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Article ; Online: An uneven distribution of strontium in the coccolithophore

Walker, Jessica M / Greene, Hallam J M / Moazzam, Yousef / Quinn, Paul D / Parker, Julia E / Langer, Gerald

Environmental science. Processes & impacts

2024

Abstract: Coccolithophores are biogeochemically and ecologically important phytoplankton that produce a composite calcium carbonate-based exoskeleton - the coccosphere - comprised of individual platelets, known as coccoliths. Coccoliths are stunning examples of ... ...

Abstract	Coccolithophores are biogeochemically and ecologically important phytoplankton that produce a composite calcium carbonate-based exoskeleton - the coccosphere - comprised of individual platelets, known as coccoliths. Coccoliths are stunning examples of biomineralization; their formation featuring exceptional control over both biomineral chemistry and shape. Understanding how coccoliths are formed requires information about minor element distribution and chemical environment. Here, the first high-resolution 3D synchrotron X-ray fluorescence (XRF) mapping of a coccolith is presented, showing that the lopadoliths of
Language	English
Publishing date	2024-02-14
Publishing country	England
Document type	Journal Article
ZDB-ID	2703814-2
ISSN	2050-7895 ; 2050-7887
ISSN (online)	2050-7895
ISSN	2050-7887
DOI	10.1039/d3em00509g
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Article ; Online: A passive hutch-cooling system for achieving high thermal-stability operation at the Nanoprobe beamline, Diamond Light Source.

Cacho-Nerin, Fernando / Parker, Julia E / Quinn, Paul D

Journal of synchrotron radiation

2020 Volume 27, Issue Pt 4, Page(s) 912–922

Abstract: The development of low-emittance storage rings and the rapid developments in nano-optics and imaging techniques are leading to decreasing X-ray spot sizes and increasing requirements on the environmental and mechanical stability of beamline components. ... ...

Abstract	The development of low-emittance storage rings and the rapid developments in nano-optics and imaging techniques are leading to decreasing X-ray spot sizes and increasing requirements on the environmental and mechanical stability of beamline components. In particular, temperature stability in the experimental hutches is critical to minimize uncontrolled displacements caused by thermal expansion and ensure consistent performance. Here, the design and thermal performance of the experimental hutches of the Nanoprobe beamline at Diamond Light Source are described, where a standard deviation of the room temperature down to 0.017°C over extended periods is demonstrated. The rooms are kept at constant temperature using water-cooled radiant panels which line the ceiling and walls. Radiant panels are relatively common in high-end electron microscopy rooms, but this is the first demonstration of their use for fine temperature control in an X-ray hutch and may provide a useful basis for future upgrades at upcoming low-emittance sources.
Language	English
Publishing date	2020-05-19
Publishing country	United States
Document type	Journal Article
ZDB-ID	2021413-3
ISSN	1600-5775 ; 0909-0495
ISSN (online)	1600-5775
ISSN	0909-0495
DOI	10.1107/S1600577520004932
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Article ; Online: Toward Understanding the Environmental Risks of Combined Microplastics/Nanomaterials Exposures: Unveiling ZnO Transformations after Adsorption onto Polystyrene Microplastics in Environmental Solutions.

Gomez-Gonzalez, Miguel A / Da Silva-Ferreira, Tatiana / Clark, Nathaniel / Clough, Robert / Quinn, Paul D / Parker, Julia E

Global challenges (Hoboken, NJ)

2023 Volume 7, Issue 8, Page(s) 2300036

Abstract: Over recent decades, there has been a dramatic increase in the manufacture of engineered nanomaterials, which has inevitably led to their environmental release. Zinc oxide (ZnO) is among the more abundant nanomaterial manufactured due to its advantageous ...

