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The magnetization of amorphous DyCo3 and TbCo3 is studied by magnetometry, anomalous Hall effect and magneto-optic Kerr effect to understand the temperature-dependent magnetic structure. A square magnetic hysteresis loop with perpendicular magnetic anisotropy and coercivity that reaches 3.5 T in the vicinity of the compensation temperature is seen in thin films. An anhysteretic soft component, seen in the magnetization of some films but not in their Hall or Kerr loops is an artefact due to sputter-deposition on the sides of the substrate. The temperature-dependence of the net rare earth moment from 4-300K is deduced, using the cobalt moment in amorphous YxCo1-x. The single-ion anisotropy of the quadrupole moments of the 4f atoms in the randomly-oriented local electrostatic field gradient overcomes their exchange coupling to the cobalt subnetwork, resulting in a sperimagnetic ground state where spins of the noncollinear rare-earth subnetwork are modelled by a distribution of rare earth moments within a cone whose axis is antiparallel to the ferromagnetic axis z of the cobalt subnetwork. The reduced magnetization (Jz)/J at T=0 is calculated from an atomic Hamiltonian as a function of the ratio of anisotropy to exchange energy per rare-earth atom for a range of angles between the local anisotropy axis and -z and then averaged over all directions in a hemisphere. The experimental and calculated values of (J-z)/J are close to 0.7 at low temperature for both Dy and Tb. On increasing temperature, the magnitude of the rare earth moment and the local random anisotropy that creates the cone are reduced; the cone closes and the structure approaches collinear ferrimagnetism well above ambient temperature. An asymmetric spin flop of the exchange-coupled subnetworks appears in the vicinity of the magnetization compensation temperatures of 175K for amorphous Dy0.25Co0.75 and 200 K for amorphous TbCo3., Comment: 23 pages, 12 figures

Sputtered thin films of binary YxCo1-x with 0 < x < 0.54 and thickness 15 nm are investigated to help understand the ferromagnetism of cobalt in amorphous rare-earth cobalt alloys. The magnetic moment per cobalt falls to zero at x0 = 0.50, where the appearance of magnetism is marked by a para-process with a dimensionless susceptibility of up to 0.015. All films are magnetically soft, with densities that fall between those of crystalline Y-Co intermetallic compounds and the density of a relaxed 10,000-atom binary random close-packed model of hard spheres with an Y:Co volume ratio of 3:1, where the packing fractions for all films lies in a narrow range around 0.633 and Co is coordinated by 3.2 Co and 3.2 Y atoms at x = 0.5. All films with x < 0.4 exhibit in-plane shape anisotropy that is about six times as great as an intrinsic perpendicular component. Average cobalt spin and orbital moments obtained by X-ray magnetic circular dichroism were 1.31 and 0.32 Bohr magnetons, respectively for amorphous Y0.25Co0.75. Strong local anisotropy is associated with the large cobalt orbital moment, but there is little influence of anisotropy on the ferromagnetic order because of exchange averaging. The Hall effect and magnetoresistance are modelled in terms of effective uniform rotation of the magnetization, with spontaneous and band contributions. Amorphous YxCo1-x is contrasted with amorphous YxFe1-x, which exhibits random noncollinear magnetic order that is very sensitive to the film density., Comment: 16 pages, 9 figures

Magnetic properties of multicomponent alloys depend sensitively on the degree of atomic order on the different crystallographic sites. In this work we demonstrate the magnetic contrast between bulk and thin-film samples of the Heusler alloy V$_{2}$FeAl. Arc-melted bulk ingots show practically no site preference of the elements (A2 structure), whereas magnetron-sputtered thin-film samples display a higher degree of atomic ordering with a tendency towards XA-type order. Electronic structure calculations favour ferrimagnetic XA-type ordering, and the effect of different pairwise atomic disorder on the element specific and net magnetic moments are evaluated to reproduce experimental observations. XA-type thin-films with iron moment of 1.24 $\mu_{\mathrm{B}}$ determined by X-ray magnetic circular dichroism are in agreement with calculation, but the measured net moment of 1.0 $\mu_{\mathrm{B}}$ per formula unit and average vanadium moment are smaller than expected from calculations. The measured Curie temperature is approximately 500 K. Films with a higher degree of disorder have a T$_{\mathrm{C}}$ close to 300 K with a net moment of 0.1 $\mu_{\mathrm{B}}$ at low temperature. The large calculated vanadium moments are destroyed by partial disorder on $4d$ vanadium sites. By contrast, the arc-melted and annealed bulk alloy with a fully-disordered A2 structure shows no spontaneous magnetization; it is a Pauli paramagnet with dimensionless susceptibility $\chi_{\mathrm{v}}=-2.95\times10^{-4}$., Comment: 10 pages, 7 figures

