I13-1-Coherence
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Abstract: The butterfly wing scales are biocomposites with impressive structural and optical properties, owing to their features spanning from hundreds of microns to a few nanometers. Though they demonstrate efficient color production and structural rigidity, the mechanisms to achieve them are well-concealed across different length scales. As a result, understanding these biocomposites' composition, structure, and corresponding function remains challenging. No single technique can provide a high-resolution three-dimensional (3D) volume with an accurate color map. Traditionally, approaches such as light microscopy (LM) and spectrophotometry for color responses, and scanning electron microscopes (SEM) and transmission electron microscopes (TEM) for structural imaging provide key insights. However, these methods offer either limited resolution (LM) or limited field of view (TEM), falling short of capturing the full complexity of the scales. Here, we used ptychographic X-ray computed tomography (PXCT), which provides 3D density maps at an intermediate resolution (66.5nm) over hundreds of microns. This allowed us to combine the inferences from the high-resolution (<1 nm), limited view structural insights from TEM/SEM with the low-resolution (>1 microm) color response from LM/spectrophotometry. In Figure 1, the images obtained from various modalities are shown along with their corresponding length scales. Notably, PXCT provides both 3D structural measurements and density values. The 3D structural measurements enable us to estimate the tilt map of the continuous lower lamina structure of the scale and the thickness map of the intricate upper lamina structure. The known physics behind the reflectance and absorbance spectra enables us to combine insights from a wide range of imaging modalities synergistically. An optical model estimates reflectance spectra by integrating thickness and tilt information from PXCT and sub-layer separation insights from the resin section TEM. This computational scheme iteratively solves for the refractive indices of the scale layers from the experimentally measured reflectance spectra. Further, such correlative modeling provides the reflectance map of the scale (Fig. 2), which explains the spatial colour variation (adwing) and the influence of the upper lamina in diffusing the color (abwing). In addition, the 3D thickness map of the upper lamina is utilized to get the absorption coefficient of the upper and the lower lamina from the measured absorbance spectra. The absorption coefficient values showed that the upper and lower lamina have similar pigment densities. This work demonstrates that a multi-modal imaging approach, integrating computational and optical modeling, can reveal unique and novel insights into biocomposites that cannot be possible with any single imaging method alone.
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Feb 2025
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I13-1-Coherence
I13-2-Diamond Manchester Imaging
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Christoph
Rau
,
Darren J.
Batey
,
Shashidhara
Marathe
,
Leonard
Turpin
,
Kudakwashe
Jakata
,
Silvia
Cipiccia
,
Isabel
Anthony
,
Roberto
Volpe
,
Claus-Peter
Richter
,
Alessandra
Carriero
,
Maud
Dumoux
,
Jurgen E.
Schneider
,
Erica
Dall'Armellina
,
Marc W.
Holderied
,
Jan
Van Den Bulcke
Open Access
Abstract: We report about the experimental work related to hierarchical structures at the Diamond I13L beamlines. The I13-2 Imaging and I13-1 Coherence beamlines provide imaging with micro- and nano-resolution. The Diamond II upgrade for the synchrotron source and the OCTOPI upgrade for I13L provide new opportunities for expanding the existing scientific areas in multiscale and operando imaging. We describe the scientific research benefitting from the instrumental upgrade. Comparable recording times across all length scales will enable hierarchical operando imaging. With the implementation of automated high-throughput data acquisition and analysis, large numbers of samples will be analyzed.
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Nov 2024
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I13-1-Coherence
I16-Materials and Magnetism
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David
Serban
,
Daniel G.
Porter
,
Ahmed H.
Mokhtar
,
Mansoor
Nellikkal
,
Sivaperuma
Uthayakumar
,
Min
Zhang
,
Stephen P.
Collins
,
Alessandro
Bombardi
,
Peng
Li
,
Christoph
Rau
,
Marcus
Newton
Diamond Proposal Number(s):
[31929, 34075, 34025, 29880, 27621]
Open Access
Abstract: Although the LiCoO2 (LCO) cathode material has been widely used in commercial lithium ion batteries (LIB) and shows high stability, LIB’s improvements have several challenges that still need to be overcome. In this paper, we have studied the in-operando structural properties of LCO within battery cells using Bragg Coherent X-ray Diffraction Imaging to identify ways to optimise the LCO batteries’ cycling. We have successfully reconstructed the X-ray scattering phase variation (a fingerprint of atomic displacement) within a ≈ (1.6 × 1.4 × 1.3) μm3 LCO nanocrystal across a charge/discharge cycle. Reconstructions indicate strained domains forming, expanding, and fragmenting near the surface of the nanocrystal during charging, with a determined maximum relative lattice displacements of 0.467 Å. While discharging, all domains replicate in reverse the effects observed from the charging states, but with a lower maximum relative lattice displacements of 0.226 Å. These findings show the inefficiency-increasing domain dynamics within LCO lattices during cycling.