Abstract	Over recent decades, there has been a dramatic increase in the manufacture of engineered nanomaterials, which has inevitably led to their environmental release. Zinc oxide (ZnO) is among the more abundant nanomaterial manufactured due to its advantageous properties, used for piezoelectric, semiconducting, and antibacterial purposes. Plastic waste is ubiquitous and may break down or delaminate into smaller microplastics, leaving open the question of whether these small polymers may alter the fate of ZnO through adsorption within aquatic media (tap-water and seawater). Here, scanning electron microscopy analysis confirms the effective Zn nano/microstructures adsorption onto polystyrene surfaces after only 24-h incubation in the aquatic media. After pre-aging the nanomaterials for 7-days in different environmental media, nanoprobe X-ray absorption near-edge spectroscopy analysis reveals significant ZnO transformation toward Zn-sulfide and Zn-phosphate. The interaction between a commercial ZnO-based sunscreen with polystyrene and a cleanser consumer containing microbeads with ZnO nanomaterials is also studied, revealing the adsorption of transformed Zn-species in the microplastics surfaces, highlighting the environmental relevancy of this work. Understanding the structural and functional impacts of the microplastics/ZnO complexes, and how they evolve, will provide insights into their chemical nature, stability, transformations, and fate, which is key to predicting their bioreactivity in the environment.
Language	English
Publishing date	2023-07-05
Publishing country	Germany
Document type	Journal Article
ISSN	2056-6646
ISSN (online)	2056-6646
DOI	10.1002/gch2.202300036
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Article ; Online: A Photodynamic and Photochemotherapeutic Platinum-Iridium Charge-Transfer Conjugate for Anticancer Therapy.

Shi, Huayun / Carter, Oliver W L / Ponte, Fortuna / Imberti, Cinzia / Gomez-Gonzalez, Miguel A / Cacho-Nerin, Fernando / Quinn, Paul D / Parker, Julia E / Sicilia, Emilia / Huang, Huaiyi / Sadler, Peter J

Angewandte Chemie (International ed. in English)

2024 , Page(s) e202400476

Abstract: The novel hetero-dinuclear complex trans,trans,trans-[ ... ...

Abstract	The novel hetero-dinuclear complex trans,trans,trans-[Pt
Language	English
Publishing date	2024-04-24
Publishing country	Germany
Document type	Journal Article
ZDB-ID	2011836-3
ISSN	1521-3773 ; 1433-7851
ISSN (online)	1521-3773
ISSN	1433-7851
DOI	10.1002/anie.202400476
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Article ; Online: Beam and sample movement compensation for robust spectro-microscopy measurements on a hard X-ray nanoprobe.

Quinn, Paul D / Gomez-Gonzalez, Miguel / Cacho-Nerin, Fernando / Parker, Julia E

Journal of synchrotron radiation

2021 Volume 28, Issue Pt 5, Page(s) 1528–1534

Abstract: Static and in situ nanoscale spectro-microscopy is now routinely performed on the Hard X-ray Nanoprobe beamline at Diamond and the solutions implemented to provide robust energy scanning and experimental operation are described. A software-based scheme ... ...

Abstract	Static and in situ nanoscale spectro-microscopy is now routinely performed on the Hard X-ray Nanoprobe beamline at Diamond and the solutions implemented to provide robust energy scanning and experimental operation are described. A software-based scheme for active feedback stabilization of X-ray beam position and monochromatic beam flux across the operating energy range of the beamline is reported, consisting of two linked feedback loops using extremum seeking and position control. Multimodal registration methods have been implemented for active compensation of drift during an experiment to compensate for sample movement during in situ experiments or from beam-induced effects.
Language	English
Publishing date	2021-08-19
Publishing country	United States
Document type	Journal Article
ZDB-ID	2021413-3
ISSN	1600-5775 ; 0909-0495
ISSN (online)	1600-5775
ISSN	0909-0495
DOI	10.1107/S1600577521007736
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Article ; Online: The Hard X-ray Nanoprobe beamline at Diamond Light Source.

Quinn, Paul D / Alianelli, Lucia / Gomez-Gonzalez, Miguel / Mahoney, David / Cacho-Nerin, Fernando / Peach, Andrew / Parker, Julia E

Journal of synchrotron radiation

2021 Volume 28, Issue Pt 3, Page(s) 1006–1013

Abstract: The Hard X-ray Nanoprobe beamline, I14, at Diamond Light Source is a new facility for nanoscale microscopy. The beamline was designed with an emphasis on multi-modal analysis, providing elemental mapping, speciation mapping by XANES, structural phase ... ...

Abstract	The Hard X-ray Nanoprobe beamline, I14, at Diamond Light Source is a new facility for nanoscale microscopy. The beamline was designed with an emphasis on multi-modal analysis, providing elemental mapping, speciation mapping by XANES, structural phase mapping using nano-XRD and imaging through differential phase contrast and ptychography. The 185 m-long beamline operates over a 5 keV to 23 keV energy range providing a ≤50 nm beam size for routine user experiments and a flexible scanning system allowing fast acquisition. The beamline achieves robust and stable operation by imaging the source in the vertical direction and implementing horizontally deflecting primary optics and an overfilled secondary source in the horizontal direction. This paper describes the design considerations, optical layout, aspects of the hardware engineering and scanning system in operation as well as some examples illustrating the beamline performance.
Language	English
Publishing date	2021-04-09
Publishing country	United States
Document type	Journal Article
ZDB-ID	2021413-3
ISSN	1600-5775 ; 0909-0495
ISSN (online)	1600-5775
ISSN	0909-0495
DOI	10.1107/S1600577521002502
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Article ; Online: Multi-resolution Correlative Ultrastructural and Chemical Analysis of Carious Enamel by Scanning Microscopy and Tomographic Imaging.

