I09-Surface and Interface Structural Analysis
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Diamond Proposal Number(s):
[35796]
Open Access
Abstract: Two-dimensional (2D) transition metal dichalcogenides have emerged as a promising platform for next-generation optoelectronic and spintronic devices. Mechanical exfoliation using adhesive tape remains the dominant method for preparing 2D materials of highest quality, including transition metal dichalcogenides, but always results in small-sized flakes. This limitation poses a significant challenge for investigations and applications where large scale flakes are needed. To overcome these constraints, we explored the preparation of 2D
WS
2
and
WSe
2
using a recently developed kinetic in situ single-layer synthesis method (KISS). In particular, we focused on the influence of different substrates, Au and Ag, and chalcogen atoms, S and Se, on the yield and quality of the 2D films. The crystallinity and spatial morphology of the 2D films were characterized using optical microscopy and atomic force microscopy, providing a comprehensive assessment of exfoliation quality. Low-energy electron diffraction verified that there is no preferential orientation between the 2D film and the substrate, while optical microscopy revealed that
WSe
2
consistently outperformed
WS
2
in producing large monolayers, regardless of the substrate used. Finally, X-ray diffraction and X-ray photoelectron spectroscopy demonstrate that no covalent bonds are formed between the 2D material and the underlying substrate. These results identify KISS method as a non-destructive method for a more scalable approach of high-quality 2D transition metal dichalcogenides.
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May 2025
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I06-Nanoscience (XPEEM)
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Diamond Proposal Number(s):
[27482]
Open Access
Abstract: We present a spectroscopic study of the magnetic properties of Fe3-δGeTe2 single crystals with varying Fe content, achieved by tuning the stoichiometry of the crystals. We carried out x-ray absorption spectroscopy and analyzed the x-ray circular magnetic dichroism spectra using the sum rules, to determine the orbital and spin magnetic moments of the materials. We find a clear reduction of the spin and orbital magnetic moment with increasing Fe deficiency. Magnetic susceptibility measurements show that the reduction in magnetization is accompanied by a reduced Curie temperature. Multiplet calculations reveal that the Fe2+ state increasingly mixes with a higher valence state when the Fe deficiency is increased. This effect is correlated with the weakening of the magnetic moment. As single crystals are the base material for exfoliation processes, our results are relevant for the assembly of 2D magnetic heterostructures.
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Jul 2024
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I14-Hard X-ray Nanoprobe
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Lucas Atila
Bernardes Marcal
,
Nils
Lamers
,
Susanna
Hammarberg
,
Zhaojun
Zhang
,
Huaiyu
Chen
,
Dmitry
Dzhigaev
,
Miguel
Gomez-Gonzalez
,
Julia
Parker
,
Alexander
Bjorling
,
Anders
Mikkelsen
,
Jesper
Wallentin
Diamond Proposal Number(s):
[25924]
Open Access
Abstract: Over the last years metal halide perovskites have demonstrated remarkable potential for integration in light emitting devices. Heterostructures allow for tunable bandgap depending on the local anion composition, crucial for optoelectronic devices, but local structural effects of anion exchange in single crystals is not fully understood. Here, we investigate how the anion exchange of CsPbBr3 nanowires fully and locally exposed to HCl vapor affects the local crystal structure, using nanofocused x-rays. We study the nanoscale composition and crystal structure as function of HCl exposure time and demonstrate the correlation of anion exchange with changes in the lattice parameter. The local composition was measured by x-ray fluorescence and x-ray diffraction, with general agreement of both methods but with much less variation using latter. The heterostructured nanowires exhibit unintentional gradients in composition, both axially and radially. Ferroelastic domains are observed for all HCl exposure times, and the magnitude of the lattice tilt decreases for higher Cl concentrations.
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Mar 2024
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B18-Core EXAFS
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Diamond Proposal Number(s):
[15151]
Abstract: Various techniques were employed to prepare a dual support system of CeZrO2 and H-ZSM-5 (80) including physically mixing, co-precipitation and sonochemical methods, which were followed by the deposition of bimetallic Pd and Pt via wet impregnation to obtain the final catalysts. The catalysts were tested in the total methane oxidation between 200 and 500 °C and the most active is the material derived from sonochemical synthesis. This catalyst achieved a remarkable methane conversion of 84% at a low temperature of 300 °C and high Gas Hourly Space Velocity (GHSV) of 100000 ml g−1 h−1. Characterisation using x-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), scanning electron microscope (SEM), scanning transmission electron microscope (STEM), Energy-dispersive x-ray spectroscopy (EDS), temperature-programmed reduction (TPR) and x-ray absorption fine structure (XAFS) techniques revealed the intimate distribution of catalyst components and facile redox behaviour of both Pd and CeZrO2 components. The catalysts based on sonochemical CeZrO2 was proven to be relatively stable with only 7% methane conversion loss after 50 h continuously on stream at 300 °C compared to the corresponding 14% witnessed with the commercial TiO2-based material.
