E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[22549]
Abstract: Monolayer PtSe2 holds great potential in extending 2D devices functionality, but their atomic-level-defect study is still limited. Here, we investigate the atomic structures of lattice imperfections from point to stretched 1D defects in 1T-PtSe2 monolayers, using annular dark-field scanning transmission electron microscopy (ADF-STEM). We show Se vacancies (VSe) have preferential sites with high beam-induced mobility. Diverse divacancies form with paired VSe. We found stretched linear defects triggered by dynamics of VSe that altered strain fields, distinct from the line vacancies in 2H-phase 2D materials. The paired VSe stability and formation possibility of vacancy lines are evaluated by density functional theory. Lower sputtering energy in PtSe2 than that in MoS2 can cause larger possibility of atomic loss compared to diffusion required for creating VSe lines. This provides atomic insights into the defects in 1T-PtSe2 and shows how a deviated 1D structure is embedded in a 2D system without losing atom lines.
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Apr 2022
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B18-Core EXAFS
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Diamond Proposal Number(s):
[14239]
Abstract: Terbium-doped YVO4 has been considered a nonluminescent solid since the first classic studies on rare-earth-doped phosphors in the 1960s. However, we demonstrate that defect engineering of YVO4:Tb3+ nanoparticles overcomes the metal–metal charge transfer (MMCT) process which is responsible for the quenching of the Tb3+ luminescence. Tetragonal (Y1–xTbx)VO4 nanoparticles obtained by colloidal precipitation showed expanded unit cells, high defect densities, and intimately mixed carbonates and hydroxides, which contribute to a shift of the MMCT states to higher energies. Consequently, we demonstrate unambiguously for the first time that Tb3+ luminescence can be excited by VO43– → Tb3+ energy transfer and by direct population of the 5D4 state in YVO4. We also discuss how thermal treatment removes these effects and shifts the quenching MMCT state to lower energies, thus highlighting the major consequences of defect density and microstructure in nanosized phosphors. Therefore, our findings ultimately show nanostructured YVO4:Tb3+ can be reclassified as a UV-excitable luminescent material.
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Apr 2022
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I10-Beamline for Advanced Dichroism
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Diamond Proposal Number(s):
[26148]
Open Access
Abstract: A major challenge in topological magnetism lies in the three-dimensional (3D) exploration of their magnetic textures. A recent focus has been the question of how 2D skyrmion sheets vertically stack to form distinct types of 3D topological strings. Being able to manipulate the vertical coupling should therefore provide a route to the engineering of topological states. Here, we present a new type of axially bound magnetic skyrmion string state in which the strings in two distinct materials are glued together across their interface. With quasi-tomographic resonant elastic X-ray scattering, the 3D skyrmion profiles before and after their binding across the interface were unambiguously determined and compared. Their attractive binding is accompanied by repulsive twisting; i.e., the coupled skyrmions mutually affect each other via a compensating twisting. This state exists in chiral magnet–magnetic thin film heterostructures, providing a new arena for the engineering of 3D topological phases.
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Apr 2022
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I10-Beamline for Advanced Dichroism
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Maciej
Dabrowski
,
Jade N.
Scott
,
William R.
Hendren
,
Colin M.
Forbes
,
Andreas
Frisk
,
David
Burn
,
David G.
Newman
,
Connor R. J.
Sait
,
Paul S.
Keatley
,
Alpha T.
N'Diaye
,
Thorsten
Hesjedal
,
Gerrit
Van Der Laan
,
Robert
Bowman
,
Robert J.
Hicken
Diamond Proposal Number(s):
[17745, 19116, 20760]
Abstract: All-optical switching of magnetization has great potential for use in future ultrafast and energy efficient nanoscale magnetic storage devices. So far, research has been almost exclusively focused on rare-earth based materials, which limits device tunability and scalability. Here, we show that a perpendicularly magnetized synthetic ferrimagnet composed of two distinct transition metal ferromagnetic layers, Ni3Pt and Co, can exhibit helicity independent magnetization switching. Switching occurs between two equivalent remanent states with antiparallel alignment of the Ni3Pt and Co magnetic moments and is observable over a broad temperature range. Time-resolved measurements indicate that the switching is driven by a spin-polarized current passing through the subnanometer Ir interlayer. The magnetic properties of this model system may be tuned continuously via subnanoscale changes in the constituent layer thicknesses as well as growth conditions, allowing the underlying mechanisms to be elucidated and paving the way to a new class of data storage devices.
