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The discovery of a novel long-lived metastable skyrmion phase in the multiferroic insulator Cu2 OSeO3 visualized with Lorentz transmission electron microscopy for magnetic fields below the equilibrium skyrmion pocket is reported. This phase can be accessed by exciting the sample non-adiabatically with near-infrared femtosecond laser pulses and cannot be reached by any conventional field-cooling protocol, referred as a hidden phase. From the strong wavelength dependence of the photocreation process and via spin-dynamics simulations, the magnetoelastic effect is identified as the most likely photocreation mechanism. This effect results in a transient modification of the magnetic free energy landscape extending the equilibrium skyrmion pocket to lower magnetic fields. The evolution of the photoinduced phase is monitored for over 15 min and no decay is found. Because such a time is much longer than the duration of any transient effect induced by a laser pulse in a material, it is assumed that the newly discovered skyrmion state is stable for practical purposes, thus breaking ground for a novel approach to control magnetic state on demand at ultrafast timescales and drastically reducing heat dissipation relevant for next-generation spintronic devices.
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Skyrmions are chiral magnetic textures with non-trivial topology, and due to their unique properties they are widely considered as promising information carriers in novel magnetic storage applications. While electric field writing/erasing and manipulation of skyrmions have been recently achieved, quantitative insights into the energetics of those phenomena remain scarce. Here, we report our in situ electric field writing/erasing of skyrmions in magnetoelectric helimagnet Cu2OSeO3 utilizing real-space and real-time Lorentz transmission electron macroscopy. Through the quantitavie analysis on our massive video data, we obtained a linear dependence of the number of skyrmions on the amplitude of the applied electric field, from which a local energy barried to write/erase skyrmions is estimated to be per skyrmion. Such an ultralow energy barrier implies the potential of precise control of skyrmions in future spintronics applications.
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The synthesis and X-ray structural study of the new family of compounds Ba4Fe4ClO9.5-x with tunable structural modulation are reported. The framework of the structure has the Ba2Fe4O9.5-x composition, with open hexagonal channels extending along the c-axis. The channels are filled with linear [Ba-Cl-Ba] triplets. The oxygen stoichiometry and the oxidation state of iron both are controlled by the redox conditions during crystal preparation. The modulation of the crystal structure arises from the distribution of the oxygen atoms in the framework and iron coordination polyhedra are a combination of FeO4-tetrahedra, FeO5-bipyramids, and FeO6-octahedra. The structure modulation also originates from the ordered or disordered distribution of the [Ba-Cl-Ba] triplets filling the channels which is also affected by the conditions of the thermal treatment of the crystals. The structure investigation reveals a composition variation from Ba4Fe4ClO9.5 (x = 0), in which Fe exhibits a 3+ oxidation state, to Ba4Fe4ClO8 (x = 1.5) with the framework built exclusively of FeO4 tetrahedra.
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We present a method to directly visualise a statistical analysis of skyrmion defect alignment at grain boundaries in the skyrmion host [Formula: see text]OSeO3. Using Lorentz transmission electron microscopy, we collected large data sets with several hundreds of frames containing skyrmion lattices with grain boundaries in them. To address the behaviour of strings of dislocations in these grain boundaries, we developed an algorithm to automatically extract and classify strings of dislocations separating the grains. This way we circumvent the problem of having to create configurations with well-defined relative grain orientations by performing a statistical analysis on a dynamically rearranging image sequence. With this statistical method, we are able to experimentally extract the relationship between grain boundary alignment and defect spacing and find an agreement with geometric expectations. The algorithms used can be extended to other types of lattices such as Abrikosov lattices or colloidal systems in optical microscopy.
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Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K_{2}Ni_{2}(SO_{4})_{3} forming a three-dimensional network of Ni^{2+} spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field Bâ³4 T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.
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The crystal structure of Ba5(IO6)2, penta-barium bis-(orthoperiodate), has been re-investigated at room temperature based on single-crystal X-ray diffraction data. In comparison with a previous crystal structure determination by the Rietveld method, an improved precision of the structural parameters was achieved. Additionally, low-temperature measurements allowed the crystal structure evolution to be studied down to 80â K. No evidence of structural transition was found even at the lowest temperature. Upon cooling, the lattice contraction is more pronounced along the b axis. This contraction is found to be inhomogeneous along different crystallographic axes. The inter-atomic distances between different Ba atoms reduce drastically with lowering temperature, resulting in a closer packing around the IO6 octa-hedra, which remain largely unaffected.
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An amendment to this paper has been published and can be accessed via a link at the top of the paper.
