Large Perpendicular Magnetic Anisotropy Induced by an Intersite Charge Transfer in Strained EuVO2H Films.

Perovskite oxides ABO3 continue to be a major focus in materials science. Of particular interest is the interplay between A and B cations as exemplified by intersite charge transfer (ICT), which causes novel phenomena including negative thermal expansion and metal-insulator transition. However, the ICT properties were achieved and optimized by cationic substitution or ordering. Here we demonstrate an anionic approach to induce ICT using an oxyhydride perovskite, EuVO2H, which has alternating layers of EuH and VO2. A bulk EuVO2H behaves as a ferromagnetic insulator with a relatively high transition temperature (TC) of 10 K. However, the application of external pressure to the EuIIVIIIO2H bulk or compressive strain from the substrate in the thin films induces ICT from the EuIIH layer to the VIIIO2 layer due to the extended empty V dxy orbital. The ICT phenomenon causes the VO2 layer to become conductive, leading to an increase in TC that is dependent on the number of carriers in the dxy orbitals (up to a factor of 4 for 10 nm thin films). In addition, a large perpendicular magnetic anisotropy appears with the ICT for the films of <100 nm, which is unprecedented in materials with orbital-free Eu2+, opening new perspectives for applications. The present results provide opportunities for the acquisition of novel functions by alternating transition metal/rare earth layers with heteroanions.

Growth of self-integrated atomic quantum wires and junctions of a Mott semiconductor.

Continued advances in quantum technologies rely on producing nanometer-scale wires. Although several state-of-the-art nanolithographic technologies and bottom-up synthesis processes have been used to engineer these wires, critical challenges remain in growing uniform atomic-scale crystalline wires and constructing their network structures. Here, we discover a simple method to fabricate atomic-scale wires with various arrangements, including stripes, X-junctions, Y-junctions, and nanorings. Single-crystalline atomic-scale wires of a Mott insulator, whose bandgap is comparable to those of wide-gap semiconductors, are spontaneously grown on graphite substrates by pulsed-laser deposition. These wires are one unit cell thick and have an exact width of two and four unit cells (1.4 and 2.8 nm) and lengths up to a few micrometers. We show that the nonequilibrium reaction-diffusion processes may play an essential role in atomic pattern formation. Our findings offer a previously unknown perspective on the nonequilibrium self-organization phenomena on an atomic scale, paving a unique way for the quantum architecture of nano-network.

Dehydration of Electrochemically Protonated Oxide: SrCoO2 with Square Spin Tubes.

Controlling oxygen deficiencies is essential for the development of novel chemical and physical properties such as high-Tc superconductivity and low-dimensional magnetic phenomena. Among reduction methods, topochemical reactions using metal hydrides (e.g., CaH2) are known as the most powerful method to obtain highly reduced oxides including Nd0.8Sr0.2NiO2 superconductor, though there are some limitations such as competition with oxyhydrides. Here we demonstrate that electrochemical protonation combined with thermal dehydration can yield highly reduced oxides: SrCoO2.5 thin films are converted to SrCoO2 by dehydration of HSrCoO2.5 at 350 °C. SrCoO2 forms square (or four-legged) spin tubes composed of tetrahedra, in contrast to the conventional infinite-layer structure. Detailed analyses suggest the importance of the destabilization of the SrCoO2.5 precursor by electrochemical protonation that can greatly alter reaction energy landscape and its gradual dehydration (H1-xSrCoO2.5-x/2) for the SrCoO2 formation. Given the applicability of electrochemical protonation to a variety of transition metal oxides, this simple process widens possibilities to explore novel functional oxides.

Epitaxial Stabilization of SrCu3O4 with Infinite Cu3/2O2 Layers.

We report the epitaxial thin-film synthesis of SrCu3O4 with infinitely stacked Cu3O4 layers composed of edge-sharing CuO4 square planes, using molecular-beam epitaxy. Experimental and theoretical characterizations showed that this material is a metastable phase that can exist by applying tensile biaxial strain from the (001)-SrTiO3 substrate. SrCu3O4 shows an insulating electrical resistivity in accordance with the Cu2+ valence state revealed by X-ray photoelectron spectroscopy. First-principles calculations also indicated that the unoccupied d3z2-r2 band becomes substantially stabilized owing to the absence of apical anions, in contrast to A2Cu3O4Cl2 (A = Sr, Ba) with an A2Cl2 block layer and therefore a trans-CuO4Cl2 octahedron. These results suggest that SrCu3O4 is a suitable parent material for electron-doped superconductivity based on the Cu3O4 plane.

Heavy interstitial hydrogen doping into SrTiO3.

We achieve the introduction of an extremly large amount of interstitial hydrogen into strontium titanate (SrTiO3) by low-temperature hydrogen ion beam irradiation. The in situ transport measurements reveal an unprecedented thermal hysteresis of the resistivity.

Epitaxial thin films of ATiO(3-x)H(x) (A = Ba, Sr, Ca) with metallic conductivity.

Epitaxial thin films of titanium perovskite oxyhydride ATiO(3-x)H(x) (A = Ba, Sr, Ca) were prepared by CaH(2) reduction of epitaxial ATiO(3) thin films deposited on a (LaAlO(3))(0.3)(SrAl(0.5)Ta(0.5)O(3))(0.7) substrate. Secondary ion mass spectroscopy detected a substantial amount and uniform distribution of hydride within the film. SrTiO(3)/LSAT thin film hydridized at 530 °C for 1 day had hydride concentration of 4.0 × 10(21) atoms/cm(3) (i.e., SrTiO(2.75)H(0.25)). The electric resistivity of all the ATiO(3-x)H(x) films exhibited metallic (positive) temperature dependence, as opposed to negative as in BaTiO(3-x)H(x) powder, revealing that ATiO(3-x)H(x) are intrinsically metallic, with high conductivity of 10(2)-10(4) S/cm. Treatment with D(2) gas results in hydride/deuteride exchange of the films; these films should be valuable in further studies on hydride diffusion kinetics. Combined with the materials' inherent high electronic conductivity, new mixed electron/hydride ion conductors may also be possible.

Quasiparticle scattering induced by charge doping of iron-pnictide superconductors probed by collective vortex pinning.

Charge doping of iron-pnictide superconductors leads to collective pinning of flux vortices, whereas isovalent doping does not. Moreover, flux pinning in the charge-doped compounds is consistently described by the mean-free path fluctuations introduced by the dopant atoms, allowing for the extraction of the elastic quasiparticle scattering rate. The absence of scattering by dopant atoms in isovalently doped BaFe2(As(1-x)P(x))(2) is consistent with the observation of a linear temperature dependence of the low-temperature penetration depth in this material.