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Oct 2021
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Abstract: Structural polymorphism is known for many bulk materials; however, on the nanoscale metastable polymorphs tend to form more readily than in the bulk, and with more structural variety. One such metastable polymorph observed for colloidal Ag2Se nanocrystals has traditionally been referred to as the “tetragonal” phase. While there are reports on the chemistry and properties of this metastable polymorph, its crystal structure, and therefore electronic structure, has yet to be determined. We report that an anti-PbCl2-like structure type (space group P21/n) more accurately describes the powder X-ray diffraction and X-ray total scattering patterns of colloidal Ag2Se nanocrystals prepared by several different methods. Density functional theory (DFT) calculations indicate that this anti-PbCl2-like Ag2Se polymorph is a dynamically stable, narrow-band-gap semiconductor. The anti-PbCl2-like structure of Ag2Se is a low-lying metastable polymorph at 5–25 meV/atom above the ground state, depending on the exchange-correlation functional used.
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Jul 2021
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I12-JEEP: Joint Engineering, Environmental and Processing
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Chi Ming
Yim
,
Soumendra Nath
Panja
,
Christopher
Trainer
,
Craig
Topping
,
Christoph
Heil
,
Alexandra S.
Gibbs
,
Oxana
Magdysyuk
,
Vladimir
Tsurkan
,
Alois
Loidl
,
Andreas W.
Rost
,
Peter
Wahl
Diamond Proposal Number(s):
[22974]
Open Access
Abstract: A key property of many quantum materials is that their ground state depends sensitively on small changes of an external tuning parameter, e.g., doping, magnetic field, or pressure, creating opportunities for potential technological applications. Here, we explore tuning of the ground state of the nonsuperconducting parent compound, Fe1+xTe, of the iron chalcogenides by uniaxial strain. Iron telluride exhibits a peculiar (π, 0) antiferromagnetic order unlike the (π, π) order observed in the Fe-pnictide superconductors. The (π, 0) order is accompanied by a significant monoclinic distortion. We explore tuning of the ground state by uniaxial strain combined with low-temperature scanning tunneling microscopy. We demonstrate that, indeed under strain, the surface of Fe1.1Te undergoes a transition to a (π, π)-charge-ordered state. Comparison with transport experiments on uniaxially strained samples shows that this is a surface phase, demonstrating the opportunities afforded by 2D correlated phases stabilized near surfaces and interfaces.
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Apr 2021
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Gerard M.
Leteba
,
Yi-Chi
Wang
,
Thomas J. A.
Slater
,
Rongsheng
Cai
,
Conor
Byrne
,
Christopher P.
Race
,
David R. G.
Mitchell
,
Pieter B. J.
Levecque
,
Neil P.
Young
,
Stuart M.
Holmes
,
Alex
Walton
,
Angus I.
Kirkland
,
Sarah J.
Haigh
,
Candace I.
Lang
Open Access
Abstract: We report a rapid solution-phase strategy to synthesize alloyed PtNi nanoparticles which demonstrate outstanding functionality for the oxygen reduction reaction (ORR). This one-pot coreduction colloidal synthesis results in a monodisperse population of single-crystal nanoparticles of rhombic dodecahedral morphology with Pt-enriched edges and compositions close to Pt1Ni2. We use nanoscale 3D compositional analysis to reveal for the first time that oleylamine (OAm)-aging of the rhombic dodecahedral Pt1Ni2 particles results in Ni leaching from surface facets, producing aged particles with concave faceting, an exceptionally high surface area, and a composition of Pt2Ni1. We show that the modified atomic nanostructures catalytically outperform the original PtNi rhombic dodecahedral particles by more than two-fold and also yield improved cycling durability. Their functionality for the ORR far exceeds commercially available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific activities (up to a 25-fold increase) and intrinsic area-specific activities (up to a 27-fold increase).