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The phase transition most commonly observed is probably melting, a transition from ordered crystalline solids to disordered isotropic liquids. In three dimensions, melting is a single, first-order phase transition. In two-dimensional systems, however, theory predicts a general scenario of two continuous phase transitions separated by an intermediate, oriented liquid state, the so-called hexatic phase with short-range translational and quasi-long-range orientational orders. Such hexatic phases occur in colloidal systems, Wigner solids and liquid crystals, all composed of real-matter particles. In contrast, skyrmions are countable soliton configurations with non-trivial topology and these quasi-particles can form two-dimensional lattices. Here we show, by direct imaging with cryo-Lorentz transmission electron microscopy, that magnetic field variations can tune the phase of the skyrmion ensembles in Cu2OSeO3 from a two-dimensional solid through the long-speculated skyrmion hexatic phase to a liquid. The local spin order persists throughout the process. Remarkably, our quantitative analysis demonstrates that the aforementioned topological-defect-induced crystal melting scenario well describes the observed phase transitions.
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The crystal structure of [ZnCl2(NH3)2], diamminedi-chlorido-zinc, was re-investigated at low temperature, revealing the positions of the hydrogen atoms and thus a deeper insight into the hydrogen-bonding scheme in the crystal packing. In comparison with previous crystal structure determinations [MacGillavry & Bijvoet (1936 â¸). Z. Kristallogr. 94, 249-255; Yamaguchi & Lindqvist (1981 â¸). Acta Chem. Scand. 35, 727-728], an improved precision of the structural parameters was achieved. In the crystal, tetra-hedral [Zn(NH3)2Cl2] units (point-group symmetry mm2) are linked through N-Hâ¯Cl hydrogen bonds into a three-dimensional network.
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The nature of the dynamics and structural changes that take place at the ferroelectric phase transition in lead oxides is a rich field of study. Solid-state nuclear magnetic resonance (NMR) of 207Pb is well suited to study the local structure and disorder in lead oxide ferroelectric transitions at the atomic level. However, very large 207Pb shielding anisotropy results in poor resolution in 1D static and magic angle spinning (MAS) NMR spectra. We address this problem by using short high-power adiabatic pulses (SHAPs) with magic-angle-turning sequences to correlate the isotropic and anisotropic parts of the 207Pb chemical shift tensor in a 2D NMR experiment, yielding resolved 207Pb NMR spectra of the nine distinct lead sites in uniaxial ferroelectric lead germanate (Pb5Ge3O11). Using this technique we detect the magnetic environments of displaced Pb2+ ions and unambiguously identify the nature of the phase transition as mixed displacive and order-disorder. We also observe that the atomic-level process responsible for the phase transition in ferroelectric lead germanate is chemical exchange on the kilohertz timescale. We derive an activation energy of 103.4 ± 1.7 kJ mol-1 and compare it to dielectric spectroscopy studies on similar materials. These results show that this method can be used to characterize ferroelectric phase transitions of complex materials with high resolution using nuclei that are typically inaccessible due to their large shielding anisotropy.
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The semimetal MoTe_{2} is studied by spin- and angle-resolved photoemission spectroscopy across the centrosymmetry-breaking structural transition temperature of the bulk. A three-dimensional spin-texture is observed in the bulk Fermi surface in the low temperature, noncentrosymmetric phase that is consistent with first-principles calculations. The spin texture and two types of surface Fermi arc are not completely suppressed above the bulk transition temperature. The lifetimes of quasiparticles forming the Fermi arcs depend on thermal history and lengthen considerably upon cooling toward the bulk structural transition. The results indicate that a new form of polar instability exists near the surface when the bulk is largely in a centrosymmetric phase.
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Exploiting additional degrees of freedom in solid-state materials may be the most-promising solution when approaching the quantum limit of Moore's law for the conventional electronic industry. Recently discovered topologically nontrivial spin textures, skyrmions, are outstanding among such possibilities. However, the controlled creation of skyrmions, especially by electric means, remains a pivotal challenge in technological applications. Here, we report that skyrmions can be created locally via electric field in the magnetoelectric helimagnet Cu2OSeO3. Using Lorentz transmission electron microscopy, we successfully write skyrmions in situ from a helical-spin background. Our discovery is highly coveted because it implies that skyrmionics can be integrated into modern field effect transistor based electronic technology, in which very low energy dissipation can be achieved and, hence, realize a large step forward toward its practical applications.
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A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.
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Junctions between n-type semiconductors of different electron affinity show rectification if the junction is abrupt enough. With the advent of 2D materials, we are able to realize thin van der Waals (vdW) heterostructures based on a large diversity of materials. In parallel, strongly correlated functional oxides have emerged, having the ability to show reversible insulator-to-metal (IMT) phase transition by collapsing their electronic bandgap under a certain external stimulus. Here, we report for the first time the electronic and optoelectronic characterization of ultra-thin n-n heterojunctions fabricated using deterministic assembly of multilayer molybdenum disulphide (MoS2) on a phase transition material, vanadium dioxide (VO2). The vdW MoS2/VO2 heterojunction combines the excellent blocking capability of an n-n junction with a high conductivity in on-state, and it can be turned into a Schottky rectifier at high applied voltage or at temperatures higher than 68 °C, exploiting the metal state of VO2. We report tunable diode-like current rectification with a good diode ideality factor of 1.75 and excellent conductance swing of 120 mV/dec. Finally, we demonstrate unique tunable photosensitivity and excellent junction photoresponse in the 500/650 nm wavelength range.
