B18-Core EXAFS
I18-Microfocus Spectroscopy
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Swaroop
Chakraborty
,
Iuliia
Mikulska
,
Rhiannon
Boseley
,
Sang
Pham
,
Prathmesh
Bhadane
,
Pankti
Dhumal
,
Santanu
Majumder
,
Jajati
Mandal
,
Tina
Geraki
,
Superb K.
Misra
,
Christian
Pfrang
,
Iseult
Lynch
Diamond Proposal Number(s):
[33674, 35117, 41674]
Open Access
Abstract: Metal–organic frameworks (MOFs) are increasingly deployed in environmental technologies, yet their fate and hazard under realistic multistep exposure scenarios remain poorly constrained. Here, we track hierarchical transformations of nanoscale ZIF-8 (Zeolitic Imidazolate Framework-8) across an exposure cascade spanning atmospheric aging (air and reactive gases O3/NO2), aqueous aging in environmentally and biologically relevant media, and ingestion by the freshwater crustacean Daphnia magna. Synchrotron Zn K-edge X-ray absorption spectroscopy (XAS), micro-X-ray fluorescence (μ-XRF), X-ray photoelectron spectroscopy (XPS), and electron microscopy show that gas-phase exposure produces only minor surface perturbations, whereas aqueous contact drives pronounced medium-dependent restructuring, including nitrogen depletion and oxygen enrichment at the surface and time-resolved dissolved Zn release with chemistry-imposed plateaus. In vivo, Zn speciation diverges from the pristine Zn–N fingerprint; an unexposed endogenous Zn baseline and linear combination fitting (LCF) indicate a mixture of endogenous Zn with transformed Zn pools dominated by O/P/S-type coordination environments. Acute ecotoxicity assay demonstrates strong concentration dependence (48 h immobilization EC50 ≈0.5 μg mL–1), and chronic exposure at 0.10 μg mL–1 reduces cumulative brood production with increased adult mortality over 24 days. Mechanistically, fractionated toxicity assays show that washed aged particles/precipitates and whole aged suspensions are more potent than particle-free filtrates, indicating that particle-associated transformed Zn pools contribute substantially beyond dissolved Zn alone. Together, these results show that ZIF-8 risk emerges from its sequential transformation trajectory rather than its pristine state, motivating tiered aging protocols coupled to in vivo speciation and fractionated hazard testing for MOF safety assessment.
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May 2026
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I12-JEEP: Joint Engineering, Environmental and Processing
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Abstract: Amid rising global demand for renewable energy and effective plastic waste management, adopting green methods to utilize plastic waste for chemicals is a win–win strategy. Constituting the largest amount of single-use plastic litter worldwide, cellulose diacetate (CDA) based waste cigarette filters urgently require sustainable valorization pathways. However, CDA photoconversion remains highly challenging due to substantial energy barriers for selective bond cleavage, inadequate radical generation capability, and inefficient charge-carrier separation. Herein we propose a strategy to efficiently obtain C2H4 through carbene-mediated CDA photoconversion by using a sulfur vacancy-regulated copper-gallium-zinc-sulfide (VS-CGZS) catalyst. VS-CGZS enhances the thermal effect of light and lowers the energy barrier for acetyl group (*CH3CO) desorption from CDA. VS reduces the adsorption energy of *CH3CO on VS-CGZS and facilitated :CH2 formation. Consumption of photogenerated holes via *CH3CO desorption and VS-enhanced carrier separation synergistically elevate the photogenerated electrons concentration for :CH2 coupling, thereby selectively triggering and boosting C2H4 yield. Therefore, we achieve a record-breaking 14.43 mmol·gcat–1 C2H4 for CDA photoconversion within 4 h, over 6 times exceeding previous reports on photoconverting plastic into C2H4. This work establishes a strategy for efficient ethylene production from photoconversion of cellulose diacetate and carves out a paradigm in solar-driven plastic valorization.