Exploring anisotropy and diverse magnetization dynamics in specimens with vanishing magnetic moments presents a significant challenge using traditional magnetometry, as the low resolution of existing techniques hinders the ability to obtain accurate results. In this study, we delve deeper into the examination of magnetic anisotropy and quasi-static magnetization dynamics in \mrg\,(MRG) thin films, as an example of a compensated ferrimagnetic half-metal, by employing anomalous Hall effect measurements within a tetragonal crystal lattice system. Our research proposes an innovative approach to accurately determine the complete set of anisotropy constants of these MRG thin films. To achieve this, we perform anomalous Hall voltage curve fitting, using torque models under the macrospin approximation, which allow us to obtain out-of-plane anisotropy constants $K_1=4.0\times10^4$ J m$^{-3}$ ($K_1/M=0.655$\,T) and $K_2=2.54\times10^4$ J m$^{-3}$ ($K_2/M=0.416$\,T), along with a weaker in-plane anisotropy constant $K_3=3.48\times10^3$ J m$^{-3}$ ($K_3/M=0.057$\,T). By additionally employing first-order reversal curves (FORC) and classical Preisach hysteresis (hysterons) models, we are able to validate the efficacy of the macrospin model in capturing the magnetic behavior of MRG thin films. Furthermore, our investigation substantiates that the complex quasi-static magnetization dynamics of MRG thin films can be effectively modelled using a combination of hysteronic and torque models. This approach facilitates the exploration of both linear and non-linear quasi-static magnetization dynamics, in the presence of external magnetic field and/or current-induced effective fields, generated by the spin-orbit torque and spin transfer torque mechanisms., Comment: 14 pages, 10 figures

The cubic Heusler alloy Ru$_{2-x}$Mn$_{1+x}$Al is grown in thin film form on MgO and MgAl$_2$O$_4$ substrates. It is a highly spin-polarised ferrimagnetic metal, with weak magnetocrystalline anisotropy. Although structurally and chemically similar to $\text{Mn}_2\text{Ru}_x\text{Ga}$, it does not exhibit ferrimagnetic compensation, or large magneto galvanic effects. The differences are attributed to a combination of atomic order and the hybridisation with the group 13 element Al or Ga. The spin polarisation is around 50 to 60 %. There is a gap in the density of states just above the Fermi level in fully ordered compounds., Comment: 8 pages , 7 figures, 2 tables

He$^+$ ion irradiation is used to pattern multiple areas of Pt/Co/W films with different irradiation doses in Hall bars. The resulting perpendicular magnetic anisotropy landscape enables selective multilevel current-induced switching, with full deterministic control of the position and order of the individual switching elements. Key pattern design parameters are specified, opening a way to scalable multilevel switching devices., Comment: 7 pages, 3 figures

Pendant droplets of water and paramagnetic solutions are studied in the presence of uniform and nonuniform magnetic fields produced by small permanent magnet arrays, both in static conditions and during dynamic pinch-off. Static measurements of the droplet shape are analysed in terms of an apparent surface tension {\gamma}app or an effective density \r{ho}eff. The change of surface tension of deionized water in a uniform field of 450 mT is insignificant, 0.19 - 0.21 mNm-1. Measurements on droplets of compensated zero-susceptibility solutions of Cu2+, Mn2+ and Dy3+ where the shape is unaffected by any magnetic body force show changes of surface tension of about -1% in 500 mT. Magnetic field gradients of up to 100 T2m-1 deform the droplets and lead to changes of \r{ho}eff that are negative for diamagnetic solutions (buoyancy effect) and positive for paramagnetic solutions. The droplet profile of strongly-paramagnetic 0.1 Dy M DyCl3 solution is analysed, treating the nonuniform vertical field gradient as a spatial variation of gravity. The influence of Maxwell stress on droplet shape is discussed. In dynamic measurements, the droplet shape at pinch-off is recorded by high-speed photography and analysed in terms of a relative change of dynamic surface tension in the presence of a magnetic field. The surface-tension-dependent pre-factor of the scaling law that governs the pinch-off dynamics shows no difference for pure water or 0.11 M DyCl3 solutions in the field. The nonuniform field has no influence in the pinch-off region because the filament diameter is much less than the capillary length.