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Carbon nanotubes (CTNs) with large aspect-ratios are extensively used to establish electrical connectedness in polymer melts at very low CNT loadings. However, the CNT size polydispersity and the quality of the dispersion are still not fully understood factors that can substantially alter the desired characteristics of CNT nanocomposites. Here we demonstrate that the electrical conductivity of polydisperse CNT-epoxy composites with purposely-tailored distributions of the nanotube length L is a quasiuniversal function of the first moment of L. This finding challenges the current understanding that the conductivity depends upon higher moments of the CNT length. We explain the observed quasiuniversality by a combined effect between the particle size polydispersity and clustering. This mechanism can be exploited to achieve controlled tuning of the electrical transport in general CNT nanocomposites.
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The manipulation of the electronic properties of solids by light is an exciting goal, which requires knowledge of the electronic structure with energy, momentum and temporal resolution. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) is the most direct probe of the effects of an optical excitation on the band structure of a material. In particular, tr-ARPES in the extreme ultraviolet (VUV) range gives access to the ultrafast dynamics over the entire Brillouin zone. VUV tr-ARPES experiments can now be performed at the ASTRA (ARPES Spectrometer for Time-Resolved Applications) end station of Harmonium, at LACUS. Its capabilities are illustrated by measurements of the ultrafast electronic response of ZrSiTe, a novel topological semimetal characterized by linearly dispersing states located at the Brillouin zone boundary.
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Despite the rapid increase in the performance of perovskite solar cells (PSC), they still suffer from low lab-to-lab or people-to-people reproducibility. Aiming for a universal condition to high-performance devices, we investigated the morphology evolution of a composite perovskite by tuning annealing temperature and precursor concentration of the perovskite film. Here, we introduce thermal annealing as a powerful tool to generate a well-controlled excess of PbI2 in the perovskite formulation and show that this benefits the photovoltaic performance. We demonstrated the correlation between the film microstructure and electronic property and device performance. An optimized average grain size/thickness aspect ratio of the perovskite crystallite is identified, which brings about a highly reproducible power conversion efficiency (PCE) of 19.5 %, with a certified value of 19.08 %. Negligible hysteresis and outstanding morphology stability are observed with these devices. These findings lay the foundation for further boosting the PCE of PSC and can be very instructive for fabrication of high-quality perovskite films for a variety of applications, such as light-emitting diodes, field-effect transistors, and photodetectors.
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Compuestos de Calcio/química , Suministros de Energía Eléctrica , Ingeniería , Óxidos/química , Energía Solar , Titanio/química , Temperatura , Transistores ElectrónicosRESUMEN
Perovskite alkaline niobates, due to their strong nonlinear optical properties, including birefringence and the capability to produce second-harmonic generation (SHG) signals, attract a lot of attention as potential candidates for applications as local nano/microsized mechano-optical probes. Here, we report on an implementation of photonic force microscopy (PFM) to explore the Brownian motion and optical trappability of monocrystalline potassium niobate (KNbO3) nano/microsized particles having sizes within the range of 50 to 750 nm. In particular, we exploit the anisotropic translational diffusive regime of the Brownian motion to quantify thermal fluctuations and optical forces of singly-trapped KNbO3 particles within the optical trapping volume of a PFM microscope. We also show that, under near-infrared (NIR) excitation of the highly focused laser beam of the PFM microscope, a single optically-trapped KNbO3 particle reveals a strong SHG signal manifested by a narrow peak (λ(em) = 532 nm) at half the excitation wavelength (λ(ex) = 1064 nm). Moreover, we demonstrate that the thus induced SHG emission can be used as a local light source that is capable of optically exciting molecules of an organic dye, Rose Bengal (RB), which adhere to the particle surface, through the mechanism of luminescence energy transfer (LET).
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Magnetic skyrmions are promising candidates as information carriers in logic or storage devices thanks to their robustness, guaranteed by the topological protection, and their nanometric size. Currently, little is known about the influence of parameters such as disorder, defects, or external stimuli on the long-range spatial distribution and temporal evolution of the skyrmion lattice. Here, using a large (7.3 × 7.3 µm(2)) single-crystal nanoslice (150 nm thick) of Cu2OSeO3, we image up to 70,000 skyrmions by means of cryo-Lorentz transmission electron microscopy as a function of the applied magnetic field. The emergence of the skyrmion lattice from the helimagnetic phase is monitored, revealing the existence of a glassy skyrmion phase at the phase transition field, where patches of an octagonally distorted skyrmion lattice are also discovered. In the skyrmion phase, dislocations are shown to cause the emergence and switching between domains with different lattice orientations, and the temporal fluctuation of these domains is filmed. These results demonstrate the importance of direct-space and real-time imaging of skyrmion domains for addressing both their long-range topology and stability.