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May 2026
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I07-Surface & interface diffraction
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Diamond Proposal Number(s):
[35227]
Open Access
Abstract: Organic semiconductors offer a long-spin coherence time and diffusion length due to the weak spin–orbit and hyperfine interactions in these materials. However, in commonly used lateral field-effect transistor structures, it is challenging to define device dimensions comparable to the spin diffusion length. On the other hand, vertical structures, offering smaller device dimensions, are facing issues due to the low carrier mobilities in the vertical dimension. Here, we investigate spin relaxation in rubrene thin films with a triclinic phase, which are doped with C60F48 by coevaporation. The doping provides an efficient way to generate charge carriers, and their high out-of-plane mobility should enhance long-spin diffusion. Using electron-spin resonance, we show that the spin relaxation is governed by the interaction with the dopant counterions and estimate the spin diffusion length to be ∼200 nm. This is comparable to the film thickness, which should make such doped rubrene films an attractive system for spintronic device applications.
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Mar 2026
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I04-1-Macromolecular Crystallography (fixed wavelength)
I04-Macromolecular Crystallography
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André
Shamsabadi
,
Adam
Creamer
,
Christy J.
Sadler
,
Aida
Abdelwahed
,
Katherine U.
Gaynor
,
Yuliya
Demydchuk
,
Gabriela
Ivanova-Berndt
,
Katerine
Van Rietschoten
,
Paul
Beswick
,
Liuhong
Chen
,
Gustavo
Arruda Bezerra
,
Aleksei
Lulla
,
Paul
Brear
,
Marko
Hyvonen
,
Michael J.
Skynner
,
Molly M.
Stevens
Diamond Proposal Number(s):
[25402]
Open Access
Abstract: Constrained bicyclic peptides (Bicycle molecules) with high affinity for biological targets have emerged as potentially powerful therapeutic agents, particularly for the in vivo targeting of cancer receptors. However, their antibody-mimetic properties have yet to be explored for use in diagnostic immunoassays. These synthetically derived compounds serve as biorecognition scaffolds that allow for facile site-selective modification and large-scale production. A phage display screen against various constructs of the SARS-CoV-2 nucleocapsid (N) protein identified several Bicycle molecules with binding affinities ranging from the micromolar to the low nanomolar range. These Bicycle molecules were validated in the development of enzyme- and nanozyme-linked immunosorbent assays, as well as enzymatic and colorimetric nanoparticle-based lateral flow immunoassays (LFIA) for the detection of ultralow concentrations of the SARS-CoV-2 N protein. We envision that these moieties enable robust, cost-effective, and large-scale development of ultrasensitive biosensors for a diverse range of biomarkers by leveraging their high binding affinity, minimalistic scaffold, and synthetic accessibility.
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Feb 2026
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Sanghyo
Lee
,
Sojin
Kim
,
Jinseok
Ryu
,
Jaewook
Lee
,
Jinseok
Hong
,
Ji Eun
Kim
,
Ju-Young
Cha
,
Yunho
Shin
,
Daewoong
Kwon
,
Jung Ho
Yoon
,
Min Hyuk
Park
,
Miyoung
Kim
,
Seung-Yong
Lee
Abstract: Understanding electric-field-induced phase transitions is crucial for optimizing the ferroelectric and antiferroelectric properties of hafnium zirconium oxide (Hf0.5Zr0.5O2, HZO) thin films. Here, we use in situ transmission electron microscopy (TEM) to uncover the nanoscale mechanism of field-induced phase evolution in ultrathin HZO films at the morphotropic phase boundary (MPB), directly visualizing oxygen vacancy migration and its correlation with the transformation from the nonpolar tetragonal to polar orthorhombic phase. Our in situ TEM setup applied sub-100 μs bipolar voltage pulses, mimicking real device operation while allowing the detection of the subtle changes induced by such short pulses. Unsupervised machine learning analysis of electron energy-loss spectroscopy spectrum images (EELS-SIs) revealed distinct spectral features associated with local structural evolution, with quantitative results confirming oxygen-deficient regions aligned with orthorhombic phase formation. Unlike conventional TEM studies confined to a few nanoscale domains, this approach enables film-scale interpretation of phase evolution, capturing broader trends beyond isolated observations. Concurrent oxygen content changes in the TiN electrode further indicate active vacancy exchange between HZO and TiN under bias. These findings directly link oxygen vacancy dynamics to polarization switching, offering critical guidance for stabilizing ferroelectric phases and advancing next-generation memory and logic devices.
