Search

The binary fluorite oxide Hf0.5Zr0.5O2 tends to grab a significant amount of notice due to the distinct and superior ferroelectricity found in its metastable phase. Stabilizing the metastable ferroelectric phase and delineating the underlying growth mechanism, however, are still challenging. Recent discoveries of metastable ferroelectric Hf0.5Zr0.5O2 epitaxially grown on structurally dissimilar perovskite oxides have triggered intensive investigations on the ferroelectricity in materials that are nonpolar in bulk form. Nonetheless, the growth mechanism for the unique fluorite/perovskite heterostructures has yet to be fully explored. Here we show that the metastable ferroelectric Hf0.5Zr0.5O2 films can be stabilized even on a one-unit-cell-thick perovskite La0.67Sr0.33MnO3 buffer layer. In collaboration with scanning transmittance electron microscopy (STEM) based characterizations, we show that monolayer reconstruction driven by interfacial redox reactions plays a vital role in the formation of a unique heterointerface between the two structurally dissimilar oxides, providing the template monolayer that facilitates the epitaxial growth of the metastable HZO films. Our findings offer significant insights into the stabilization mechanism of the ferroelectric Hf0.5Zr0.5O2, and this mechanism could be extended for exploring functional metastable phases of various metal oxides.

The diode effect is fundamental to electronic devices and is widely used in rectifiers and AC-DC converters. At low temperatures, however, conventional semiconductor diodes possess a high resistivity, which yields energy loss and heating during operation. The superconducting diode effect (SDE), which relies on broken inversion symmetry in a superconductor may mitigate this obstacle: in one direction a zero-resistance supercurrent can flow through the diode, but for the opposite direction of current flow, the device enters the normal state with ohmic resistance. The application of a magnetic field can induce SDE in Nb/V/Ta superlattices with a polar structure, in superconducting devices with asymmetric patterning of pinning centres, or in superconductor/ferromagnet hybrid devices with induced vortices. The need for an external magnetic field limits their practical application. Recently, a field-free SDE was observed in a NbSe2/Nb3Br8/NbSe2 junction, and it originates from asymmetric Josephson tunneling that is induced by the Nb3Br8 barrier and the associated NbSe2/Nb3Br8 interfaces. Here, we present another implementation of zero-field SDE using noncentrosymmetric [Nb/V/Co/V/Ta]20 multilayers. The magnetic layers provide the necessary symmetry breaking and we can tune the SDE by adjusting the structural parameters, such as the constituent elements, film thickness, stacking order, and number of repetitions. We control the polarity of the SDE through the magnetization direction of the ferromagnetic layers. Artificially stacked structures, as the one used in this work, are of particular interest as they are compatible with microfabrication techniques and can be integrated with devices such as Josephson junctions. Energy-loss-free SDEs as presented in this work may therefore enable novel non-volatile memories and logic circuits with ultralow power consumption., Comment: 31 pages, 11 figures

Recently, all-optical magnetization control has been garnering considerable attention in realizing next-generation ultrafast magnetic information devices. Here, employing a magneto-optical Kerr effect (MOKE) microscope, we observed the laser-induced magnetization switching of ferrimagnetic oxide NiCo2O4 (NCO) epitaxial thin films with perpendicular magnetic anisotropy, where the sample was pumped at 1030-nm laser pulses, and magnetic domain images were acquired via the MOKE microscope with a white light emitting diode. Laser pulses irradiated an NCO thin film at various temperatures from 300 K to 400 K while altering the parameters of pulse interval, fluence, and the number of pulses with the absence of the external magnetic field. We observed accumulative all-optical switching at 380 K and above. Our observation of oxide NCO thin films facilitates the realization of chemically stable magnetization switching using ultrafast lasers, and without applying a magnetic field., Comment: 6 pages, 6 figures