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Oct 2024
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I13-1-Coherence
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Diamond Proposal Number(s):
[25097, 28495, 30308]
Abstract: Understanding the impact of strain (structural deformation) is crucial to the success of halide perovskite materials used in optoelectronic devices such as solar cells, X-ray detectors, and LEDs. While halide perovskites demonstrate the potential for enhanced efficiency in these devices, research is ongoing to investigate strain and defects that still hinder device performance and stability.
In experiments to understand the structural changes that can occur during device operation, scientists used Synchrotron-based Bragg Coherent Diffraction Imaging (BCDI) - an X-ray-based imaging technique - to map nanoscale strain in halide perovskite microcrystals (MAPbBr3 [MA = CH3NH3]), including strain around defects. Published in Advanced Materials, the experiments were part of a recent study from Diamond’s I13-1 beamline (Figure 1), which reveals the dynamic migration of nanoscale extended defects in halide perovskites under continuous light illumination. These insights demonstrate the highly dynamic nature of the structure of halide perovskite materials and how they evolve under operational conditions, highlighting the close links between nanoscale structure, dislocations, and device performance and stability.
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Sep 2024
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I13-1-Coherence
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Diamond Proposal Number(s):
[33421]
Abstract: Promotion of oxygen reduction reaction (ORR) kinetics, to a large extent, depends on the rational modulation of the electronic structure and mass diffusion of electrocatalysts. Herein, a ferrocene (Fc)–assisted strategy is developed to prepare Fc-trapped ZnMo–hybrid zeolitic imidazolate framework (Fc@ZnMo-HZIF-50) and the derived Fe single atom coupling with MoC nanoparticles, coembedded in hierarchically porous N-doped carbon cubes (MoC@FeNC-50). The introduced Fc is utilized not only as an iron source for single atoms but also as a morphology regulator for generating a hierarchically porous structure. The redistribution of electrons between Fe single atoms and MoC nanoparticles effectively promotes the adsorption of O2 and the formation of *OOH intermediates during the ORR process. Along with a 3D hierarchically porous architecture for enhanced mass transport, the as-fabricated MoC@FeNC-50 presents excellent activity (E1/2 = 0.83 V) and durability (only 9.5% decay in current after 40000 s). This work could inspire valuable insights into the construction of efficient electrocatalysts through electron configuration and kinetics engineering.
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Aug 2024
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I13-1-Coherence
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Diamond Proposal Number(s):
[34119]
Open Access
Abstract: We introduce the weighted average of sequential projections, or WASP, an algorithm for ptychography. Using both simulations and real-world experiments, we test this new approach and compare performance against several alternative algorithms. These tests indicate that WASP effectively combines the benefits of its competitors, with a rapid initial convergence rate, robustness to noise and poor initial conditions, a small memory footprint, easy tuning, and the ability to reach a global minimum when provided with noiseless data. We also show how WASP can be parallelised to split operation across several different computation nodes.
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May 2024
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I13-1-Coherence
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Diamond Proposal Number(s):
[34189, 32306]
Open Access
Abstract: X-ray ptychography, a scanning coherent diffraction imaging technique, is one of the most used techniques at synchrotron facilities for high resolution imaging, with applications spanning from life science to nano-electronics. In the recent years there has been a great effort to make the technique faster to enable high throughput nanoscale imaging. Here we apply a fast ptychography scanning method to image in 3D
μ
of brain-like phantom at 3 kHz, in a 7 h acquisition with a resolution of 270 nm. We then present the latest advances in fast ptychography by showing 2D images acquired at 110 kHz by combining the fast-acquisition scheme with a high-acquisition rate prototype detector from DECTRIS Ltd. We finally review the experimental outcome and discuss the prospective use of fast ptychography schemes for the investigation of mm size samples of brain-like phantom, by extrapolating the current results to the high coherent flux scenario of diffraction limited storage rings.
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May 2024
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I13-1-Coherence
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Kieran W. P.
Orr
,
Jiecheng
Diao
,
Krishanu
Dey
,
Madsar
Hameed
,
Milos
Dubajic
,
Hayley L.
Gilbert
,
Thomas A.
Selby
,
Szymon J.
Zelewski
,
Yutong
Han
,
Melissa R.
Fitzsimmons
,
Bart
Roose
,
Peng
Li
,
Jiadong
Fan
,
Huaidong
Jiang
,
Joe
Briscoe
,
Ian K.
Robinson
,
Samuel D.
