I11-High Resolution Powder Diffraction
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Yukun
Ye
,
Lixia
Guo
,
Jiarui
Fan
,
Zhixin
Wang
,
Zhaozhao
Hu
,
Ruohan
Li
,
Siyu
Zhou
,
Lifei
Lin
,
Yiheng
Wang
,
Mark R.
Warren
,
Ben
Coulson
,
Pascal
Manuel
,
Sarah
Day
,
Eamonn T.
Connolly
,
Jiangnan
Li
,
Sihai
Yang
Diamond Proposal Number(s):
[45967]
Abstract: We report the exceptional propyne (C3H4) storage and propylene (C3H6) purification in a metal-organic framework, PKU-101, controlled via regulation of aromaticity. The pyrene-fused pore interior of PKU-101 provides multiple C─H···π interactions for alkyne, resulting in a record C3H4 adsorption of 250 cm3 cm−3 at 298 K and 1 bar, representing a benchmark sorbent for C3H4. Additionally, the supramolecular interactions enable fine thermodynamic discrimination for alkenes, resulting in excellent separation of C2H4/C3H6 (v/v = 1/1), delivering simultaneously high productivities of C3H6 and C2H4 (267 and 174 L kg−1, respectively; C2H4 purity > 99.9 %). Effective separation of C3H6/C3H8 (v/v = 1/1) and C3H4/C3H6 (v/v = 1/99) with a high C3H6 productivity of 532 L kg−1 (purity of 99.99 %) has also been achieved by PKU-101. In situ crystallographic and spectroscopic studies confirmed the key role of enhanced aromaticity on the discrimination of alkanes/alkenes/alkynes. Importantly, these weak supramolecular interactions enable complete regeneration at only 318 K.
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Sep 2026
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B18-Core EXAFS
I11-High Resolution Powder Diffraction
I19-Small Molecule Single Crystal Diffraction
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Xu
Chen
,
Lik Hong
Wee
,
Mohammad Reza
Alizadeh Kiapi
,
Christos
Tampaxis
,
Jiarui
Fan
,
Hamish W.
Macleod
,
Yan
Zheng
,
Benjamin J.
Moore
,
Pascal
Manuel
,
Fabio
Orlandi
,
Luke L.
Keenan
,
Enci
Zhang
,
Mehrdad
Asgari
,
Dhruv
Menon
,
Georgia
Charalambopoulou
,
Tom
Willhammar
,
Sihai
Yang
,
William
Shepard
,
Yong
Cui
,
Theodore
Steriotis
,
David
Fairen-Jimenez
Diamond Proposal Number(s):
[37562, 44352, 42292]
Open Access
Abstract: The construction of highly porous metal–organic frameworks with complex topologies requires precise matching between linker conformation and node connectivity. Here we report the reticular design and synthesis of CU-6-M (M = Fe or Cr), assembled from conformationally adaptive diphenylethynyl linkers and six-connected trinuclear oxo-centred clusters. The ability of the linker to adopt multiple out-of-plane conformations satisfies the geometric requirements of a red topology, resulting in a highly interconnected hierarchical pore architecture. CU-6-Fe and CU-6-Cr exhibit an interconnected hierarchical pore system with Brunauer–Emmett–Teller surface areas up to 7,145 m2 g−1. This architecture enables total H2 uptakes of up to 17.5 wt% and 45.4 g l−1 at 100 bar and 77 K. Under temperature–pressure swing conditions, CU-6-Fe and CU-6-Cr deliver up to 16.9 wt% and 44.1 g l−1 and also show record gravimetric CH4 storage at ambient temperature. These results establish linker flexibility as a key design parameter for the realization of complex, highly porous topologies for high-capacity storage of clean-energy fuel gases.
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Sep 2026
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Pratap
Pal
,
Xiaoxi
Deng
,
Gi‐yeop
Kim
,
Kyoungjun
Lee
,
Jheng-Cyuan
Lin
,
Prithwijit
Mandal
,
Jiangfeng
Yang
,
Paul
Steadman
,
Pascal
Manuel
,
Roger D.
Johnson
,
Si-Young
Choi
,
Paolo G.