The evaporation of drops of water placed at the center of long poly(methyl methacrylate) microfluidic channels with a rectangular cross section of 0.38 mm2 is studied by simultaneously monitoring the shapes of two samples, one is in a 300 mT magnetic field, the other is in no field. A magnetic enhancement of the evaporation rate of up to 140 % is observed, which can be understood by treating the ortho and para nuclear isomers of water vapor as quasi-independent gasses with an ortho:para ratio in fresh vapor close to 2:3. It would take much longer than the 2 - 4 h duration of an experiment in the channel, for the ratio to approach the 3:1 equilibrium value. Magnetic field influences evaporation rate by equalizing the isomeric populations in the vapor phase. The atmosphere in the channel is saturated with water vapor yet the evaporation rate far exceeds that in open beakers., Comment: 13 pages, 4 Figures

Hypothesis. Ortho and para water are the two nuclear isomers where the hydrogen protons align to give a total nuclear spin of 0 or 1.The equilibrium ratio of 3:1 is established slowly in freshly evaporated water vapour and the isomers then behave distinct gasses, with their own partial pressures. Magnetic-field-induced ortho to para transformations are expected to alter the evaporation rate. Experiment. Evaporation from beakers of deionized water and a 6 M solution of urea is monitored simultaneously for periods from 1 to 60 hours with and without a 500 mT magnetic field, while logging the ambient temperature and humidity. The balances with the two beakers are shielded in the same Perspex container. Many runs have been conducted over a two-year period. Findings. The evaporation rate of water is found to increase by 12 % of in the field but that of water in urea solution decreases by 28 6 %. Two effects are at play. One is dephasing of the Larmor precession of adjacent protons on a water molecule in a field gradient, which tends to equalize the isomer populations. The other is Lorentz stress on the moving charge dipole, which can increase the proportion of the ortho isomer. From analysis of the time and field dependence of the evaporation, we infer an ortho fraction of 39 % in fresh vapour from water and 60 % in fresh vapour from urea., Comment: 27 pages (9 Figures, 1 Table)

Metallic Mn-based alloys with a nearest-neighbor Mn-Mn distance greater than 0.4 nm exhibit large, well-localized magnetic moments. Here we investigate the magnetism of tetragonal Au4Mn with a Curie temperature of 385 K, where manganese has a spin moment of 4.1 muB and its orbital moment is quenched. Since 80% of the atoms are gold, the spin orbit interaction is strong and Au4Mn exhibits uniaxial magnetocrystalline anisotropy with surface maze domains at room temperature. The magnetic hardness parameter of 1.0 is sufficient to maintain the magnetization along the c-axis for a sample of any shape. Au also reduces the spin moment of Mn through 5d-3d orbital hybridization. An induced moment of 0.05 muB was found on Au under a pulsed field of 40 T. Density functional theory calculations indicate that the Mn-Mn exchange is mediated by spin-polarized gold 5d and 6p electrons. The distance-dependence shows that it is ferromagnetic or zero for the first ten shells of Mn neighbors out to 1.041 nm (64 atoms), and very weak and oscillatory thereafter.

An overview of the effect of a magnetic field gradient on fluids with linear magnetic susceptibilities is given. It is shown that two commonly encountered expressions, the magnetic field gradient force and the concentration gradient force for paramagnetic species in solution are equivalent for incompressible fluids. The magnetic field gradient and concentration gradient forces are approximations of the Kelvin force and Korteweg-Helmholtz force densities, respectively. The criterion for the appearance of magnetically induced convection is derived. Experimental work in which magnetically induced convection plays a role is reviewed.

