E01-JEM ARM 200CF
E02-JEM ARM 300CF
I14-Hard X-ray Nanoprobe
I18-Microfocus Spectroscopy
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Open Access
Abstract: Phyllosilicate minerals in the carbonaceous chondrites provide insights into processes in primitive parent bodies of the early Solar System. It is widely agreed that the CM- and CI-type carbonaceous chondrites underwent aqueous alteration on their parent bodies, resulting in phyllosilicate-rich matrices, where the dominant mineral phase is serpentine. There are many previous studies investigating phyllosilicate structure in carbonaceous chondrites, however, the presence of sulfur in these minerals and its effect on crystal lattice structure has not been studied in detail. We are investigating how the presence of sulfur (up to ≃9-10 wt% SO3) in serpentine phyllosilicate regions effects basal lattice spacing measurements of serpentine-like minerals in CM- and CI-type chondritic and related asteroidal material.
Four specimens are being studied for this work: Winchcombe and Aguas Zarcas (CM-type), and Ryugu samples (A0058-C2001-08, A0104-00200502 and A0104-01700602) from Hayabusa2 and Ivuna (CI-type). All samples are TEM wafers. We have used a multi-technique approach to study the samples, with the E01 JEOL ARM200CF and E02 JEOL ARM300CF electron microscopes at the ePSIC facility at Diamond Light Source in Harwell, UK. EDS compositional data has been collected using the E01 microscope, whilst HRTEM and HAADF imaging data has been collected at E02. At E02 we are also applying a new 4D-STEM nano-diffraction technique in order to collect lattice spacing data to correlate with our other HRTEM results. Fe-K XANES analyses on Winchcombe and Ryugu have been carried out using the I18 microprobe and I14 hard x-ray nanoprobe respectively, also at Diamond Light Source, to constrain Fe3+/ΣFe. By combining these techniques we aim to better understand the physical and chemical structure of serpentine-like minerals in carbonaceous chondrites.
Initial analyses have shown that sulfur presence in carbonaceous chondrite phyllosilicates reduces the basal lattice spacings of serpentine-like minerals. In these sulfur-bearing regions, we have been finding lattice spacings in the range ~0.60-0.74nm for the CM-type chondrites. For the CI-type, these range between ~0.65-0.76nm. Differences in the reduced lattice spacing ranges are likely related to the redox state of the sulfur. In Ryugu and other carbonaceous chondrites the sulfur appears reduced; its content in serpentine is low and we see FeS grains. Comparatively, in Winchcombe (and others) more of the sulfur seems to be in the serpentine structure.
We can conclude that in serpentine-like minerals, the presence of sulfur appears to reduce basal lattice spacing values compared to the expected d-spacing value of 0.70nm for serpentine. Possible reasons for this include further investigations into the valency of the sulfur ions, the bonding environment within serpentine layers, and the location of sulfur in either the octa- or tetrahedral lattice sites.
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Feb 2023
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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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Diamond Proposal Number(s):
[28142]
Open Access
Abstract: The interaction of a focused X-ray beam with a sample in a scanning probe experiment can provide a variety of information about the interaction volume. In many scanning probe experiments X-ray fluorescence (XRF) is supplemented with measurements of the transmitted or scattered intensity using a pixelated detector. The automated extraction of different signals from an area pixelated detector is described, in particular the methodology for extracting differential phase contrast (DPC) is demonstrated and different processing methods are compared across a range of samples. The phase shift of the transmitted X-ray beam by the sample, extracted from DPC, is also compared with ptychography measurements to provide a qualitative and quantitative comparison. While ptychography produces a superior image, DPC can offer a simple, flexible method for phase contrast imaging which can provide fast results and feedback during an experiment; furthermore, for many science problems, such as registration of XRF in a lighter matrix, DPC can provide sufficient information to meet the experimental aims. As the DPC technique is a quantitative measurement, it can be expanded to spectroscopic studies and a demonstration of DPC for spectro-microscopy measurements is presented. Where ptychography can separate the absorption and phase shifts by the sample, quantitative interpretation of a DPC image or spectro-microscopy signal can only be performed directly when absorption is negligible or where the absorption contribution is known and the contributions can be fitted.
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Dec 2022
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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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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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Diamond Proposal Number(s):
[31039]
Open Access
Abstract: Combinations of spectroscopic analysis and microscopic techniques are used across many disciplines of scientific research, including material science, chemistry and biology. X-ray spectromicroscopy, in particular, is a powerful tool used for studying chemical state distributions at the micro and nano scales. With the beam fixed, a specimen is typically rastered through the probe with continuous motion and a range of multimodal data is collected at fixed time intervals. The application of this technique is limited in some areas due to: long scanning times to collect the data, either because of the area/volume under study or the compositional properties of the specimen; and material degradation due to the dose absorbed during the measurement. In this work, we propose a novel approach for reducing the dose and scanning times by undersampling the raster data. This is achieved by skipping rows within scans and reconstructing the x-ray spectromicroscopic measurements using low-rank matrix completion. The new method is robust and allows for 5 to 6-fold reduction in sampling. Experimental results obtained on real data are illustrated.
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Nov 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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I14-Hard X-ray Nanoprobe
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Yeseul
Park
,
Zohar
Eyal
,
Péter
Pekker
,
Daniel M.
Chevrier
,
Christopher T.
Lefèvre
,
Pascal
Arnoux
,
Jean
Armengaud
,
Caroline L.
Monteil
,
Assaf
Gal
,
Mihály
Pósfai
,
Damien
Faivre
Diamond Proposal Number(s):
[23693]
Open Access
Abstract: Metal sulfides are a common group of extracellular bacterial biominerals. However, only a few cases of intracellular biomineralization are reported in this group, mostly limited to greigite (Fe3S4) in magnetotactic bacteria. Here, a previously unknown periplasmic biomineralization of copper sulfide produced by the magnetotactic bacterium Desulfamplus magnetovallimortis strain BW-1, a species known to mineralize greigite (Fe3S4) and magnetite (Fe3O4) in the cytoplasm is reported. BW-1 produces hundreds of spherical nanoparticles, composed of 1–2 nm substructures of a poorly crystalline hexagonal copper sulfide structure that remains in a thermodynamically unstable state. The particles appear to be surrounded by an organic matrix as found from staining and electron microscopy inspection. Differential proteomics suggests that periplasmic proteins, such as a DegP-like protein and a heavy metal-binding protein, could be involved in this biomineralization process. The unexpected periplasmic formation of copper sulfide nanoparticles in BW-1 reveals previously unknown possibilities for intracellular biomineralization that involves intriguing biological control and holds promise for biological metal recovery in times of copper shortage.
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Aug 2022
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