Radaelli
,
Chang-Beom
Eom
Open Access
Abstract: The spin cycloid characteristic of noncollinear antiferromagnets offers significant potential for energy-efficient, magnon-mediated spintronic applications. Multiferroic BiFeO3 is among the most promising candidate materials because its antiferromagnetic order can be controlled by an electric field. However, in epitaxial BiFeO3 thin films, substrate clamping and epitaxial strain modify the cycloidal magnetic structure while limiting efficient ferroelastic-ferroelectric switching. Here, we show that strain-released freestanding BiFeO3 membranes overcome these limitations. Compared with substrate-clamped epitaxial thin films, a 100-nm-thick freestanding membrane exhibits ≈50% faster electric-field-driven ferroelectric switching and a spatially uniform, bulk-like single spin cycloid, as revealed by resonant elastic X-ray scattering. In contrast, the epitaxial thin film exhibits an expanded cycloid periodicity and slower ferroelectric switching dynamics, reflecting the influence of substrate-induced strain. Freestanding BiFeO3 membranes therefore overcome substrate-induced constraints by simultaneously restoring the intrinsic bulk-like spin cycloid and enabling substantially faster ferroelectric switching. This combination of robust noncollinear antiferromagnetic order and efficient electric-field switching establishes freestanding BiFeO3 membranes as a promising magnetoelectric platform for low-power magnonic and spintronic technologies, while enabling heterogeneous integration with Si-based devices.
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Aug 2026
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I11-High Resolution Powder Diffraction
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Robert D.
Smyth
,
Bradley C.
Sheath
,
Lemuel E.
Crentsil
,
Xiaoyu
Xu
,
Simon J.
Cassidy
,
Maria
Batuk
,
Pascal
Manuel
,
Emmanuelle
Suard
,
Andrew N.
Fitch
,
Joke
Hadermann
,
Simon J.
Clarke
Diamond Proposal Number(s):
[18786, 25166, 32893, 39378]
Open Access
Abstract: The contrasting crystal and magnetic structures of four related iron oxide chalcogenides are reported. Ae2FeO3CuCh (Ae = Ca, Sr; Ch = S, Se) all crystallize in the Sr2GaO3CuS structure with alkaline earth iron oxide layers containing double layers of linked FeO5 square pyramids containing Fe3+ ions separated by antifluorite-type [Cu2Ch2]2– layers. Structural distortions occur below room temperature when the small Ca2+ ions are present, and these involve cooperative tilting of the FeO5 square pyramids. Magnetic reflections present in the diffraction patterns can be indexed using either √2a × √2a × c or √2a × √2a × 2c expansions of the nuclear cell with nearest-neighbor Fe3+ moments coupling antiferromagnetically and with temperature-dependent orientations relative to the crystallographic directions. The magnetic structures of these compounds are subtly different in detail, partly on account of the low directional preference of the high-spin d5 Fe3+ moments.
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Jun 2026
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I19-Small Molecule Single Crystal Diffraction
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Jakob
Nagl
,
Kirill Yu.
Povarov
,
Benjamin
Duncan
,
Catharina
Näppi
,
Dmitry
Khalyavin
,
Pascal
Manuel
,
Fabio
Orlandi
,
Jeremy
Sourd
,
Beat Valentin
Schwarze
,
Freya
Husstedt
,
Sergei A.
Zvyagin
,
Oksana
Zaharko
,
Paul
Steffens
,
Arno
Hiess
,
David R.
Allan
,
Sarah A.
Barnett
,
Zewu
Yan
,
Severian
Gvasaliya
,
Andrey
Zheludev
Diamond Proposal Number(s):
[39239]
Open Access
Abstract: The prospect of merging the paradigms of geometric frustration on a triangular lattice and bond anisotropies in the strong spin-orbit coupling limit holds tremendous promise in the search for exotic quantum materials. Here we identify a new candidate system to realize such physics, the organic quantum antiferromagnet (CD3ND3)2NaRuCl6. We report a combination of thermodynamic, magneto-elastic and neutron scattering experiments on single-crystals to determine the phase diagram in axial magnetic fields H∥c and propose a minimal model Hamiltonian. (CD3ND3)2NaRuCl6 displays an ideal triangular arrangement of Ru3+ ions adopting the spin-orbital entangled jeff = 1/2 state. It hosts residual magnetic order below TN = 0.23 K and a highly unusual H − T phase diagram including three different incommensurate states. Spin-waves in the high-field polarized regime are described by a Heisenberg triangular lattice Hamiltonian with a potential sub-leading bond dependent anisotropy term J±±. We argue that the multi-q ground state in zero magnetic field is a prime candidate for hosting the
vortex crystal proposed on the triangular Heisenberg-Kitaev model. (CD3ND3)2NaRuCl6 is the first member in an extended family of quantum triangular lattice magnets, providing a new playground to study the interplay of geometric frustration and spin-orbit effects.