Besnard, Cyril / Marie, Ali / Sasidharan, Sisini / Buček, Petr / Walker, Jessica M / Parker, Julia E / Spink, Matthew C / Harper, Robert A / Marathe, Shashidhara / Wanelik, Kaz / Moxham, Thomas E J / Salvati, Enrico / Ignatyev, Konstantin / Kłosowski, Michał M / Shelton, Richard M / Landini, Gabriel / Korsunsky, Alexander M

ACS applied materials & interfaces

2023 Volume 15, Issue 31, Page(s) 37259–37273

Abstract: Caries, a major global disease associated with dental enamel demineralization, remains insufficiently understood to devise effective prevention or minimally invasive treatment. Understanding the ultrastructural changes in enamel is hampered by a lack of ... ...

Abstract	Caries, a major global disease associated with dental enamel demineralization, remains insufficiently understood to devise effective prevention or minimally invasive treatment. Understanding the ultrastructural changes in enamel is hampered by a lack of nanoscale characterization of the chemical spatial distributions within the dental tissue. This leads to the requirement to develop techniques based on various characterization methods. The purpose of the present study is to demonstrate the strength of analytic methods using a correlative technique on a single sample of human dental enamel as a specific case study to test the accuracy of techniques to compare regions in enamel. The science of the different techniques is integrated to genuinely study the enamel. The hierarchical structures within carious tissue were mapped using the combination of focused ion beam scanning electron microscopy with synchrotron X-ray tomography. The chemical changes were studied using scanning X-ray fluorescence (XRF) and X-ray wide-angle and small-angle scattering using a beam size below 80 nm for ångström and nanometer length scales. The analysis of XRF intensity gradients revealed subtle variations of Ca intensity in carious samples in comparison with those of normal mature enamel. In addition, the pathways for enamel rod demineralization were studied using X-ray ptychography. The results show the chemical and structural modification in carious enamel with differing locations. These results reinforce the need for multi-modal approaches to nanoscale analysis in complex hierarchically structured materials to interpret the changes of materials. The approach establishes a meticulous correlative characterization platform for the analysis of biomineralized tissues at the nanoscale, which adds confidence in the interpretation of the results and time-saving imaging techniques. The protocol demonstrated here using the dental tissue sample can be applied to other samples for statistical study and the investigation of nanoscale structural changes. The information gathered from the combination of methods could not be obtained with traditional individual techniques.
MeSH term(s)	Humans ; Microscopy, Electron, Scanning ; Scattering, Small Angle ; X-Rays ; Microscopy, Confocal ; Dental Enamel/diagnostic imaging ; Dental Caries/diagnostic imaging
Language	English
Publishing date	2023-07-31
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.3c08031
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Article ; Online: The Delta Robot-A long travel nano-positioning stage for scanning x-ray microscopy.

Kelly, Jon / Male, Andrew / Rubies, Nicholas / Mahoney, David / Walker, Jessica M / Gomez-Gonzalez, Miguel A / Wilkin, Guy / Parker, Julia E / Quinn, Paul D

The Review of scientific instruments

2022 Volume 93, Issue 4, Page(s) 43712

Abstract: A new stage design concept, the Delta Robot, is presented, which is a parallel kinematic design for scanning x-ray microscopy applications. The stage employs three orthogonal voice coils, which actuate parallelogram flexures. The design has a 3 mm travel ...

Abstract	A new stage design concept, the Delta Robot, is presented, which is a parallel kinematic design for scanning x-ray microscopy applications. The stage employs three orthogonal voice coils, which actuate parallelogram flexures. The design has a 3 mm travel range and achieves rms position jitter, integrated from 1 Hz to 1 kHz, of 2.8 and 1.3 nm perpendicular to the beam and 5.6 nm along the beam direction with loads up to 350 g. The Delta Robot design process used a mechatronics approach of iterative modeling and simulation to develop the system and validate performance. The design considerations, design process, stability, and operational performance on the hard x-ray nanoprobe at Diamond Light Source are presented.
MeSH term(s)	Computer Simulation ; Microscopy ; Radiography ; Robotics ; X-Rays
Language	English
Publishing date	2022-04-26
Publishing country	United States
Document type	Journal Article
ZDB-ID	209865-9
ISSN	1089-7623 ; 0034-6748
ISSN (online)	1089-7623
ISSN	0034-6748
DOI	10.1063/5.0084806
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Article ; Online: A cell design for correlative hard X-ray nanoprobe and electron microscopy studies of catalysts under in situ conditions.

