E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[16854]
Abstract: We examine the atomic structure of chemical vapour deposition grown multilayer WS2 pyramids using aberration corrected annular dark field scanning transmission electron microscopy coupled with an in situ heating holder. The stacking orders and specific types of defects after partial degradation by S and W atomic loss at high temperature are resolved layer-by-layer. Our study of an individual WS2 pyramid with at least six layers, reveals a mixed 2H and 3R polytype stacking. Etching occurred both top and bottom of the WS2 pyramid, which aids in determining the exact vertical layer stacking configurations in the thicker regions. We provide an extensive catalogue of the contrast profiles associated with defects in WS2 as a function of layer number and stacking type, as imaged using ADF-STEM. These results provide extensive details about the identification of a wide range of defects in S2 layers, and the unique ADF-STEM contrast patterns that arise from complex multilayer stacking.
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May 2019
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[18627]
Open Access
Abstract: Among the many remarkable properties of diamond, the ability to superconduct when heavily doped with boron has attracted much interest in the carbon community. When considering the nanocrystalline boron doped system, the reduced dimensionality and confinement effects have led to several intriguing observations most notably, signatures of a mixed superconducting phase. Here we present ultra-high-resolution transmission electron microscopy imaging of the grain boundary and demonstrate how the complex microstructure leads to enhanced carrier correlations. We observe hallmark features of spin–orbit coupling (SOC) manifested as the weak anti-localization effect. The enhanced SOC is believed to result from a combination of inversion symmetry breaking at the grain boundary interfaces along with antisymmetric confinement potential between grains, inducing a Rashba-type SOC. From a pronounced zero bias peak in the differential conductance, we demonstrate signatures of a triplet component believed to result from spin mixing caused by tunneling of singlet Cooper pairs through such Rashba-SOC grain boundary junctions.
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Sep 2020
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[16967]
Abstract: Single atom catalysts (SACs) are ideal model systems in catalysis research. Here we employ SACs to address the fundamental catalytic challenge of generating well-defined active metal centers to elucidate their interactions with coordinating atoms, which define their catalytic performance. We introduce a soft-landing molecular strategy for tailored SACs based on metal phthalocyanines (MPcs, M = Ni, Co, Fe) on graphene oxide (GO) layers to generate well-defined model targets for mechanistic studies. The formation of electronic channels through π–π conjugation with the graphene sheets enhances the MPc-GO performance in both oxygen evolution and reduction reactions (OER and ORR). Density functional theory (DFT) calculations unravel that the outstanding ORR activity of FePc-GO among the series is due to the high affinity of Fe atoms toward O2 species. Operando X-ray absorption spectroscopy and DFT studies demonstrate that the OER performance of the catalysts relates to thermodynamic or kinetic control at low- or high-potential ranges, respectively. We furthermore provide evidence that the participation of ligating N and C atoms around the metal centers provides a wider selection of active OER sites for both NiPc-GO and CoPc-GO. Our strategy promotes the understanding of coordination–activity relationships of high-performance SACs and their optimization for different processes through tailored combinations of metal centers and suitable ligand environments.
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Oct 2020
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[26559]
Open Access
Abstract: Single-particle reconstruction can be used to perform three-dimensional (3D) imaging of homogeneous populations of nano-sized objects, in particular viruses and proteins. Here, it is demonstrated that it can also be used to obtain 3D reconstructions of heterogeneous populations of inorganic nanoparticles. An automated acquisition scheme in a scanning transmission electron microscope is used to collect images of thousands of nanoparticles. Particle images are subsequently semi-automatically clustered in terms of their properties and separate 3D reconstructions are performed from selected particle image clusters. The result is a 3D dataset that is representative of the full population. The study demonstrates a methodology that allows 3D imaging and analysis of inorganic nanoparticles in a fully automated manner that is truly representative of large particle populations.
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Nov 2020
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E02-JEM ARM 300CF
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Mathias
Uller Rothmann
,
Judy S.
Kim
,
Juliane
Borchert
,
Kilian B.
Lohmann
,
Colum M.
O'leary
,
Alex A.
Sheader
,
Laura
Clark
,
Henry J.
Snaith
,
Michael B.
Johnston
,
Peter D.
Nellist
,
Laura M.
Herz
Diamond Proposal Number(s):
[21734]
Abstract: Hybrid organic-inorganic perovskites have high potential as materials for solar energy applications, but their microscopic properties are still not well understood. Atomic-resolution scanning transmission electron microscopy has provided invaluable insights for many crystalline solar cell materials, and we used this method to successfully image formamidinium lead triiodide [CH(NH2)2PbI3] thin films with a low dose of electron irradiation. Such images reveal a highly ordered atomic arrangement of sharp grain boundaries and coherent perovskite/PbI2 interfaces, with a striking absence of long-range disorder in the crystal. We found that beam-induced degradation of the perovskite leads to an initial loss of formamidinium [CH(NH2)2+] ions, leaving behind a partially unoccupied perovskite lattice, which explains the unusual regenerative properties of these materials. We further observed aligned point defects and climb-dissociated dislocations. Our findings thus provide an atomic-level understanding of technologically important lead halide perovskites.