Compensated ferrimagnets, like antiferromagnets, show no net magnetization but their transport and magneto-optic properties resemble those of ferromagnets, thereby creating opportunities for applications in high-frequency spintronics and low-energy loss communications. Here we study the modification the noncollinear ferrimagnetic spin structure of Mn4N by a variety of metallic substitutions Z (Z = Cu - Ge and Ag - Sn) to achieve compensation at room temperature. The noncollinear frustrated 2.35 Bohr magneton moments of Mn on 3c sites of the (111) kagome planes tilt about 20 degree out-of-plane in Mn4N and are easily influenced by the substitutions on 1a sites, leading to different efficiency of compensation in Mn4-xZxN that increases gradually from group 11 (Cu, Ag) to group 14 (Ge, Sn) with increasing number of valance electrons. Elements from the 5th period are more efficient for compensation than those from the 4th period due to lattice expansion. The manganese site moments are determined by Z, orbital hybridization, charge transfer and the tilt angle, analyzed by constrained density functional theory. The Ga compound with compensation at room temperature for x = 0.26 is recommended for high-frequency spintronic applications.

Repeated uniform switching of the magnetization of thin films of ferrimagnetic amorphous Gd$_{x}$(FeCo)$_{1-x}$ in response to single fast laser pulses is well established. Here we report unusual toggle switching in thin films of sperimagnetic amorphous Dy$_x$Co$_{1-x}$ and Tb$_x$Co$_{1-x}$ with $\it{x} \simeq$ 0.25 irradiated with single 200 fs pulses of 800 nm laser light. The samples have strong local random anisotropy due to the non-S state rare earth. The compensation temperature of the films is $\le$ 180 K and their Curie temperature is $\simeq$ 500 K. They are mostly switched by the first pulse, and subsequent pulses lead to partial re-switching of a decreasing amount of the irradiated area, with a granular structure of submicron regions of switched and unswitched material. Individual switched domains about 700 nm in size are observed around the edge of the irradiated spots where the fluence is at the threshold for switching. Results are discussed in terms of a random anisotropy model where the ratio of local anisotropy to exchange is temperature dependent and close to the threshold for strong pinning., Comment: The following article has been submitted to Applied Physics Letters - Special Issue

The electrosorption of Gd$^{3+}$ ions from aqueous 70 mM Gd(NO$_3$)$_3$ solution in monolithic carbon aerogel electrodes was recorded by dynamic neutron imaging. The aerogels have a bimodal pore size distribution consisting of macropores and mesopores centered at 115 nm and 15 nm, respectively. After the uptake of Gd$^{3+}$ ions by the negatively charged surface of the porous structure, an inhomogeneous magnetic field was applied to the system of discharging electrodes. This led to a convective flow and confinement of Gd(NO$_3$)$_3$ solution in the magnetic field gradient. Thus, a way to desalt and capture paramagnetic ions from an initially homogeneous solution is established.

Perpendicular heterostructures based on a ferrimagnetic Mn2RuxGa (MRG) layer and a ferromagnetic Co/Pt multilayer were examined to understand the effects of different spacer layers (V, Mo, Hf, HfOx and TiN) on the interfaces with the magnetic electrodes, after annealing at 350 C. Loss of perpendicular anisotropy in MRG is strongly correlated with a reduction in the substrate-induced tetragonality due to relaxation of the crystal structure. In the absence of diffusion, strain and chemical ordering within MRG are correlated. The limited solubility of both Hf and Mo in MRG is a source of additional valence electrons, which results in an increase in compensation temperature Tcomp. This also stabilises perpendicular anisotropy, compensating for changes in strain and defect density. The reduction in squareness of the MRG hysteresis loop measured by anomalous Hall effect is <10 %, making it useful in active devices. Furthermore, a CoPt3 phase with (2 2 0) texture in the perpendicular Co/Pt free layer promoted by a Mo spacer layer is the only one that retains its perpendicular anisotropy on annealing., Comment: 1st revision - addition of XRD strain analysis, XRR fitting data, additional references, detail added to text

All-optical re-switching has been investigated in the half-metallic Heusler ferrimagnet Mn2Ru0.9Ga, where Mn atoms occupy two inequivalent sites in the XA-type structure. The effect of a second 200 fs 800 nm pump pulse that follows a first pulse, when both are above the threshold for switching, is studied as a function of t12, the time between them. The aims are to identify the physical mechanisms involved and to determine the minimum time needed for re-switching. The time trajectory of the switching process on a plot of sublattice angular momentum, S4a vs S4c, is in three stages; When t < 0.1 ps, the sublattice moments are rapidly disordered, but not destroyed, while conserving net angular momentum via optical spin-wave excitations. This leads to transient parallel alignment of the residual Mn spins in the first quadrant. The net angular momentum associated with the majority sublattice then flips in about 2 ps, and a fully-reversed ferrimagnetic state is then established via the spin-lattice interaction, which allows re-switching provided t12 > 10 ps., Comment: 13 pages - 4 figures