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Feb 2026
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I05-ARPES
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Oliver J.
Clark
,
Anugrah
Azhar
,
Thi-Hai-Yen
Vu
,
Benjamin A.
Chambers
,
Federico
Mazzola
,
Sadhana
Sridhar
,
Geetha
Balakrishnan
,
Aaron
Bostwick
,
Chris
Jozwiak
,
Eli
Rotenberg
,
Sarah L.
Harmer
,
Mohammad Saeed
Bahramy
,
Michael S.
Fuhrer
,
Mark T.
Edmonds
Diamond Proposal Number(s):
[40610]
Open Access
Abstract: Discovering and engineering spin-polarized surface states in the electronic structures of condensed matter systems is a crucial first step in the development of spintronic devices, wherein spin-polarized bands crossing the Fermi level can facilitate information transfer. Here, through nanofocused angle-resolved photoemission spectroscopy (nano-ARPES) and density functional theory-based calculations, we show that the interface between monolayer WSe2 and metallic NbSe2 exhibits a negative Schottky barrier height of ∼ −30 meV: the K-point valleys of the semiconducting layer are shifted by ∼800 meV to produce a surface-localized Fermi surface populated only by spin-polarized charge carriers. By increasing the WSe2 thickness, the Fermi pockets can be moved from K to Γ, demonstrating tunability of novel semimetallic phases that exist atop a substrate additionally possessing charge density wave and superconducting phases. Together, this study provides a spectroscopic understanding into p-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development.
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Feb 2026
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I22-Small angle scattering & Diffraction
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Diamond Proposal Number(s):
[33542]
Open Access
Abstract: Artificial cells assembled from materials such as hydrogels have emerged as platforms to replicate and understand biological functionalities, processes, and behaviors. However, hydrogels lack a lipid membrane, a vital property of cellular systems. Here we develop a process for the assembly of a fluid and stable lipid membrane which coats the hydrogel mesh network within the particle, through electostatically-mediated fusion of nanoscale lipid vesicles. This confers cell-mimetic and biotechnologically relevant properties upon microscale, cell sized, hydrogel artificial cells generated through microfluidics. We exploit the properties of the created membrane to augment existing hydrogel properties through permeability alteration and protection of the hydrogel from small molecule degraders. Furthermore, we show that the lipid membrane is compatible with organelle substructures within the hydrogels, which enables the exploitation of an enhanced material design space to build hydrogel artificial cells that increasingly mimic the organization of cells. This platform paves the way for producing next generation artificial cells and functional microdevices from interfaced hydrogel-lipid materials. Our technologies may underpin new opportunities for integrating membranes into hydrogel-based systems, inlcuding for drug delivery and tissue engineering.
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Jan 2026
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E02-JEM ARM 300CF
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Wendong
Wang
,
Gareth R.
Tainton
,
Nicholas J.
Clark
,
James G.
Mchugh
,
Xue
Li
,
Sam
Sullivan-Allsop
,
David G.
Hopkinson
,
Oldrich
Cicvárek
,
Francisco
Selles
,
Rui
Zhang
,
Joshua D.
Swindell
,
Alex
Summerfield
,
David J.
Lewis
,
Vladimir I.