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Apr 2021
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I04-1-Macromolecular Crystallography (fixed wavelength)
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Alistair P.
Curd
,
Joanna
Leng
,
Ruth E.
Hughes
,
Alexa J.
Cleasby
,
Brendan
Rogers
,
Chi H.
Trinh
,
Michelle A.
Baird
,
Yasuharu
Takagi
,
Christian
Tiede
,
Christian
Sieben
,
Suliana
Manley
,
Thomas
Schlichthaerle
,
Ralf
Jungmann
,
Jonas
Ries
,
Hari
Shroff
,
Michelle
Peckham
Diamond Proposal Number(s):
[15378]
Abstract: Inferring the organization of fluorescently labeled nanosized structures from single molecule localization microscopy (SMLM) data, typically obscured by stochastic noise and background, remains challenging. To overcome this, we developed a method to extract high-resolution ordered features from SMLM data that requires only a low fraction of targets to be localized with high precision. First, experimentally measured localizations are analyzed to produce relative position distributions (RPDs). Next, model RPDs are constructed using hypotheses of how the molecule is organized. Finally, a statistical comparison is used to select the most likely model. This approach allows pattern recognition at sub-1% detection efficiencies for target molecules, in large and heterogeneous samples and in 2D and 3D data sets. As a proof-of-concept, we infer ultrastructure of Nup107 within the nuclear pore, DNA origami structures, and α-actinin-2 within the cardiomyocyte Z-disc and assess the quality of images of centrioles to improve the averaged single-particle reconstruction.
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Nov 2020
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[19315, 21597]
Abstract: Suspended specimens of 2D crystals and their heterostructures are required for a range of studies including transmission electron microscopy (TEM), optical transmission experiments and nanomechanical testing. However, investigating the properties of laterally small 2D crystal specimens, including twisted bilayers and air sensitive materials, has been held back by the difficulty of fabricating the necessary clean suspended samples. Here we present a scalable solution which allows clean free-standing specimens to be realized with 100% yield by dry-stamping atomically thin 2D stacks onto a specially developed adhesion-enhanced support grid. Using this new capability, we demonstrate atomic resolution imaging of defect structures in atomically thin CrBr3, a novel magnetic material which degrades in ambient conditions.
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Aug 2020
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E02-JEM ARM 300CF
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Jonas
Bekaert
,
Ekaterina
Khestanova
,
David G.
Hopkinson
,
John
Birkbeck
,
Nick
Clark
,
Mengjian
Zhu
,
Denis
Bandurin
,
Roman
Gorbachev
,
Simon
Fairclough
,
Yichao
Zou
,
Matthew
Hamer
,
Daniel J.
Terry
,
Jonathan J. P.
Peters
,
Ana M.
Sanchez
,
Bart
Partoens
,
Sarah
Haigh
,
Milorad
Milosevic
,
Irina V.
Grigorieva
Diamond Proposal Number(s):
[19315, 21597]
Abstract: When approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional materials. While defects are generally thought to negatively affect superconductivity in 2D materials, here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS2). Our first-principles calculations show that incorporation of oxygen into the TaS2 crystal lattice is energetically favourable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the electronic band structure and the carrier density to the intrinsic characteristics of TaS2. Strikingly, this leads to a strong enhancement of the electron-phonon coupling, by up to 80% in the highly-oxygenated limit. Using transport measurements on fresh and aged (oxygenated) few-layer TaS2, we found a marked increase of the superconducting critical temperature (Tc) upon aging, in agreement with our theory, while concurrent electron microscopy and electron-energy loss spectroscopy confirmed the presence of sulfur vacancies in freshly prepared TaS2 and incorporation of oxygen into the crystal lattice with time. Our work thus reveals the mechanism by which certain atomic-scale defects can be beneficial to superconductivity and opens a new route to engineer Tc in ultrathin materials.
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Apr 2020
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