The ruthenium content of half-metallic Mn$_2$Ru$_x$Ga thin films, with a biaxially-strained inverse Heusler structure, controls the ferrimagnetism that determines their magnetic and electronic properties. An extensive study of Mn$_y$Ru$_x$Ga films on MgO (100) substrates with $1.8 \leq y \leq 2.6$ and $x = 0.5$, 0.7 or 0.9, including crystallographic, magnetic order, magneto-transport and spin polarisation is undertaken to map specific composition-dependent properties in this versatile ternary system. A comparison of experimental densities obtained from X-ray reflectivity with calculated densities indicates full site occupancy for all compositions, which implies chemical disorder. All moments lie on the Slater-Pauling plot with slope 1 and all except $x = 0.5$, $y = 2.2$ exhibit magnetic compensation at \tcmp~below 500~K. The coercivity near \tcmp~exceeds 10~T. Increasing the Mn or Ru content raises \tcmp, but increasing Ru also decreases the spin polarisation determined by point contact Andreev reflection. Molecular field theory is used to model the temperature dependence of the net ferrimagnetic moment and three principal exchange coefficients are deduced. Marked differences in the shape of anomalous Hall and net magnetisation hysteresis loops are explained by substantial canting of the small net moment by up to \SI{40}{\degree} relative to the $c$-axis in zero field, which is a result of slight non-collinearity of the Mn$^{4c}$ sublattice moments due to competing intra-sublattice exchange interactions arising from antisite disorder and excess Mn in the unit cell. Consequences are reduced spin polarisation and an enhanced intrinsic contribution to the anomalous Hall effect. The systematic investigation of the physical properties as a function of $x$ and $y$ will guide the selection of compositions to meet the requirements for magnonic and spintronic MRG-based devices.

The development of high-density magnetic recording media is limited by the superparamagnetism in very small ferromagnetic crystals. Hard magnetic materials with strong perpendicular anisotropy offer stability and high recording density. To overcome the difficulty of writing media with a large coercivity, heat assisted magnetic recording (HAMR) has been developed, rapidly heating the media to the Curie temperature Tc before writing, followed by rapid cooling. Requirements are a suitable Tc, coupled with anisotropic thermal conductivity and hard magnetic properties. Here we introduce Rh2CoSb as a new hard magnet with potential for thin film magnetic recording. A magnetocrystalline anisotropy of 3.6 MJm-3 is combined with a saturation magnetization of {\mu}0Ms = 0.52 T at 2 K (2.2 MJm-3 and 0.44 T at room-temperature). The magnetic hardness parameter of 3.7 at room temperature is the highest observed for any rare-earth free hard magnet. The anisotropy is related to an unquenched orbital moment of 0.42 {\mu}B on Co, which is hybridized with neighbouring Rh atoms with a large spin-orbit interaction. Moreover, the pronounced temperature-dependence of the anisotropy that follows from its Tc of 450 K, together with a high thermal conductivity of 20 Wm-1K-1, makes Rh2CoSb a candidate for development for heat assisted writing with a recording density in excess of 10 Tb/in2.

Spin orbit torque driven switching is a favourable way to manipulate nanoscale magnetic objects for both memory and wireless communication devices. The critical current required to switch from one magnetic state to another depends on the geometry and the intrinsic properties of the materials used, which are difficult to control locally. Here we demonstrate how focused helium ion beam irradiation can modulate the local magnetic anisotropy of a Co thin film at the microscopic scale. Real-time in-situ characterisation using the anomalous Hall effect showed up to an order of magnitude reduction of the magnetic anisotropy under irradiation, and using this, multi-level switching is demonstrated. The result is that spin-switching current densities, down to 800 kA cm$^{-2}$, can be achieved on predetermined areas of the film, without the need for lithography. The ability to vary critical currents spatially has implications not only for storage elements, but also neuromorphic and probabilistic computing., Comment: Main text: 22 pages, 3 figures, 2 tables, 1 TOC graphic. Included SI: 2 pages, 2 figures

