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In situ transmission electron microscope (TEM) characterization techniques provide valuable information on structure-property correlations to understand the behavior of materials at the nanoscale. However, understanding nanoscale structures and their interaction with the electron beam is pivotal for the reliable interpretation of in situ/ex situ TEM studies. Here, we report that oxides commonly used in nanoelectronic applications, such as transistor gate oxides or memristive devices, are prone to electron beam induced damage that causes small structural changes even under very low dose conditions, eventually changing their electrical properties as examined via in situ measurements. In this work, silicon, titanium, and niobium oxide thin films are used for in situ TEM electrical characterization studies. The electron beam induced reduction of the oxides turns these insulators into conductors. The conductivity change is reversible by exposure to air, supporting the idea of electron beam reduction of oxides as primary damage mechanism. Through these measurements we propose a limit for the critical dose to be considered for in situ scanning electron microscopy and TEM characterization studies.
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A highly sophisticated pulsed laser deposition (PLD) chamber has recently been installed at the NANO beamline at the synchrotron facility ANKA (Karlsruhe, Germany), which allows for comprehensive studies on the PLD growth process of dielectric, ferroelectric and ferromagnetic thin films in epitaxial oxide heterostructures or even multilayer systems by combining inâ situ reflective high-energy diffraction with the inâ situ synchrotron high-resolution X-ray diffraction and surface diffraction methods. The modularity of the inâ situ PLD chamber offers the opportunity to explore the microstructure of the grown thin films as a function of the substrate temperature, gas pressure, laser fluence and target-substrate separation distance. Ba0.5Sr0.5TiO3 grown on MgO represents the first system that is grown in this inâ situ PLD chamber and studied by inâ situ X-ray reflectivity, inâ situ two-dimensional reciprocal space mapping of symmetric X-ray diffraction and acquisition of time-resolved diffraction profiles during the ablation process. In situ PLD synchrotron investigation has revealed the occurrence of structural distortion as well as domain formation and misfit dislocation which all depend strongly on the film thickness. The microstructure transformation has been accurately detected with a time resolution of 1â s. The acquisition of two-dimensional reciprocal space maps during the PLD growth has the advantage of simultaneously monitoring the changes of the crystalline structure as well as the formation of defects. The stability of the morphology during the PLD growth is demonstrated to be remarkably affected by the film thickness. A critical thickness for the domain formation in Ba0.5Sr0.5TiO3 grown on MgO could be determined from the acquisition of time-resolved diffraction profiles during the PLD growth. A splitting of the diffraction peak into two distinguishable peaks has revealed a morphology change due to modification of the internal strain during growth.
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The chiral anomaly - a hallmark of chiral spin-1/2 Weyl fermions - is an imbalance between left- and right-moving particles that underpins phenomena such as particle decay and negative longitudinal magnetoresistance in Weyl semimetals. The discovery that chiral crystals can host higher-spin generalizations of Weyl quasiparticles without high-energy counterparts, known as multifold fermions, raises the fundamental question of whether the chiral anomaly is a more general phenomenon. Answering this question requires materials with chiral quasiparticles within a sizable energy window around the Fermi level that are unaffected by extrinsic effects such as current jetting. Here, we report the chiral anomaly of multifold fermions in CoSi, which features multifold bands within ~0.85 eV of the Fermi level. By excluding current jetting through the squeezing test, we measure an intrinsic, longitudinal negative magnetoresistance. We develop a semiclassical theory to show that the negative magnetoresistance originates in the chiral anomaly, despite a sizable and detrimental orbital magnetic moment contribution. A concomitant non-linear Hall effect supports the multifold-fermion origin of the magnetotransport. Our work confirms the chiral anomaly of higher-spin generalizations of Weyl fermions, currently inaccessible outside solid-state platforms.
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Semiconductor transistors operate by modulating the charge carrier concentration of a channel material through an electric field coupled by a capacitor. This mechanism is constrained by the fundamental transport physics and material properties of such devices-attenuation of the electric field, and limited mobility and charge carrier density in semiconductor channels. In this work, we demonstrate a new type of transistor that operates through a different mechanism. The channel material is a Weyl semimetal, NbP, whose resistivity is modulated via a magnetic field generated by an integrated superconductor. Due to the exceptionally large electron mobility of this material, which reaches over 1,000,000 cm2/Vs, and the strong magnetoresistive coupling, the transistor can generate significant transconductance amplification at nanowatt levels of power. This type of device can enable new low-power amplifiers, suitable for qubit readout operation in quantum computers.