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May 2026
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B18-Core EXAFS
I11-High Resolution Powder Diffraction
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James M. A.
Steele
,
Joshua D.
Bocarsly
,
Liam A. V.
Nagle-Cocco
,
George S.
Phillips
,
Farheen N.
Sayed
,
Giulio I.
Lampronti
,
Fabio
Orlandi
,
Pascal
Manuel
,
Iuliia
Mikulska
,
Clare P.
Grey
,
Sian E.
Dutton
Diamond Proposal Number(s):
[34243, 32018]
Open Access
Abstract: NaNiO2 is a promising cathode material for sodium-ion batteries due to its high theoretical capacity of 235.8 mAh.g–1. However, as with many Na-ion cathode materials, a series of poorly understood phase transitions occur on electrochemical cycling, inducing volume mismatch-based stress/strain, resulting in particle cracking, electrochemically disconnected particles and, therefore, irreversible capacity loss. This behavior is one key obstacle to developing long-lasting, high-performance Na-ion batteries. Although the series of phases that form as NaxNiO2 is electrochemically cycled have been previously identified, their structures remained unsolved, limiting our ability to understand and control the phase transition behavior. Here, we report structural solutions based on Rietveld refinement against high-resolution synchrotron x-ray diffraction (SXRD) and neutron powder diffraction (NPD) for the phases obtained on desodiation: P″3-Na1/2NiO2, O″3-Na2/5NiO2, and O‴3-Na1/3NiO2. Each phase contains a unique Na+/vacancy ordering, minimizing intralayer electrostatic repulsions between Na+ ions, and Nix+-charge ordering decreasing interlayer repulsions through the location of lower valence Nix+ nearer to vacancies. Using these structures, we conduct sequential Rietveld refinement against operando SXRD data, which supports prior identification of a transient P‴3-Na1/2<x<2/3NiO2 phase, not isolable ex situ. Operando data also identify the presence of a solid-solution phase O″3δ-Na1/3<x<2/5NiO2 and second-order behavior of the O″3-Na2/5NiO2 → O‴3-Na1/3NiO2 phase transition at the top of charge. This work provides unprecedented insight into structural evolution during electrochemical cycling in Ni-rich Na cathodes (and likely Li analogues), paving the way toward rational doping regimes designed to disrupt degradation-inducing phase transitions, increasing capacity and cycle lifetime, thus improving the performance of Co-free Na and Li cathodes.
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May 2026
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I15-1-X-ray Pair Distribution Function (XPDF)
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Diamond Proposal Number(s):
[38563]
Open Access
Abstract: The development of diverse battery chemistries demands advanced diagnostic techniques to study them. Neutron diffraction, which is sensitive to light elements and capable of distinguishing transition metals with similar electronic configurations, is well-suited to probe crystallographic transformations in battery materials and their degradation pathways. Yet its use has been limited by compromised data quality, low time resolution, and the absence of resource-efficient, reproducible, benchmarked electrochemical cells. Here, using the high-resolution cold-neutron diffractometer WISH, we demonstrate operando neutron diffraction studies of standard laboratory-scale single-layer pouch cells without build modifications, electrolyte deuteration, or isotope enrichment of the electrodes, under practical cycling conditions. This expands the battery diagnostic toolkit beyond X-rays and enables academic exploration of both established and emerging technologies, especially lithium–metal, anode-less, and lithium–sulfur batteries.
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Mar 2026
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I06-Nanoscience (XPEEM)
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Purnima P.
Balakrishnan
,
Hemian
Yi
,
Zi-Jie
Yan
,
Wei
Yuan
,
Andreas
Suter
,
Christopher J.
Jensen
,
Pascal
Manuel
,
Fabio
Orlandi
,
Takayasu
Hanashima
,
Christy J.
Kinane
,
Andrew J.
Caruana
,
Dirk
Backes
,
Padraic
Shafer
,
Brian B.
Maranville
,
Zaher
Salman
,
Thomas
Prokscha
,
Cui-Zu
Chang
,
Alexander J.
