E02-JEM ARM 300CF
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Dengyang
Guo
,
Thomas A.
Selby
,
Simon
Kahmann
,
Sebastian
Gorgon
,
Linjie
Dai
,
Milos
Dubajic
,
Terry
Chien-Jen Yang
,
Simon M.
Fairclough
,
Thomas
Marsh
,
Ian E.
Jacobs
,
Baohu
Wu
,
Renjun
Guo
,
Satyawan
Nagane
,
Tiarnan A. S.
Doherty
,
Kangyu
Ji
,
Cheng
Liu
,
Yang
Lu
,
Taeheon
Kang
,
Capucine
Mamak
,
Jian
Mao
,
Peter
Muller-Buschbaum
,
Henning
Sirringhaus
,
Paul A.
Midgley
,
Samuel D.
Stranks
Diamond Proposal Number(s):
[35894]
Open Access
Abstract: The high optoelectronic quality of halide perovskites makes them suitable for use in optoelectronic devices and, recently, in emerging quantum emission applications. Advancements in perovskite nanomaterials have led to the discovery of processes in which luminescence decay times are below 100 picoseconds, stimulating the exploration of even faster radiative rates for advanced quantum applications, which have only been realized in III–V materials grown using costly epitaxial growth methods. Here we discovered ultrafast quantum transients with timescales of around two picoseconds at low temperature in bulk formamidinium lead iodide films grown via scalable solution or vapour approaches. Using a multimodal strategy, combining ultrafast spectroscopy, optical and electron microscopy, we show that these transients originate from quantum tunnelling in nanodomain superlattices. The outcome of the transient decays, that is, photoluminescence, mirrors the photoabsorption of the states, with an ultranarrow linewidth at low temperature that can reach <2 nm (~4 meV). Localized correlation of the emission and structure reveals that the nanodomain superlattices are formed by alternating ordered layers of corner-sharing and face-sharing octahedra. This discovery opens new applications leveraging intrinsic quantum properties and demonstrates powerful multimodal approaches for quantum investigations.
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Oct 2025
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I13-2-Diamond Manchester Imaging
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Xuekun
Lu
,
Rhodri
Owen
,
Wenjia
Du
,
Zhenyu
Zhang
,
Antonio
Bertei
,
Roby
Soni
,
Xun
Zhang
,
Francesco
Iacoviello
,
Daqing
Li
,
Alice
Llewellyn
,
Jianuo
Chen
,
Han
Zhang
,
Xuhui
Yao
,
Qi
Li
,
Yunlong
Zhao
,
Shashidhara
Marathe
,
Christoph
Rau
,
Paul R.
Shearing
Diamond Proposal Number(s):
[29068]
Open Access
Abstract: Silicon is a promising negative electrode material for high-energy batteries, but its volume changes during cell cycling cause rapid degradation, limiting its loading to about 10 wt.% in conventional graphite/Si composite electrodes. Overcoming this threshold requires evidence-based design for the formulation of advanced electrodes. Here we combine multimodal operando imaging techniques, assisted by structural and electrochemical characterizations, to elucidate the multiscale electro-chemo-mechanical processes in graphite/Si composite negative electrodes. We demonstrate that the electrochemical cycling stability of Si particles strongly depends on the design of intraparticle nanoscale porous structures, and the encapsulation and loss of active Si particles result in excessive charging current being directed to the graphite particles, increasing the risk of lithium plating. We also show that heterogeneous strains are present between graphite and Si particles, in the carbon-binder domain and the electrode’s porous structures. Focusing on the volume expansion of the electrode during electrochemical cycling, we prove that the rate performance and Si utilization are heavily influenced by the expansion of the carbon-binder domain and the decrease in porosity. Based on this acquired knowledge, we propose a tailored double-layer graphite/Si composite electrode design that exhibits lower polarization and capacity decay compared with conventional graphite/Si electrode formulations.
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Oct 2025
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I19-Small Molecule Single Crystal Diffraction
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Milos
Dubajic
,
James R.
Neilson
,
Johan
Klarbring
,
Xia
Liang
,
Stephanie A.