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Oct 2020
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[19064]
Abstract: Electromagnetic pulse welding (EMPW) is a promising solid-state joining process, offering fast and strong bonding with no heat affected zone. Despite the growing interest in this process, there is little understanding of the dynamic phenomena that lead to bonding and microstructural changes during EMPW of key engineering materials such as age-hardenable aluminium alloys. This study combines experiments with numerical modelling of plastic deformation to provide an insight to these phenomena in joining of a high-strength aluminium alloy in the T4 and T6 temper conditions. Initially, bonding criteria are postulated in view of the calculated plastic strain at the interface of the T4 sample. These criteria are then used for the prediction of the extent of bonded interfaces for different sets of materials and process parameters. The predictions are shown to be in quantitative agreement with the experimental results for the T6 sample. The corresponding microstructural studies show that bonding is associated with remarkable microstructural changes in the samples, including dissolution of precipitates, formation of high-angle boundaries, and recrystallisation, especially near the bonded interfaces. Moreover, the results of post-weld heat treatments and mechanical testing demonstrate that the impact-induced deformation in EMPW can also influence subsequent precipitations, hence result in improved properties of the entire sample, in a way not achievable by conventional age hardening treatments.
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Nov 2020
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[20527]
Open Access
Abstract: Hybrid metal extrusion & bonding (HYB) is a joining method that enables solid-state bonding by combining addition of aluminium filler material through continuous extrusion with pressure exerted by a rotating steel tool. This work presents mechanical and microstructural characterisation of a second generation HYB butt joint of aluminium alloy 6082 and structural steel S355. The ultimate tensile strength was measured to be in the range of 184–220 MPa, which corresponds to 60–72% joint efficiency. Digital image correlation analysis of the strain development during tensile testing revealed that root cracks formed, before the final fracture ran close to the aluminium-steel interface. A significant amount of residual aluminium was found on the steel fracture surface, especially in regions that experienced higher pressure during joining. Scanning and transmission electron microscopy revealed that the bond strength could be attributed to a combination of microscale mechanical interlocking and a discontinuous nanoscale interfacial Al-Fe-Si intermetallic phase layer. Analysis of scanning electron diffraction data acquired in a tilt series, indicated that the polycrystalline intermetallic phase layer contained the cubic αc phase. The results give insight into the bonding mechanisms of aluminium-steel joints and into the performance of HYB joints, which may be used to better understand and further develop aluminium-steel joining processes.
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Nov 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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E02-JEM ARM 300CF
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Liqi
Zhou
,
Jingdong
Song
,
Judy S.
Kim
,
Xudong
Pei
,
Chen
Huang
,
Mark
Boyce
,
Luiza
Mendonca
,
Daniel
Clare
,
Alistair
Siebert
,
Christopher
Allen
,
Emanuela
Liberti
,
David
Stuart
,
Xiaoqing
Pan
,
Peter
Nellist
,
Peijun
Zhang
,
Angus
Kirkland
,
Peng
Wang
Diamond Proposal Number(s):
[19243, 20431, 20961, 22317]
Open Access
Abstract: Cryo-electron microscopy is an essential tool for high-resolution structural studies of biological systems. This method relies on the use of phase contrast imaging at high defocus to improve information transfer at low spatial frequencies at the expense of higher spatial frequencies. Here we demonstrate that electron ptychography can recover the phase of the specimen with continuous information transfer across a wide range of the spatial frequency spectrum, with improved transfer at lower spatial frequencies, and as such is more efficient for phase recovery than conventional phase contrast imaging. We further show that the method can be used to study frozen-hydrated specimens of rotavirus double-layered particles and HIV-1 virus-like particles under low-dose conditions (5.7 e/Å2) and heterogeneous objects in an Adenovirus-infected cell over large fields of view (1.14 × 1.14 μm), thus making it suitable for studies of many biologically important structures.
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Jun 2020
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E02-JEM ARM 300CF
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Abstract: We show interlayer stacking shifts occur in transition metal dichalcogenides (TMD) bilayers due to the strain introduced during sample heating, and attributed to rippling of one layer relative to the other. The atomic structure of the interlayer stacking is studied using annular dark field scanning transmission electron microscopy with an in situ heating holder. Before heating, bilayers show uniform interlayer stacking of AA′ and AB. When heated, contrast change is seen and associated with interlayer stacking changes at the atomic scale due to ripples. When cooled down to room temperature, these contrast features disappear, confirming it is a reversible process that is not related to defects or vacancies. Because the bottom layer is attached to the in situ heating chip made from Si3N4 and the top layer is in contact with the underlying TMD layer with weak van der Waals interaction, the two layers experience different forces during thermal expansion.
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Jun 2020
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