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In recent times the chiral semimetal cobalt monosilicide (CoSi) has emerged as a prototypical, nearly ideal topological conductor hosting giant, topologically protected Fermi arcs. Exotic topological quantum properties have already been identified in CoSi bulk single crystals. However, CoSi is also known for being prone to intrinsic disorder and inhomogeneities, which, despite topological protection, risk jeopardizing its topological transport features. Alternatively, topology may be stabilized by disorder, suggesting the tantalizing possibility of an amorphous variant of a topological metal, yet to be discovered. In this respect, understanding how microstructure and stoichiometry affect magnetotransport properties is of pivotal importance, particularly in case of low-dimensional CoSi thin films and devices. Here we comprehensively investigate the magnetotransport and magnetic properties of ≈25 nm Co1-xSix thin films grown on a MgO substrate with controlled film microstructure (amorphous vs textured) and chemical composition (0.40 < x < 0.60). The resistivity of Co1-xSix thin films is nearly insensitive to the film microstructure and displays a progressive evolution from metallic-like (dρxx/dT > 0) to semiconducting-like (dρxx/dT < 0) regimes of conduction upon increasing the silicon content. A variety of anomalies in the magnetotransport properties, comprising for instance signatures consistent with quantum localization and electron-electron interactions, anomalous Hall and Kondo effects, and the occurrence of magnetic exchange interactions, are attributable to the prominent influence of intrinsic structural and chemical disorder. Our systematic survey brings to attention the complexity and the challenges involved in the prospective exploitation of the topological chiral semimetal CoSi in nanoscale thin films and devices.
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Owing to electric-field screening, the modification of magnetic properties in ferromagnetic metals by applying small voltages is restricted to a few atomic layers at the surface of metals. Bulk metallic systems usually do not exhibit any magneto-electric effect. Here, we report that the magnetic properties of micron-scale ferromagnetic metals can be modulated substantially through electrochemically-controlled insertion and extraction of hydrogen atoms in metal structure. By applying voltages of only ~ 1 V, we show that the coercivity of micrometer-sized SmCo5, as a bulk model material, can be reversibly adjusted by ~ 1 T, two orders of magnitudes larger than previously reported. Moreover, voltage-assisted magnetization reversal is demonstrated at room temperature. Our study opens up a way to control the magnetic properties in ferromagnetic metals beyond the electric-field screening length, paving its way towards practical use in magneto-electric actuation and voltage-assisted magnetic storage.
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Ferroelectric oxide memristors are currently in the highlights of a thriving area of research aiming at the development of nonvolatile, adaptive memories for applications in neuromorphic computing. However, to date a precise control of synapse-like functionalities by adjusting the interplay between ferroelectric polarization and resistive switching processes is still an ongoing challenge. Here, it is shown that by means of controlled electron beam radiation, a prototypical ferroelectric film of BaTiO3 can be turned into a memristor with multiple configurable resistance states. Ex situ and in situ analyses of current/voltage characteristics upon electron beam exposure confirm the quasi-continuous variation of BaTiO3 resistance up to two orders of magnitude under the typical experimental conditions employed in electron beam patterning and characterization techniques. These results demonstrate an unprecedented effective route to locally and scalably engineering multilevel ferroelectric memristors via application of moderate electron beam radiation.
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The control of magnetism by means of low-power electric fields, rather than dissipative flowing currents, has the potential to revolutionize conventional methods of data storage and processing, sensing, and actuation. A promising strategy relies on the utilization of magnetoelectric composites to finely tune the interplay between electric and magnetic degrees of freedom at the interface of two functional materials. Albeit early works predominantly focused on the magnetoelectric coupling at solid/solid interfaces; however, recently there has been an increased interest related to the opportunities offered by liquid-gating techniques. Here, a comparative overview on voltage control of magnetism in all-solid-state and solid/liquid composites is presented within the context of the principal coupling mediators, i.e., strain, charge carrier doping, and ionic intercalation. Further, an exhaustive and critical discussion is carried out, concerning the suitability of using the common definition of coupling coefficient α C = Δ M Δ E to compare the strength of the interaction between electricity and magnetism among different magnetoelectric systems.
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The ever-growing technological demand for more advanced microelectronic and spintronic devices keeps catalyzing the idea of controlling magnetism with an electric field. Although voltage-driven on/off switching of magnetization is already established in some magnetoelectric (ME) systems, often the coupling between magnetic and electric order parameters lacks an adequate reversibility, energy efficiency, working temperature, or switching speed. Here, the ME performance of a manganite supercapacitor composed of a ferromagnetic, spin-polarized ultrathin film of La0.74 Sr0.26 MnO3 (LSMO) electrically charged with an ionic liquid electrolyte is investigated. Fully reversible, rapid, on/off switching of ferromagnetism in LSMO is demonstrated in combination with a shift in Curie temperature of up to 26 K and a giant ME coupling coefficient of ≈226 Oe V-1 . The application of voltages of only ≈2 V results in ultralow energy consumptions of about 90 µJ cm-2 . This work provides a step forward toward low-power, high-endurance electrical switching of magnetism for the development of high-performance ME spintronics.