Bird
,
Kirrily C.
Rule
,
Josie E.
Auckett
,
Thomas A.
Selby
,
Ganbaatar
Tumen-Ulzii
,
Yang
Lu
,
Young-Kwang
Jung
,
Cullen
Chosy
,
Zimu
Wei
,
Yorrick
Boeije
,
Martin V.
Zimmermann
,
Andreas
Pusch
,
Leilei
Gu
,
Xuguang
Jia
,
Qiyuan
Wu
,
Julia C.
Trowbridge
,
Eve M.
Mozur
,
Arianna
Minelli
,
Nikolaj
Roth
,
Kieran W. P.
Orr
,
Arman
Mahboubi Soufiani
,
Simon
Kahmann
,
Irina
Kabakova
,
Jianning
Ding
,
Tom
Wu
,
Gavin J.
Conibeer
,
Stephen P.
Bremner
,
Michael P.
Nielsen
,
Aron
Walsh
,
Samuel D.
Stranks
Diamond Proposal Number(s):
[33123]
Open Access
Abstract: Lead halide perovskites have emerged as promising materials for solar energy conversion and X-ray detection owing to their remarkable optoelectronic properties. However, the microscopic origins of their superior performance remain unclear. Here we show that low-symmetry dynamic nanodomains present in the high-symmetry average cubic phases, whose characteristics are dictated by the A-site cation, govern the macroscopic behaviour. We combine X-ray diffuse scattering, inelastic neutron spectroscopy, hyperspectral photoluminescence microscopy and machine-learning-assisted molecular dynamics simulations to directly correlate local nanoscale dynamics with macroscopic optoelectronic response. Our approach reveals that methylammonium-based perovskites form densely packed, anisotropic dynamic nanodomains with out-of-phase octahedral tilting, whereas formamidinium-based systems develop sparse, isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains present in formamidinium-based systems reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of formamidinium-based lead halide perovskite devices. By elucidating the influence of the A-site cation on local dynamic nanodomains, and consequently, on the macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics and X-ray imaging.
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Jun 2025
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I06-Nanoscience (XPEEM)
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O. J.
Amin
,
S. F.
Poole
,
S.
Reimers
,
L. X.
Barton
,
A.
Dal Din
,
F.
Maccherozzi
,
S. S.
Dhesi
,
V.
Novák
,
F.
Krizek
,
J. S.
Chauhan
,
R. P.
Campion
,
A. W.
Rushforth
,
T.
Jungwirth
,
O. A.
Tretiakov
,
K. W.
Edmonds
,
P.
Wadley
Diamond Proposal Number(s):
[26255, 27845]
Open Access
Abstract: Topologically protected magnetic textures are promising candidates for information carriers in future memory devices, as they can be efficiently propelled at very high velocities using current-induced spin torques. These textures—nanoscale whirls in the magnetic order—include skyrmions, half-skyrmions (merons) and their antiparticles. Antiferromagnets have been shown to host versions of these textures that have high potential for terahertz dynamics, deflection-free motion and improved size scaling due to the absence of stray field. Here we show that topological spin textures, merons and antimerons, can be generated at room temperature and reversibly moved using electrical pulses in thin-film CuMnAs, a semimetallic antiferromagnet that is a testbed system for spintronic applications. The merons and antimerons are localized on 180° domain walls, and move in the direction of the current pulses. The electrical generation and manipulation of antiferromagnetic merons is a crucial step towards realizing the full potential of antiferromagnetic thin films as active components in high-density, high-speed magnetic memory devices.
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May 2023
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I19-Small Molecule Single Crystal Diffraction
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Haofan
Yang
,
Chao
Li
,
Tao
Liu
,
Thomas
Fellowes
,
Samantha Y.
Chong
,
Luca
Catalano
,
Mounib
Bahri
,
Weiwei
Zhang
,
Yongjie
Xu
,
Lunjie
Liu
,
Wei
Zhao
,
Adrian M.
Gardner
,
Rob
Clowes
,
Nigel D.