Grutter
Diamond Proposal Number(s):
[42224]
Abstract: The search for chiral topological superconductivity in magnetic topological insulator (TI)-FeTe heterostructures is a key frontier in condensed matter physics, with potential applications in topological quantum computing. The combination of ferromagnetism, superconductivity, and topologically nontrivial surface states brings together the key elements required for chiral Majorana physics. In this work, we examine the interplay between magnetism and superconductivity at the interfaces between FeTe and a series of Te-based TI overlayers. In both Te/FeTe and superconducting MnBi2Te4/FeTe, any interfacial suppression of antiferromagnetism must affect at most a few nanometers. On the other hand, (Bi,Sb)2Te3/FeTe layers exhibit near-total suppression of antiferromagnetic ordering. Ferromagnetic Cr𝑥(Bi,Sb)2−𝑥Te3 (CBST)/FeTe bilayers exhibit net magnetization in both CBST and FeTe layers, with evidence of interactions between superconductivity and ferromagnetism. These observations identify magnetic TI/FeTe interfaces as an exceptionally robust platform to realize chiral topological superconductivity.
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Oct 2025
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Rebecca
Scatena
,
Alberto
Hernández-Melián
,
Benjamin M.
Huddart
,
Sam
Curley
,
Robert C.
Williams
,
Pascal
Manuel
,
Stephen J.
Blundell
,
Zurab
Guguchia
,
Zachary E.
Manson
,
Jamie L.
Manson
,
G. Timothy
Noe
,
John
Singleton
,
Tom
Lancaster
,
Paul A.
Goddard
,
Roger D.
Johnson
Open Access
Abstract: We present single-crystal neutron diffraction, powder muon spin rotation, and pulsed-field magnetometry measurements on the Heisenberg quantum chiral chain [Cu(pym)(H2O)4]SiF6·H2O (pym = pyrimidine), which displays a fourfold-periodic rotation of the local environment around the Cu(ii) 𝑆=1/2 ions from site to site along the chain. Previous measurements on this material have shown the absence of magnetic order down to surprisingly low temperatures ≥20 mK, as well as the presence of an energy gap for magnetic excitations that grows linearly with magnetic field. Here we find evidence at dilution refrigerator temperatures for a field-induced transition to long-range magnetic order above an applied magnetic field of 3 T. From the polarization of magnetic moments observed with magnetic fields applied in the [−1,2,0] direction, we can identify the static magnetic structure that best accounts for the data. The proposed model is supported microscopically by the presence of an alternating component of the 𝑔 tensor, which produces an internal twofold staggered field that dictates both the direction of the ordered moments and the effective coupling between adjacent chains. The observed magnetic structure is contrary to previous proposals for the departure of the magnitude and field dependence of the energy gap from the predictions of the sine-Gordon model.
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Aug 2025
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I11-High Resolution Powder Diffraction
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Diamond Proposal Number(s):
[32893]
Open Access
Abstract: Layered transition metal chalcogenides are a versatile class of compounds that exhibit exotic physical phenomena, including superconductivity, thermoelectric properties and magnetic properties. The magnetic properties of ThCr2Si2-type solid solutions KCo2–xNixCh2 (Ch = S, Se; 0 ≤ x ≤ 2) with metallic properties were probed using magnetometry and powder neutron diffraction (PND). KCo2Se2 is ferromagnetic below ∼90 K and powder neutron diffraction (PND) showed evidence for long-range ferromagnetic order with localized moments of 0.6 μB per cobalt ion. With increasing nickel substitution, the system starts to order antiferromagnetically at x = 0.5. In these cases, PND experiments showed long-range A-type antiferromagnetic order with localized moments of around 1 μB per transition metal at 5 K. The Néel temperature (TN) for three-dimensional long-range ordering exhibits a maximum at x = 1, suggesting that nickel substitution enhances the antiferromagnetic interactions along the stacking direction. Higher nickel content suppresses the magnetic ordering temperature, and KCo0.5Ni1.5Se2 shows no magnetic long-range order with a lack of measurable Bragg peaks by PND (although a magnetic transition is evident by magnetometry), and further increasing the nickel content causes the system to become paramagnetic in the region 1.6 ≤ x ≤ 2. Our results show that increasing the electron count in the KCo2–xNixSe2 series has a dramatic effect on the physical properties. The analogous sulfide series - KCo2–xNixS2─shows similar behavior, and the series CsCo2–xNixSe2, containing a larger alkali metal ion, is comparable apart from the lack of a ferromagnetic region at high Co contents in the absence of an applied magnetic field.
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Jul 2025
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