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Chemical doping via insertion of ions into the lattice of a host material is a key strategy to flexibly manipulate functionalities of materials. In this work, we present a novel case study on the topotactic insertion of fluoride ions into oxygen-deficient ferromagnetic thin films of La0.74Sr0.26MnO3-δ (LSMO) epitaxially grown onto single-crystal SrTiO3 (STO) substrates. The effect of fluorination on the film structure, composition, and magnetic properties is compared with the case of oxygen-deficient and fully-oxidized LSMO films. Although incorporation of F- anions does not significantly alter the volume of the LSMO unit cell, a strong impact on the magnetic characteristics, including a remarkable suppression of Curie temperature and saturation magnetization accompanied by an increase in magnetic coercivity, was found. The change in magnetic properties can be ascribed to the disruption of the ferromagnetic exchange interactions along Mn-anion-Mn chains driven by F- doping into the LSMO lattice. Our results indicate that F- doping is a powerful means to effectively modify the magnetic functional properties of perovskite manganites.
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Electric field tuning of magnetism is one of the most intensely pursued research topics of recent times aiming at the development of new-generation low-power spintronics and microelectronics. However, a reversible magnetoelectric effect with an on/off ratio suitable for easy and precise device operation is yet to be achieved. Here we propose a novel route to robustly tune magnetism via the charging/discharging processes of hybrid supercapacitors, which involve electrostatic (electric-double-layer capacitance) and electrochemical (pseudocapacitance) doping. We use both charging mechanisms-occurring at the La0.74Sr0.26MnO3/ionic liquid interface to control the balance between ferromagnetic and non-ferromagnetic phases of La1-xSrxMnO3 to an unprecedented extent. A magnetic modulation of up to ≈33% is reached above room temperature when applying an external potential of only about 2.0 V. Our case study intends to draw attention to new, reversible physico-chemical phenomena in the rather unexplored area of magnetoelectric supercapacitors.
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Reduction of the operating temperature to an intermediate temperature range between 350 °C and 600 °C is a necessity for Solid Oxide Fuel/Electrolysis Cells (SOFC/SOECs). In this respect the application of proton-conducting oxides has become a broad area of research. Materials that can conduct protons and electrons at the same time, to be used as electrode catalysts on the air electrode, are especially rare. In this article we report on the proton conduction in expitaxially grown BaFeO2.5+δ (BFO) thin films deposited by pulsed laser deposition on Nb:SrTiO3 substrates. By using Electrochemical Impedance Spectroscopy (EIS) measurements under different wet and dry atmospheres, the bulk proton conductivity of BFO (between 200 °C and 300 °C) could be estimated for the first time (3.6 × 10-6 S cm-1 at 300 °C). The influence of oxidizing measurement atmosphere and hydration revealed a strong dependence of the conductivity, most notably at temperatures above 300 °C, which is in good agreement with the hydration behavior of BaFeO2.5 reported previously.
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Scleractinian corals are a major source of biogenic calcium carbonate, yet the relationship between their skeletal microstructure and mechanical properties has been scarcely studied. In this work, the skeletons of two coral species:solitary Balanophyllia europaea and colonial Stylophora pistillata, were investigated by nanoindentation. The hardness HIT and Young's modulus E(IT) were determined from the analysis of several load-depth data on two perpendicular sections of the skeletons: longitudinal (parallel to the main growth axis) and transverse. Within the experimental and statistical uncertainty,the average values of the mechanical parameters are independent on the section's orientation. The hydration state of the skeletons did not affect the mechanical properties. The measured values, EIT in the 76-77 GPa range, and H(IT) in the 4.95.1 GPa range, are close to the ones expected for polycrystalline pure aragonite. Notably, a small difference in H(IT) is observed between the species. Different from corals, single-crystal aragonite and the nacreous layer of the seashell Atrina rigida exhibit clearly orientation-dependent mechanical properties. The homogeneous and isotropic mechanical behaviour of the coral skeletons at the microscale is correlated with the microstructure,observed by electron microscopy and atomic force microscopy, and with the X-ray diffraction patterns of the longitudinal and transverse sections.