Browning
,
Xiaobo
Li
,
Alexander J.
Cowan
,
Andrew I.
Cooper
Abstract: Molecular packing controls optoelectronic properties in organic molecular nanomaterials. Here we report a donor–acceptor organic molecule (2,6-bis(4-cyanophenyl)-4-(9-phenyl-9H-carbazol-3-yl)pyridine-3,5-dicarbonitrile) that exhibits two aggregate states in aqueous dispersions: amorphous nanospheres and ordered nanofibres with π–π molecular stacking. The nanofibres promote sacrificial photocatalytic H2 production (31.85 mmol g−1 h−1) while the nanospheres produce hydrogen peroxide (H2O2) (3.20 mmol g−1 h−1 in the presence of O2). This is the first example of an organic photocatalyst that can be directed to produce these two different solar fuels simply by changing the molecular packing. These different packings affect energy band levels, the extent of excited state delocalization, the excited state dynamics, charge transfer to O2 and the light absorption profile. We use a combination of structural and photophysical measurements to understand how this influences photocatalytic selectivity. This illustrates the potential to achieve multiple photocatalytic functionalities with a single organic molecule by engineering nanomorphology and solid-state packing.
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Jan 2023
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I14-Hard X-ray Nanoprobe
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Kyle
Frohna
,
Miguel
Anaya
,
Stuart
Macpherson
,
Jooyoung
Sung
,
Tiarnan A. S.
Doherty
,
Yu-Hsien
Chiang
,
Andrew J.
Winchester
,
Kieran W. P.
Orr
,
Julia E.
Parker
,
Paul D.
Quinn
,
Keshav M.
Dani
,
Akshay
Rao
,
Samuel D.
Stranks
Diamond Proposal Number(s):
[19023, 20420]
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.
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Nov 2021
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E02-JEM ARM 300CF
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Astrid
Weston
,
Yichao
Zou
,
Vladimir
Enaldiev
,
Alex
Summerfield
,
Nicholas
Clark
,
Viktor
Zólyomi
,
Abigail
Graham
,
Celal
Yelgel
,
Samuel
Magorrian
,
Mingwei
Zhou
,
Johanna
Zultak
,
David
Hopkinson
,
Alexei
Barinov
,
Thomas H.
Bointon
,
Andrey
Kretinin
,
Neil R.
Wilson
,
Peter H.
Beton
,
Vladimir I.
Fal’ko
,
Sarah J.
Haigh
,
Roman
Gorbachev
Diamond Proposal Number(s):
[19315, 21597]
Abstract: Van der Waals heterostructures form a unique class of layered artificial solids in which physical properties can be manipulated through controlled composition, order and relative rotation of adjacent atomic planes. Here we use atomic-resolution transmission electron microscopy to reveal the lattice reconstruction in twisted bilayers of the transition metal dichalcogenides, MoS2 and WS2. For twisted 3R bilayers, a tessellated pattern of mirror-reflected triangular 3R domains emerges, separated by a network of partial dislocations for twist angles θ < 2°. The electronic properties of these 3R domains, featuring layer-polarized conduction-band states caused by lack of both inversion and mirror symmetry, appear to be qualitatively different from those of 2H transition metal dichalcogenides. For twisted 2H bilayers, stable 2H domains dominate, with nuclei of a second metastable phase. This appears as a kagome-like pattern at θ ≈ 2°, transitioning at θ → 0 to a hexagonal array of screw dislocations separating large-area 2H domains. Tunnelling measurements show that such reconstruction creates strong piezoelectric textures, opening a new avenue for engineering of 2D material properties.
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May 2020
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Katharina
Zeissler
,
Simone
Finizio
,
Kowsar
Shahbazi
,
Jamie
Massey
,
Fatma Al
Ma’mari
,
David M.
Bracher
,
Armin
Kleibert
,
Mark C.
Rosamond
,
Edmund H.
Linfield
,
Thomas A.
Moore
,
Jörg
Raabe
,
Gavin
Burnell
,
Christopher H.