Using a time-resolved magneto-optical Kerr effect (TR-MOKE) microscope, we observed ultrafast demagnetization of inverse-spinel-type NiCo2O4 (NCO) epitaxial thin films of the inverse spinel type ferrimagnet NCO with perpendicular magnetic anisotropy. This microscope uses a pump-probe method, where the sample is pumped at 1030 nm, and magnetic domain images are acquired via MOKE microscopy at 515 nm (the second harmonic). We successfully observed the dynamics of the magnetic domain of the NCO thin film via laser irradiation, and obtained a demagnetization time constant of approximately 0.4 ps. This time constant was significantly smaller than the large time constants reported for other half-metallic oxides. These results, combined with the results of our x-ray photoemission spectroscopy study, indicate that this NCO thin film is a ferrimagnetic metal whose electronic structure deviates from the theoretically predicted half-metallic one., Comment: 5 pages, 5 figures

We experimentally investigated the magnetic properties of NiCo$_2$O$_4$ epitaxial films known to be conductive oxides with perpendicular magnetic anisotropy (PMA) at room temperature. Both magneto-torque and magnetization measurements at various temperatures provide clear experimental evidence of the spin reorientation transition at which the MA changes from PMA to easy-cone magnetic anisotropy (ECMA) at a certain temperature ($T_{\rm{SR}}$). ECMA was commonly observed in films grown by pulsed laser deposition and reactive radio frequency magnetron sputtering, although $T_{\mathrm{SR}}$ is dependent on the growth method as well as the conditions. The cone angles measured from the $c$-axis increased successively at $T_{\mathrm{SR}}$ and approached a maximum of 45-50 degrees at the lowest measurement temperature of 5 K. Calculation with the cluster model suggests that the Ni$^{3+}$ ions occupying the $T_d$ site could be the origin of the ECMA. Both the magnetic properties and the results of the calculation based on the cluster model indicate that the ECMA is attributable to the cation anti-site distribution of Ni$^{3+}$, which is possibly formed during the growth process of the thin films.

We carried out x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy and investigated cation valence states and spin and orbital magnetic moments in the inverse-spinel ferrimagnet Ni$_{1-x}$Co$_{2+y}$O$_{4-z}$ (NCO) epitaxial films with the perpendicular magnetic anisotropy. We show that the oxygen pressure P$_{O2}$ during the film growth by pulsed laser deposition influences not only the cation stoichiometry (site-occupation) but also the cation valence state. Our XAS results show that the Ni in the O$_{h}$-site is in the intermediate valence state between +2 and +3, Ni$^{(2+\delta)+}$ (0<$\delta$<1), whose nominal valence state (the $\delta$ value) varies depending on P$_{O2}$. On the other hand, the Co in the octahedral (O$_{h}$) and tetrahedral (T$_{d}$) sites respectively have the valence state close to +3 and +2. We also find that the XMCD signals originate mainly from the T$_{d}$-site Co$^{2+}$ (Co$_{Td}$) and O$_{h}$-site Ni$^{(2+\delta)+}$ (Ni$_{Oh}$), indicating that these cation valence states are the key in determining the magnetic and transport properties of NCO films. Interestingly, the valence state of Ni$^{(2+\delta)+}$ that gives rise to the XMCD signal remains unchanged independent of P$_{O2}$. The electronic structure of Ni$^{(2+\delta)+}$ that is responsible for the magnetic moment and electrical conduction differs from those of Ni$^{2+}$ and Ni$^{3+}$. In addition, the orbital magnetic moment originating from Co$_{Td}$ is as large as 0.14 $\mu_{B}/Co_{Td}$ and parallel to the magnetization while the Ni$_{Oh}$ orbital moment is as small as 0.07 $\mu_{B}/Ni_{Oh}$ and is rather isotropic. The Co$_{Td}$ therefore plays the key role in the perpendicular magnetic anisotropy of the films. Our results demonstrate the significance of the site-dependent cations valence states for the magnetic and transport properties of NCO films.

We clarify the physical origin of anomalies in transverse resistivity often observed in exotic materials, such as SrRuO3, in which the Berry curvature is manifested in the transport properties. The previously attributed mechanism for the anomalies, the topological Hall effect (THE), is refuted by our thorough investigations as well as formulation of a model considering inhomogeneous magnetoelectric properties in the material. Our analyses fully explain every feature of the anomalies without resorting to the THE. The present results establish a fundamental understanding, which was previously overlooked, of magneto-transport properties in such exotic materials.