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Rongsheng Cai

Publications and source records attributed to Rongsheng Cai.

8 recordsLinked to original sources

Moiré-induced lattice reconstruction at buried atomic interfaces

Atomic reconstruction at twisted two-dimensional interfaces governs many of their emergent optical, electronic, and mechanical properties, including sliding ferroelectricity. Despite recent progress in understanding lattice reconstruction in suspended twisted bilayers, structural changes at van der Waals heterointerfaces between multilayer crystals remain largely unexplored. Here we use multi-slice electron ptychography to non-invasively recover the three-dimensional atomic structure at marginally twisted rhombohedral interfaces between thick transition-metal dichalcogenide crystals. With a position precision of ~3 pm and a depth resolution ~1 nm, we resolve the twist-induced lattice reconstruction field per layer, and the resulting dislocation network at the buried interface. Despite the bulk nature, we observe markedly strong in-plane interfacial reconstruction due to suppression of the out-of-plane bending by outer layers, exceeding predictions from our three-dimensional modelling. Furthermore, we extract the strain tensor evolution during the decay of the reconstruction into the bulk, providing a structural foundation for understanding multi-layer moiré systems.

cond-mat.mes-hall

Atomic-resolution imaging of gold species at organic liquid-solid interfaces

Understanding solid-liquid interfaces at the atomic-scale is key to improved performance of heterogeneous catalysts, electrodes and membranes. Here we combine unique specimen design, record atomic resolution in situ electron microscopy, and artificial intelligence-enabled analysis to achieve a step change in quantitative understanding of interfacial atomic behaviour. We create the first graphene liquid cells with organic solvents and employ them to track over 106 gold adatoms and clusters at a graphene surface immersed in acetone and cyclohexanone. We reveal dynamic correlated behaviour of gold adatom monomers, dimers, trimers and clusters, strongly influenced by each other, the solvent properties, and the atomic lattice of the substrate, in good agreement with theoretical calculations. We use the results to interpret differences in catalytic activity towards the industrially important acetylene hydrochlorination reaction. This new capability for exploration of atomic scale chemistry could enable rational design of future catalysts, membranes and electrodes with improved functionality.

cond-mat.mtrl-sci

Noise2Void for Denoising Atomic Resolution Scanning Transmission Electron Microscopy Images

The Noise2Void technique is demonstrated for successful denoising of atomic-resolution scanning transmission electron microscopy (STEM) images. The technique is applied to denoising atomic resolution images and videos of gold adatoms on a graphene surface within a graphene liquid cell, with the denoised experimental data qualitatively demonstrating improved visibility of both the Au adatoms and the graphene lattice. The denoising performance is quantified by comparison to similar simulated data and the approach is found to significantly outperform both total variation and simple Gaussian blurring. Compared to other denoising methods, the Noise2Void technique has the combined advantages that it requires no manual intervention during training or denoising, no prior knowledge of the sample and is compatible with real time data acquisition rates of at least 45 frames per second.

cond-mat.mtrl-sci

Phase engineering of 1T$'$ and 1T CrS2 and Cr2S3 by MOCVD

Layered Cr-chalcogenides compounds offer a rich range of crystal phases with different magnetic properties some of which have been predicted only but not experimentally verified. Here we demonstrate a previously unreported crystal phase of CrS2, namely the distorted octahedral (1T$'$) structure, synthesized via metal-organic chemical vapour deposition (MOCVD). We achieved the tuneable synthesis of either 1T$'$ or 1T phase CrS2. The structure were identified using polarized Raman spectroscopy, density functional perturbation theory (DFPT), as well as scanning electron diffraction (4D-STEM). 4D-STEM reveals that 1T$'$ crystals grow from an originally nucleated kinetically favoured 1T phase which then transform into the thermodynamically stable 1T$'$ phase. Magneto-optic Kerr imaging reveals that the 1T$'$ CrS2 crystals have soft ferromagnetic nature at low temperature. Our MOCVD growth of complex phases of 2D CrS2 with long-range magnetic order paves the way for the scalable synthesis of 2D magnets for ultrathin magnetic memories for logic-in-memory applications and spintronics.

