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Register a new userResolving hydrogen atoms at metal-metal hydride interfaces
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Hydrogen as a fuel can be stored safely with high volumetric density in metals. It can, however, also be detrimental to metals causing embrittlement. Understanding fundamental behavior of hydrogen at atomic scale is key to improve the properties of metal-metal hydride systems. However, currently, there is no robust technique capable of visualizing hydrogen atoms. Here, we demonstrate that hydrogen atoms can be imaged unprecedentedly with integrated differential phase contrast, a recently developed technique performed in a scanning transmission electron microscope. Images of the titanium-titanium monohydride interface reveal remarkable stability of the hydride phase, originating from the interplay between compressive stress and interfacial coherence. We also uncovered, thirty years after three models were proposed, which one describes the position of the hydrogen atoms with respect to the interface. Our work enables novel research on hydrides and is extendable to all materials containing light and heavy elements, including oxides, nitrides, carbides and borides.
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The Dzyaloshinskii Moriya Interaction (DMI) at the heavy metal (HM) and ferromagnetic metal (FM) interface has been recognized as a key ingredient in spintronic applications. Here we investigate the chemical trend of DMI on the 5d band filling (5d^3~5d^10) of the HM element in HM/CoFeB/MgO multilayer thin films. DMI is quantitatively evaluated by measuring asymmetric spin wave dispersion using Brillouin light scattering. Sign reversal and 20 times modification of the DMI coefficient D have been measured as the 5d HM element is varied. The chemical trend can be qualitatively understood by considering the 5d and 3d bands alignment at the HM/FM interface and the subsequent orbital hybridization around the Fermi level. Furthermore, a positive correlation is observed between DMI and spin mixing conductance at the HM/FM interfaces. Our results provide new insights into the interfacial DMI for designing future spintronic devices.
Catalyzing capping layers on top of metal hydrides are often employed to enhance the hydrogenation kinetics of metal-hydride based systems such as hydrogen sensors. Here, we experimentally study the hydrogenation kinetics of capping layers composed of several alloys of Pd and Au as well as Pt, Ni and Ru, all with and without an additional PTFE protection layer using a novel method and under the same set of experimental conditions. Our results demonstrate that doping Pd with Au results in significantly faster hydrogenation kinetics, with response times up to five times shorter than Pd through enhanced diffusion and a reduction of the activation energy. The kinetics of non-Pd based materials turns out to be significantly slower and mainly limited by the diffusion through the capping layer itself. Surprisingly, the additional PTFE layer was only found to improve the kinetics of Pd-based capping materials and has no significant effect on the kinetics of Pt, Ni and Ru. Taken together, the experimental results aid in rationally choosing a suitable capping material for the application of metal hydrides and other materials in a green economy. In addition, the developed method can be used to simultaneously study the hydrogenation kinetics and determine diffusion constants in thin film materials for a wide set of experimental conditions.
Large scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. Molybdenum disulfide is one of the most promising alternative catalysts but its intrinsic activity is still inferior to platinum. There is therefore a need to explore new active site origins in molybdenum disulfide with ultrafast reaction kinetics and to understand their mechanisms. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on two-dimensional monolayers. In case of molybdenum disulfide, we design and identify a new type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 35.1 mV dec-1 and a turnover frequency of ~10^3 s-1 at 100 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly-efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.
The band alignment of semiconductor-metal interfaces plays a vital role in modern electronics, but remains difficult to predict theoretically and measure experimentally. For interfaces with strong band bending a main difficulty originates from the in-built potentials which lead to broadened and shifted band spectra in spectroscopy measurements. In this work we present a method to resolve the band alignment of buried semiconductor-metal interfaces using core level photoemission spectroscopy and self-consistent electronic structure simulations. As a proof of principle we apply the method to a clean in-situ grown InAs(100)/Al interface, a system with a strong in-built band bending. Due to the high signal-to-noise ratio of the core level spectra the proposed methodology can be used on previously inaccessible semiconductor-metal interfaces and support targeted design of novel hybrid devices and form the foundation for a interface parameter database for specified synthesis processes of semiconductor-metal systems.
While some of the most elegant applications of topological insulators, such as quantum anomalous Hall effect, require the preservation of Dirac surface states in the presence of time-reversal symmetry breaking, other phenomena such as spin-charge conversion rather rely on the ability for these surface states to imprint their spin texture on adjacent magnetic layers. In this work, we investigate the spin-momentum locking of the surface states of a wide range of monolayer transition metals (3$d$-TM) deposited on top of Bi$_{2}$Se$_{3}$ topological insulators using first principles calculations. We find an anticorrelation between the magnetic moment of the 3$d$-TM and the magnitude of the spin-momentum locking {em induced} by the Dirac surface states. While the magnetic moment is large in the first half of the 3$d$ series, following Hunds rule, the spin-momentum locking is maximum in the second half of the series. We explain this trend as arising from a compromise between intra-atomic magnetic exchange and covalent bonding between the 3$d$-TM overlayer and the Dirac surface states. As a result, while Cr and Mn overlayers can be used successfully for the observation of quantum anomalous Hall effect or the realization of axion insulators, Co and Ni are substantially more efficient for spin-charge conversion effects, e.g. spin-orbit torque and charge pumping.
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