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Aug 2023
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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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I10-Beamline for Advanced Dichroism - scattering
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Diamond Proposal Number(s):
[21872, 27487]
Open Access
Abstract: The topological surface states (TSSs) in topological insulators (TIs) offer exciting prospects for dissipationless spin transport. Common spin-based devices, such as spin valves, rely on trilayer structures in which a non-magnetic (NM) layer is sandwiched between two ferromagnetic (FM) layers. The major disadvantage of using high-quality single-crystalline TI films in this context is that a single pair of spin-momentum locked channels spans across the entire film, meaning that only a very small spin current can be pumped from one FM to the other, along the side walls of the film. On the other hand, using nanocrystalline TI films, in which the grains are large enough to avoid hybridization of the TSSs, will effectively increase the number of spin channels available for spin pumping. Here, we used an element-selective, x-ray based ferromagnetic resonance technique to demonstrate spin pumping from a FM layer at resonance through the TI layer and into the FM spin sink.
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Mar 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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Ian
Vidamour
,
Matthew O. A.
Ellis
,
David
Griffin
,
Guru
Venkat
,
Charles
Swindells
,
Richard W. S.
Dawidek
,
Thomas J
Broomhall
,
Nina-Juliane
Steinke
,
Joshaniel
Cooper
,
Francesco
Maccherozzi
,
Sarnjeet
Dhesi
,
Susan
Stepney
,
Eleni
Vasilaki
,
Dan A.
Allwood
,
Tom James
Hayward
Open Access
Abstract: Devices based on arrays of interconnected magnetic nano-rings with emergent magnetization dynamics have recently been proposed for use in reservoir computing applications, but for them to be computationally useful it must be possible to optimise their dynamical responses. Here, we use a phenomenological model to demonstrate that such reservoirs can be optimised for classification tasks by tuning hyperparameters that control the scaling and input-rate of data into the system using rotating magnetic fields. We use task-independent metrics to assess the rings' computational capabilities at each set of these hyperparameters and show how these metrics correlate directly to performance in spoken and written digit recognition tasks. We then show that these metrics, and performance in tasks, can be further improved by expanding the reservoir's output to include multiple, concurrent measures of the ring arrays' magnetic states.
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Aug 2022
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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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William
Liu
,
Salida
Mirzoeva
,
Ye
Yuan
,
Junjing
Deng
,
Si
Chen
,
Barry
Lai
,
Stefan
Vogt
,
Karna
Shah
,
Rahul
Shroff
,
Reiner
Bleher
,
Qiaoling
Jin
,
Nghia
Vo
,
Remon
Bazak
,
Carissa
Ritner
,
Stanley
Gutionov
,
Sumita
Raha
,
Julia
Sedlmair
,
Carol
Hirschmugl
,
Chris
Jacobsen
,
Tatjana
Paunesku
,
John
Kalapurkal
,
Gayle E.
Woloschak
Open Access
Abstract: Background: Neuroblastoma is the most common extracranial solid malignancy in childhood which, despite the current progress in radiotherapy and chemotherapy protocols, still has a high mortality rate in high risk tumors. Nanomedicine offers excit- ing and unexploited opportunities to overcome the shortcomings of conventional medicine. The photocatalytic properties of Fe O core-TiO shell nanocomposites and
3 4 2
their potential for cell specific targeting suggest that nanoconstructs produced using
Fe3O4 core-TiO2 shell nanocomposites could be used to enhance radiation effects in neuroblastoma. In this study, we evaluated bare, metaiodobenzylguanidine (MIBG) and 3,4-Dihydroxyphenylacetic acid (DOPAC) coated Fe3O4@TiO2 as potential radiosensitiz- ers for neuroblastoma in vitro.
Results: The uptake of bare and MIBG coated nanocomposites modestly sensitized neuroblastoma cells to ionizing radiation. Conversely, cells exposed to DOPAC coated nanocomposites exhibited a five-fold enhanced sensitivity to radiation, increased numbers of radiation induced DNA double-strand breaks, and apoptotic cell death. The addition of a peptide mimic of the epidermal growth factor (EGF) to nanoconju- gates coated with MIBG altered their intracellular distribution. Cryo X-ray fluorescence microscopy tomography of frozen hydrated cells treated with these nanoconjugates revealed cytoplasmic as well as nuclear distribution of the nanoconstructs.
Conclusions: The intracellular distribution pattern of different nanoconjugates used in this study was different for different nanoconjugate surface molecules. Cells exposed to DOPAC covered nanoconjugates showed the smallest nanoconjugate uptake,
with the most prominent pattern of large intracellular aggregates. Interestingly, cells treated with this nanoconjugate also showed the most pronounced radiosensitiza- tion effect in combination with the external beam x-ray irradiation. Further studies
are necessary to evaluate mechanistic basis for this increased radiosensitization effect. Preliminary studies with the nanoparticles carrying an EGF mimicking peptide showed.
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May 2021
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