cond-mat.mtrl-sci

Dynamics of single Au nanoparticles on graphene simultaneously in real- and diffraction space by time-series convergent beam electron diffraction

Convergent beam electron diffraction (CBED) on two-dimensional materials allows simultaneous recording of the real-space image (tens of nanometers in size) and diffraction pattern of the same sample in one single-shot intensity measurement. In this study, we employ time-series CBED to visualize single Au nanoparticles deposited on graphene. The real-space image of the probed region, with the amount, size, and positions of single Au nanoparticles, is directly observed in the zero-order CBED disk, while the atomic arrangement of the Au nanoparticles is available from the intensity distributions in the higher-order CBED disks. From the time-series CBED patterns, the movement of a single Au nanoparticle with rotation up to 4° was recorded. We also observed facet diffraction lines - intense bright lines formed between the CBED disks of the Au nanoparticle, which we explain by diffraction at the Au nanoparticle's facets. This work showcases CBED as a useful technique for studying adsorbates on graphene using Au nanoparticles as a model platform, and paves the way for future studies of different objects deposited on graphene.

cond-mat.other

Highly ${ }^{28} \mathrm{Si}$ Enriched Silicon by Localised Focused Ion Beam Implantation

Solid-state spin qubits within silicon crystals at mK temperatures show great promise in the realisation of a fully scalable quantum computation platform. Qubit coherence times are limited in natural silicon owing to coupling to the isotope ${ }^{29} \mathrm{Si}$ which has a non-zero nuclear spin. This work presents a method for the depletion of ${ }^{29} \mathrm{Si}$ in localised volumes of natural silicon wafers by irradiation using a 45 keV ${ }^{28} \mathrm{Si}$ focused ion beam with fluences above $1 \times 10^{19} \, \mathrm{ions} \, \mathrm{cm}^{-2}$. Nanoscale secondary ion mass spectrometry analysis of the irradiated volumes shows unprecedented quality enriched silicon that reaches a minimal residual ${ }^{29} \mathrm{Si}$ value of 2.3 $\pm$ 0.7 ppm and with residual C and O comparable to the background concentration in the unimplanted wafer. Transmission electron microscopy lattice images confirm the solid phase epitaxial re-crystallization of the as-implanted amorphous enriched volume extending over 200 nm in depth upon annealing. The ease of fabrication, requiring only commercially available natural silicon wafers and ion sources, opens the possibility for co-integration of qubits in localised highly enriched volumes with control circuitry in the surrounding natural silicon for large-scale devices.

cond-mat.mtrl-sci

Doped graphene/carbon black hybrid catalyst giving enhanced oxygen reduction reaction activity with high resistance to corrosion in proton exchange membrane fuel cells

Nitrogen doping of the carbon is an important method to improve the performance and durability of catalysts for proton exchange membrane fuel cells by platinum-nitrogen and carbon-nitrogen bonds. This study shows that p-phenyl groups and graphitic N acting bridges linking platinum and the graphene/carbon black (the ratio graphene/carbon black=2/3) hybrid support materials achieved the average size of platinum nanoparticles with (4.88 +/- 1.79) nm. It improved the performance of the lower-temperature hydrogen fuel cell up to 0.934 W cm-2 at 0.60 V, which is 1.55 times greater than that of commercial Pt/C. Doping also enhanced the interaction between Pt and the support materials, and the resistance to corrosion, thus improving the durability of the low-temperature hydrogen fuel cell with a much lower decay of 10 mV at 0.80 A cm-2 after 30k cycles of an in-situ accelerated stress test of catalyst degradation than that of 92 mV in Pt/C, which achieves the target of Department of Energy (<30 mV). Meanwhile, Pt/NrEGO2-CB3 remains 78% of initial power density at 1.5 A cm-2 after 5k cycles of in-situ accelerated stress test of carbon corrosion, which is more stable than the power density of commercial Pt/C, keeping only 54% after accelerated stress test.

physics.app-ph

Oleylamine aging of PtNi nanoparticles giving enhanced functionality for the oxygen reduction reaction

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 co-reduction 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 2-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).

cond-mat.mtrl-sci