Marrows
Abstract: Magnetic skyrmions are knot-like quasiparticles. They are candidates for non-volatile data storage in which information is moved between fixed read and write terminals. The read-out operation of skyrmion-based spintronic devices will rely on the electrical detection of a single magnetic skyrmion within a nanostructure. Here we present Pt/Co/Ir nanodiscs that support skyrmions at room temperature. We measured the Hall resistivity and simultaneously imaged the spin texture using magnetic scanning transmission X-ray microscopy. The Hall resistivity is correlated to both the presence and size of the skyrmion. The size-dependent part matches the expected anomalous Hall signal when averaging the magnetization over the entire disc. We observed a resistivity contribution that only depends on the number and sign of skyrmion-like objects present in the disc. Each skyrmion gives rise to 22 ± 2 nΩ cm irrespective of its size. This contribution needs to be considered in all-electrical detection schemes applied to skyrmion-based devices. Not only the area of Néel skyrmions but also their number and sign contribute to their Hall resistivity.
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Oct 2018
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E02-JEM ARM 300CF
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Zupeng
Chen
,
Evgeniya
Vorobyeva
,
Sharon
Mitchell
,
Edvin
Fako
,
Manuel A.
Ortuño
,
Núria
López
,
Sean M.
Collins
,
Paul A.
Midgley
,
Sylvia
Richard
,
Gianvito
Vilé
,
Javier
Pérez-Ramírez
Diamond Proposal Number(s):
[16967]
Abstract: Palladium-catalysed cross-coupling reactions, central tools in fine-chemical synthesis, predominantly employ soluble metal complexes despite recognized challenges with product purification and catalyst reusability. Attempts to tether these homogeneous catalysts on insoluble carriers have been thwarted by suboptimal stability, which leads to a progressively worsening performance due to metal leaching or clustering4. The alternative application of supported Pd nanoparticles has faced limitations because of insufficient activity under the mild conditions required to avoid thermal degradation of the substrates or products. Single-atom heterogeneous catalysts lie at the frontier. Here, we show that the Pd atoms anchored on exfoliated graphitic carbon nitride (Pd-ECN) capture the advantages of both worlds, as they comprise a solid catalyst that matches the high chemoselectivity and broad functional group tolerance of state-of-the-art homogeneous catalysts for Suzuki couplings, and also demonstrate a robust stability in flow. The adaptive coordination environment within the macroheterocycles of ECN facilitates each catalytic step. The findings illustrate the exciting opportunities presented by nanostructuring single atoms in solid hosts for catalytic processes that remain difficult to heterogenize.
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Jun 2018
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I06-Nanoscience (XPEEM)
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Peter
Wadley
,
Sonka
Reimers
,
Michal J.
Grzybowski
,
Carl
Andrews
,
Mu
Wang
,
Jasbinder S.
Chauhan
,
Bryan L.
Gallagher
,
Richard P.
Campion
,
Kevin W.
Edmonds
,
Sarnjeet S.
Dhesi
,
Francesco
Maccherozzi
,
Vit
Novak
,
Joerg
Wunderlich
,
Tomas
Jungwirth
Diamond Proposal Number(s):
[16376]
Abstract: Antiferromagnets have several favourable properties as active elements in spintronic devices, including ultra-fast dynamics, zero stray fields and insensitivity to external magnetic fields1. Tetragonal CuMnAs is a testbed system in which the antiferromagnetic order parameter can be switched reversibly at ambient conditions using electrical currents2. In previous experiments, orthogonal in-plane current pulses were used to induce 90° rotations of antiferromagnetic domains and demonstrate the operation of all-electrical memory bits in a multi-terminal geometry3. Here, we demonstrate that antiferromagnetic domain walls can be manipulated to realize stable and reproducible domain changes using only two electrical contacts. This is achieved by using the polarity of the current to switch the sign of the current-induced effective field acting on the antiferromagnetic sublattices. The resulting reversible domain and domain wall reconfigurations are imaged using X-ray magnetic linear dichroism microscopy, and can also be detected electrically. Switching by domain-wall motion can occur at much lower current densities than those needed for coherent domain switching.
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Mar 2018
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