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Magnesium hydride has great potential as a solid hydrogen (H) storage material because of its high H storage capacity of 7.6 wt%. However, its slow hydrogenation and dehydrogenation kinetics and the high temperature of 300 ∘C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH2is an important fundamental knowledge in solving this problem, which has been studied mainly based on density functional theory (DFT). However, few experimental studies have been performed to assess the results of DFT calculations. We have therefore introduced muon (Mu) as pseudo-H into MgH2and investigated the corresponding interstitial H states by analyzing their electronic and dynamical properties in detail. As a result, we observed multiple Mu states similar to those observed in wide-gap oxides, and found that their electronic states can be attributed to relaxed-excited states associated with donor/acceptor levels predicted by the recently proposed 'ambipolarity model'. This provides an indirect support for the DFT calculations on which the model is based via the donor/acceptor levels. An important implication of the muon results for improved hydrogen kinetics is that dehydrogenation, serving as areductionfor hydrides, stabilises the interstitial H-state.
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Semimetallic osmium pyrochlore oxide Cd2Os2O7undergoes a magnetic transition to an all-in-all-out (AIAO)-type order at 227 K, followed by a crossover to an AIAO insulator at around 210 K. Here, we studied the isostructural and isoelectronic compound Hg2Os2O7through thermodynamic measurements, muon spin rotation (µSR) spectroscopy and neutron diffraction experiments. A similar magnetic transition, probably to an AIAO-type order, was observed at 88 K, while the resistivity showed a decrease at the transition and remained metallic down to 2 K. Thus, the ground state of Hg2Os2O7is most likely an AIAO semimetal, which is analogous to the intermediate-temperature state of Cd2Os2O7. Hg2Os2O7exists on the verge of the metal-insulator boundary on the metal side and provides an excellent platform for studying the electronic instability of 5delectrons with moderate electron correlations and strong spin-orbit interactions.
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The long charge carrier lifetime of the hybrid organic-inorganic perovskites (HOIPs) is the key for their remarkable performance as a solar cell material. The microscopic mechanism for the long lifetime is still in debate. Here, by using a muon spin relaxation technique that probes the fluctuation of local magnetic fields, we show that the muon depolarization rate (Δ) of a prototype HOIP methylammonium lead iodide (MAPbI3) shows a sharp decrease with increasing temperature in two steps above 120 K and 190 K across the structural transition from orthorhombic to tetragonal structure at 162 K. Our analysis shows that the reduction of Δ is quantitatively in agreement with the expected behavior due to the rapid development of methyl ammonium (MA) jumping rotation around the C 3 and C 4 symmetry axes. Our results provide direct evidence for the intimate relation between the rotation of the electric dipoles of MA molecules and the charge carrier lifetime in HOIPs.
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Dimensionality is a critical factor in determining the properties of solids and is an apparent built-in character of the crystal structure. However, it can be an emergent and tunable property in geometrically frustrated spin systems. Here, we study the spin dynamics of the tetrahedral cluster antiferromagnet, pharmacosiderite, via muon spin resonance and neutron scattering. We find that the spin correlation exhibits a two-dimensional characteristic despite the isotropic connectivity of tetrahedral clusters made of spin 5/2 Fe3+ ions in the three-dimensional cubic crystal, which we ascribe to two-dimensionalisation by geometrical frustration based on spin wave calculations. Moreover, we suggest that even one-dimensionalisation occurs in the decoupled layers, generating low-energy and one-dimensional excitation modes, causing large spin fluctuation in the classical spin system. Pharmacosiderite facilitates studying the emergence of low-dimensionality and manipulating anisotropic responses arising from the dimensionality using an external magnetic field.
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Molecular based spin-1/2 triangular lattice systems such as LiZn2Mo3O8 have attracted research interest. Distortions, defects, and intersite disorder are suppressed in such molecular-based magnets, and intrinsic geometrical frustration gives rise to unconventional and unexpected ground states. Li2AMo3O8 (A = In or Sc) is such a compound where spin-1/2 Mo3O13 clusters in place of Mo ions form the uniform triangular lattice. Their ground states are different according to the A site. Li2InMo3O8 undergoes conventional 120° long-range magnetic order below TN = 12 K whereas isomorphic Li2ScMo3O8 exhibits no long-range magnetic order down to 0.5 K. Here, we report exotic magnetisms in Li2InMo3O8 and Li2ScMo3O8 investigated by muon spin rotation (µSR) and inelastic neutron scattering (INS) spectroscopies using polycrystalline samples. Li2InMo3O8 and Li2ScMo3O8 show completely different behaviors observed in both µSR and INS measurements, representing their different ground states. Li2InMo3O8 exhibits spin wave excitation which is quantitatively described by the nearest neighbor anisotropic Heisenberg model based on the 120° spin structure. In contrast, Li2ScMo3O8 undergoes short-range magnetic order below 4 K with quantum-spin-liquid-like magnetic fluctuations down to the base temperature. Origin of the different ground states is discussed in terms of anisotropies of crystal structures and magnetic interactions.