Stranks
Diamond Proposal Number(s):
[31362]
Open Access
Abstract: Strain is an important property in halide perovskite semiconductors used for optoelectronic applications because of its ability to influence device efficiency and stability. However, descriptions of strain in these materials are generally limited to bulk averages of bare films, which miss important property-determining heterogeneities that occur on the nanoscale and at interfaces in multilayer device stacks. Here, we present three-dimensional nanoscale strain mapping using Bragg coherent diffraction imaging of individual grains in Cs0.1FA0.9Pb(I0.95Br0.05)3 and Cs0.15FA0.85SnI3 (FA = formamidinium) halide perovskite absorbers buried in full solar cell devices. We discover large local strains and striking intragrain and grain-to-grain strain heterogeneity, identifying distinct islands of tensile and compressive strain inside grains. Additionally, we directly image dislocations with surprising regularity in Cs0.15FA0.85SnI3 grains and find evidence for dislocation-induced antiphase boundary formation. Our results shine a rare light on the nanoscale strains in these materials in their technologically relevant device setting.
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May 2024
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I13-1-Coherence
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Mattia Francesco Maria
Gerli
,
Giuseppe
Cala
,
Max Arran
Beesley
,
Beatrice
Sina
,
Lucinda
Tullie
,
Kylin Yunyan
Sun
,
Francesco
Panariello
,
Federica
Michielin
,
Joseph R.
Davidson
,
Francesca Maria
Russo
,
Brendan C.
Jones
,
Dani Do Hyang
Lee
,
Savvas
Savvidis
,
Theodoros
Xenakis
,
Ian C.
Simcock
,
Anna A.
Straatman-Iwanowska
,
Robert A.
Hirst
,
Anna L.
David
,
Christopher
O’callaghan
,
Alessandro
Olivo
,
Simon
Eaton
,
Stavros P.
Loukogeorgakis
,
Davide
Cacchiarelli
,
Jan
Deprest
,
Vivian S. W.
Li
,
Giovanni Giuseppe
Giobbe
,
Paolo
De Coppi
Diamond Proposal Number(s):
[31437]
Open Access
Abstract: Isolation of tissue-specific fetal stem cells and derivation of primary organoids is limited to samples obtained from termination of pregnancies, hampering prenatal investigation of fetal development and congenital diseases. Therefore, new patient-specific in vitro models are needed. To this aim, isolation and expansion of fetal stem cells during pregnancy, without the need for tissue samples or reprogramming, would be advantageous. Amniotic fluid (AF) is a source of cells from multiple developing organs. Using single-cell analysis, we characterized the cellular identities present in human AF. We identified and isolated viable epithelial stem/progenitor cells of fetal gastrointestinal, renal and pulmonary origin. Upon culture, these cells formed clonal epithelial organoids, manifesting small intestine, kidney tubule and lung identity. AF organoids exhibit transcriptomic, protein expression and functional features of their tissue of origin. With relevance for prenatal disease modeling, we derived lung organoids from AF and tracheal fluid cells of congenital diaphragmatic hernia fetuses, recapitulating some features of the disease. AF organoids are derived in a timeline compatible with prenatal intervention, potentially allowing investigation of therapeutic tools and regenerative medicine strategies personalized to the fetus at clinically relevant developmental stages.
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Mar 2024
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I13-1-Coherence
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Diamond Proposal Number(s):
[19194, 21309]
Open Access
Abstract: We apply X-ray ptycho-tomography to perform high-resolution, non-destructive, three-dimensional (3D) imaging of Fe-rich inclusions in paleomagnetically relevant materials (zircon single crystals from the Bishop Tuff ignimbrite). Correlative imaging using quantum diamond magnetic microscopy combined with X-ray fluorescence mapping was used to locate regions containing potential ferromagnetic remanence carriers. Ptycho-tomographic reconstructions with voxel sizes 85 nm and 21 nm were achievable across a field-of-view > 80 µm; voxel sizes as small as 5 nm were achievable over a limited field-of-view using local ptycho-tomography. Fe-rich inclusions 300 nm in size were clearly resolved. We estimate that particles as small as 100 nm—approaching single-domain threshold for magnetite—could be resolvable using this “dual-mode” methodology. Fe-rich inclusions (likely magnetite) are closely associated with apatite inclusions that have no visible connection to the exterior surface of the zircon (e.g., via intersecting cracks). There is no evidence of radiation damage, alteration, recrystallisation or deformation in the host zircon or apatite that could provide alternative pathways for Fe infiltration, indicating that magnetite and apatite grew separately as primary phases in the magma, that magnetite adhered to the surfaces of the apatite, and that the magnetite-coated apatite was then encapsulated as primary inclusions within the growing zircon. Rarer examples of Fe-rich inclusions entirely encapsulated by zircon are also observed. These observations support the presence of primary inclusions in relatively young and pristine zircon crystals. Combining magnetic and tomography results we deduce the presence of magnetic carriers that are in the optimal size range for carrying strong and stable paleomagnetic signals but that remain below the detection limits of even the highest-resolution X-ray tomography reconstructions. We recommend the use of focused ion beam nanotomography and/or correlative transmission electron microscopy to directly confirm the presence of primary magnetite in the sub 300 nm range as a necessary step in targeted paleomagnetic workflows.
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Mar 2024
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