazole (PBI) membrane in the HT-PEMFC. The doping of 1.5 wt% GO synthesised by electrochemical exfoliation with the 2-step method or reactor method in PBI increased the peak power density by 17.4% or 35.4% compared to MEA based on pure PBI membrane at 150 ℃, respectively. In addition, the doping of PGO in PBI improves its durability under accelerated stress test (AST).
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Sep 2022
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[28279]
Abstract: Parkinson’s disease (PD) is pathologically characterized by intracellular α-synuclein-rich protein aggregates, named Lewy bodies (LB), and by the progressive loss of dopaminergic neurons in the substantia nigra. Several heavy metals, including zinc (Zn), have been suggested to play a role in PD progression, although the exact role of Zn in neurodegeneration remains to be fully elucidated. To address this gap, we investigated the effects of Zn modulation on the progression of degeneration in mice injected with PD patient-derived LB-extracts carrying toxic α-synuclein aggregates. Zn modulation was achieved using either a clioquinol-enriched diet, a Zn ionophore that redistributes cellular Zn, or a Zn-enriched diet that increases Zn levels. Clioquinol treatment significantly prevented dopaminergic neurodegeneration and reduced α-synuclein-associated pathology in LB-injected mice, while no differences were observed with Zn supplementation. Biochemical analyses further demonstrate that the expression levels of vesicle-specific Zn transporter ZnT3 in the striatum of LB-injected mice treated with clioquinol were decreased, suggesting an intracellular redistribution of Zn. Additionally, we found that clioquinol modulates the autophagy-lysosomal pathway by enhancing lysosomal redistribution within the neuronal compartments. Collectively, we found that in vivo pharmacological chelation of Zn, by dampening Zn-mediated cytotoxicity, can result in an overall attenuation of PD-linked lysosomal alterations and dopaminergic neurodegeneration. The results support zinc chelation as a disease-modifying strategy for treating PD.
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Aug 2022
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