Parker, Julia E / Gomez-Gonzalez, Miguel / Van Lishout, Yolanda / Islam, Husn / Duran Martin, Desiree / Ozkaya, Dogan / Quinn, Paul D / Schuster, Manfred E

Journal of synchrotron radiation

2022 Volume 29, Issue Pt 2, Page(s) 431–438

Abstract: To improve the understanding of catalysts, and ultimately the ability to design better materials, it is crucial to study them during their catalytic active states. Using in situ or operando conditions allows insights into structure-property relationships, ...

Abstract	To improve the understanding of catalysts, and ultimately the ability to design better materials, it is crucial to study them during their catalytic active states. Using in situ or operando conditions allows insights into structure-property relationships, which might not be observable by ex situ characterization. Spatially resolved X-ray fluorescence, X-ray diffraction and X-ray absorption near-edge spectroscopy are powerful tools to determine structural and electronic properties, and the spatial resolutions now achievable at hard X-ray nanoprobe beamlines make them an ideal complement to high-resolution transmission electron microscopy studies in a multi-length-scale analysis approach. The development of a system to enable the use of a commercially available gas-cell chip assembly within an X-ray nanoprobe beamline is reported here. The novel in situ capability is demonstrated by an investigation of the redox behaviour of supported Pt nanoparticles on ceria under typical lean and rich diesel-exhaust conditions; however, the system has broader application to a wide range of solid-gas reactions. In addition the setup allows complimentary in situ transmission electron microscopy and X-ray nanoprobe studies under identical conditions, with the major advantage compared with other systems that the exact same cell can be used and easily transferred between instruments. This offers the exciting possibility of studying the same particles under identical conditions (gas flow, pressure, temperature) using multiple techniques.
Language	English
Publishing date	2022-02-15
Publishing country	United States
Document type	Journal Article
ZDB-ID	2021413-3
ISSN	1600-5775 ; 0909-0495
ISSN (online)	1600-5775
ISSN	0909-0495
DOI	10.1107/S1600577521013576
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Article ; Online: Nanoscale chemical heterogeneity dominates the optoelectronic response of alloyed perovskite solar cells.

Frohna, Kyle / Anaya, Miguel / Macpherson, Stuart / Sung, Jooyoung / Doherty, Tiarnan A S / Chiang, Yu-Hsien / Winchester, Andrew J / Orr, Kieran W P / Parker, Julia E / Quinn, Paul D / Dani, Keshav M / Rao, Akshay / Stranks, Samuel D

Nature nanotechnology

2021 Volume 17, Issue 2, Page(s) 190–196

Abstract: Halide perovskites perform remarkably in optoelectronic devices. However, this exceptional performance is striking given that perovskites exhibit deep charge-carrier traps and spatial compositional and structural heterogeneity, all of which should be ... ...

Abstract	Halide perovskites perform remarkably in optoelectronic devices. However, this exceptional performance is striking given that perovskites exhibit deep charge-carrier traps and spatial compositional and structural heterogeneity, all of which should be detrimental to performance. Here, we resolve this long-standing paradox by providing a global visualization of the nanoscale chemical, structural and optoelectronic landscape in halide perovskite devices, made possible through the development of a new suite of correlative, multimodal microscopy measurements combining quantitative optical spectroscopic techniques and synchrotron nanoprobe measurements. We show that compositional disorder dominates the optoelectronic response over a weaker influence of nanoscale strain variations even of large magnitude. Nanoscale compositional gradients drive carrier funnelling onto local regions associated with low electronic disorder, drawing carrier recombination away from trap clusters associated with electronic disorder and leading to high local photoluminescence quantum efficiency. These measurements reveal a global picture of the competitive nanoscale landscape, which endows enhanced defect tolerance in devices through spatial chemical disorder that outcompetes both electronic and structural disorder.
Language	English
Publishing date	2021-11-22
Publishing country	England
Document type	Journal Article
ZDB-ID	2254964-X
ISSN	1748-3395 ; 1748-3387
ISSN (online)	1748-3395
ISSN	1748-3387
DOI	10.1038/s41565-021-01019-7
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