Fal'Ko
,
Zdenek
Sofer
,
Sarah
Haigh
,
Roman
Gorbachev
Diamond Proposal Number(s):
[39088]
Abstract: Transition metal diiodides such as FeI2, NiI2, and CoI2 are an emerging class of 2D magnets exhibiting rich and diverse magnetic behavior, but their study at the monolayer limit has been severely hindered by fabrication challenges due to their air-sensitivity. Here, we introduce a polymer-free method for clean, rapid, and high-yield assembly of hermetically encapsulated suspended samples of air-sensitive monolayers. Applied to diiodides, it enables atomic resolution characterization of thin samples down to the monolayer limit using transmission electron microscopy. Our imaging, combined with complementary first-principles calculations, reveals an unusually small energy barrier between alternate stable stacking polytypes in few-layer films, enabling extrinsic control of the stacking phase. We also observe stable isolated iodine vacancies that do not aggregate to form extended structures and identify and verify the stability of the various edge configurations of thin samples. These results establish the structural characteristics of these materials in the thin limit and more broadly demonstrate the utility of our transfer platform for creating atomically clean suspended van der Waals heterostructures.
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Jan 2026
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B18-Core EXAFS
I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[33674, 35117, 35776, 40942]
Open Access
Abstract: Metal–organic frameworks (MOFs) are entering water technologies on the premise that abiotic stability predicts ecological safety. We overturn this assumption by showing that UiO-66 – often regarded as chemically and structurally robust – remains intact after 7-day aging in natural borehole water yet undergoes rapid in vivo transformation in Daphnia magna. Synchrotron Microfocus X-ray absorption spectroscopy (XAS) revealed collapse of the ordered Zr–carboxylate coordination into disordered Zr–O environments within the gut; Extended X-ray Absorption Fine Structure (EXAFS) showed loss of second-shell features, and Transmission Electron Microscopy (TEM) confirmed loss of crystallinity with nanoscale aggregates appearing within 24 h of ingestion. Although acute immobilization was limited (48 h EC50 ≈ 26.5 μg mL–1), a sublethal, environmentally relevant exposure (10 μg mL–1) caused pronounced chronic effects: brood initiation was delayed by 3–5 days and cumulative reproduction decreased by ∼74% without mortality. We attribute these outcomes to gut-level transformation and associated energetic/physiological burdens, not captured by standard acute tests. These results show that abiotic stability does not necessarily imply biological inertness and highlight the need to integrate in vivo transformation pathways with chronic end points in environmental risk assessment for water-sector materials. This perspective provides a mechanistic basis to inform Safe-and-Sustainable-by-Design (SSbD) MOFs before widespread deployment in water treatment.
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Dec 2025
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I09-Surface and Interface Structural Analysis
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Ye
Wang
,
Manish
Chhowalla
,
Yiru
Zhu
,
Tieyuan
Bian
,
Ziwei J.
Yang
,
Yuanyua
Zhao
,
Han
Yan
,
Yang
Li
,
Yan
Wang
,
Feng
Ding
,
Jun
Yin
Diamond Proposal Number(s):
[35092, 30105, 33391, 32963, 38086]
Open Access
Abstract: Engineering chiral optical and electronic properties of materials is interesting for applications in sensing and quantum information. State-of-the-art chiral optoelectronic devices are mostly based on three-dimensional (3D) and quasi-two-dimensional (2D) materials. Here we demonstrate chiral 2D MoS2 with sub-nanometer thickness via chirality transfer from l-/d-penicillamine (l-/d-PEN). We report a giant molar ellipticity of 108 deg·cm2/dmol in monolayer solid-state films, up to 3 orders of magnitude higher than 3D chiral materials. Phototransistors with chiral 2D MoS2 channels exhibit gate-tunable circularly polarized light detection with responsivity of >102 A/W and anisotropy g-factor of 1.98, close to the theoretical maximum of 2.0. The reduced dimensionality magnifies the chirality transfer efficiency, allowing realization of ultrasensitive detectors for circularly polarized photons.
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Oct 2025
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