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We demonstrate the presence of ferromagnetic (FM) fluctuations in the superconducting and nonsuperconducting heavily overdoped regimes of high-temperature superconducting copper oxides, using (Bi,Pb)_{2}Sr_{2}CuO_{6+δ} (Bi-2201) single crystals. Magnetization curves exhibit a tendency to be saturated in high magnetic fields at low temperatures in the heavily overdoped crystals, which is probably a precursor phenomenon of a FM transition at a lower temperature. Muon spin relaxation detects the enhancement of spin fluctuations at high temperatures below 200 K. Correspondingly, the ab-plane resistivity follows a 4/3 power law in a wide temperature range, which is characteristic of metals with two-dimensional FM fluctuations due to itinerant electrons. As the Wilson ratio evidences the enhancement of spin fluctuations with hole doping in the heavily overdoped regime, it is concluded that two-dimensional FM fluctuations reside in the heavily overdoped Bi-2201 cuprates, which is probably related to the decrease in the superconducting transition temperature in the heavily overdoped cuprates.
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Materials that show negative thermal expansion (NTE) have significant industrial merit because they can be used to fabricate composites whose dimensions remain invariant upon heating. In some materials, NTE is concomitant with the spontaneous magnetization due to the magnetovolume effect (MVE). Here the authors report a new class of MVE material; namely, a layered perovskite PrBaCo2 O5.5+x (0 ≤ x ≤ 0.41), in which strong NTE [ß ≈ -3.6 × 10-5 K-1 (90-110 K) at x = 0.24] is triggered by embedding ferromagnetic (F) clusters into the antiferromagnetic (AF) matrix. The strongest MVE is found near the boundary between F and AF phases in the phase diagram, indicating the essential role of competition between the F-clusters and the AF-matrix. Furthermore, the MVE is not limited to the PrBaCo2 O5.5+x but is also observed in the NdBaCo2 O5.5+x . The present study provides a new approach to obtaining MVE and offers a path to the design of NTE materials.
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Hydrogen in the Earth's deep interior has been thought to exist as a hydroxyl group in high-pressure minerals. We present Muon Spin Rotation experiments on SiO2 stishovite, which is an archetypal high-pressure mineral. Positive muon (which can be considered as a light isotope of proton) implanted in stishovite was found to capture electron to form muonium (corresponding to neutral hydrogen). The hyperfine-coupling parameter and the relaxation rate of spin polarization of muonium in stishovite were measured to be very large, suggesting that muonium is squeezed in small and anisotropic interstitial voids without binding to silicon or oxygen. These results imply that hydrogen may also exist in the form of neutral atomic hydrogen in the deep mantle.
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The Muon Science Establishment (MUSE) is one of the major experimental facilities, along with those for neutron, hadron and neutrino experiments, in J-PARC. It makes up a part of the Materials and Life Science Experiment Facility (MLF) that hosts a tandem neutron facility (JSNS) driven by a single proton beam. The facility consists of a superconducting solenoid (for pion confinement) with a modest-acceptance (about 45 mSr) injector of pions and muons obtained from a 20 mm thick edge-cooled stationary graphite target, delivering a 'surface muon' beam (µ(+)) and a 'decay muon' beam (µ(+)/µ(-)) for a wide variety of applications. It has recently been confirmed that the beamline has the world's highest muon intensity (â¼10(6) µ(+)/s) at a proton beam power of 120 kW. The beamline is furnished with two experimental areas (D1 and D2) at the exit branches, where an apparatus for muon spin rotation/relaxation experiments (µSR) is currently installed at the D1 area while test experiments are conducted at the D2 area. In this paper, the current performance of the MUSE facility as a whole is reviewed. The facility is still in the early stage of development, including both beamlines and infrastructure for experiments, and plans for upgrading it are discussed together with perspectives for research works envisaged with unprecedented high-intensity muons.
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The magnetic properties of PbVO 3, a PbTiO 3-type perovskite with a large tetragonal distortion ( c/a = 1.229), were investigated. The temperature dependence of the measured magnetization of multidomain single-crystal samples showed a broad maximum centered around 180 K, indicating a two-dimensional antiferromagnetism. muSR measurement revealed the presence of a long-range order below 43 K. The two-dimensional magnetism is due to the ordering of d xy orbitals, which is thought to also be related to the large tetragonal distortion of PbVO 3.
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The electronic structure and the location of muonium centers (Mu) in single-crystalline ZnO were determined for the first time. Two species of Mu centers with extremely small hyperfine parameters have been observed below 40 K. Both Mu centers have an axial-symmetric hyperfine structure along with a <0001> axis, indicating that they are located at the antibonding (AB(O, parallel )) and bond-center (BC( parallel )) sites. It is inferred from their small ionization energy ( approximately 6 and 50 meV) and hyperfine parameters ( approximately 10(-4) times the vacuum value) that these centers behave as shallow donors, strongly suggesting that hydrogen is one of the primary origins of n type conductivity in as-grown ZnO.