We study the demagnetization dynamics of the fully compensated half-metallic ferrimagnet Mn$_2$Ru$_x$Ga. While the two antiferromagnetically coupled sublattices are both composed of manganese, they exhibit different temperature dependencies due to their differing local environments. The sublattice magnetization dynamics triggered by femtosecond laser pulses are studied to reveal the roles played by the spin and intersublattice exchange. We find a two-step demagnetization process, similar to the well-established case of Gd(FeCo)$_3$, where the two Mn-sublattices have different demagnetization rates. The behaviour is analysed using a four-temperature model, assigning different temperatures to the two manganese spin baths. Even in this strongly exchange-coupled system, the two spin reservoirs have considerably different behaviour. The half-metallic nature and strong exchange coupling of Mn$_2$Ru$_x$Ga lead to spin angular momentum conservation at much shorter time scales than found for Gd(FeCo)$_3$ which suggests that low-power, sub-picosecond switching of the net moment of Mn$_2$Ru$_x$Ga is possible., Comment: 5 pages, 3 figures, J. Phys.: Condens. Matter (2021)

The method of neutron imaging was adopted to map the concentration evolution of aqueous paramagnetic Gd(NO3)3 solutions. Magnetic manipulation of the paramagnetic liquid within a miscible nonmagnetic liquid is possible by countering density-difference driven convection. The formation of salt fingers caused by double-diffusive convection in a liquid-liquid system of Gd(NO3)3 and Y(NO3)3 solutions can be prevented by the magnetic field gradient force., Comment: 5 Pages of article with 4 figures, 1 page of supplementary material with 2 figures; Time sequenced neutron images available at https://aip.scitation.org/doi/suppl/10.1063/1.5135390

Here we study both static and time-resolved dynamic magnetic properties of the compensated ferrimagnet from room temperature down to 10K, thus crossing the magnetic compensation temperature $T_{M}$. The behaviour is analysed with a model of a simple collinear ferrimagnet with uniaxial anisotropy and site-specific gyromagnetic ratios. We find a maximum zero-applied-field resonance frequency of $\sim$160GHz and a low intrinsic Gilbert damping $\alpha$$\sim$0.02, making it a very attractive candidate for various spintronic applications., Comment: 6 pages, 6 figures, accepted paper in PRB (https://journals.aps.org/prb/accepted/df07aOb2T7f1e845c21429304f825e825c3a5f190)

Energy-efficient control of magnetization without the help of a magnetic field is a key goal of spintronics. Purely heat-induced single-pulse all-optical toggle switching has been demonstrated, but so far only in Gd based amorphous ferrimagnet films. In this work, we demonstrate toggle switching in the half-metallic compensated ferrimagnetic Heusler alloys Mn2RuxGa, which have two crystallographically-inequivalent Mn sublattices. Moreover, we observe the switching at room temperature in samples that are immune to external magnetic fields in excess of 1 T, provided they exhibit compensation above room temperature. Observations of the effect in compensated ferrimagnets without Gd challenges our understanding of all-optical switching. The dynamic behavior indicates that Mn2RuxGa switches in 2 ps or less. Our findings widen the basis for fast optical switching of magnetization and break new ground for engineered materials that can be used for nonvolatile ultrafast switches using ultrashort pulses of light., Comment: 18 pages of article, 4 figures, Supplementary Information

The effect of vacuum annealing thin films of the compensated ferrimagnetic half-metal Mn2RuxGa at temperatures from 250 to 400 degree Celsius is investigated. The 39.3 nm films deposited on (100) MgO substrates exhibit perpendicular magnetic anisotropy due to a small 1% tetragonal elongation induced by substrate strain. The main change on annealing is a modification in the compensation temperature, which first increases from 50 K for the as-deposited film to 185 K after annealing at 250 degree Celsius, and then falls to 140 K after annealing at 400 degree Celsius. There are minor changes in the atomic order, coercivity, resistivity and anomalous Hall effect (AHE), but the net magnetization measured by SQUID magnetometry with the field applied in-plane or perpendicular-to-the-plane changes more significantly. It saturates at 20 to 30 kA/m at room temperature, and a small soft component is seen in the perpendicular SQUID loops which is absent in the square AHE hysteresis loops. This is explained by the half-metallic nature of the compound; the AHE probes only the 4c Mn sublattice that provides the spin-polarized electrons at the Fermi level, whereas the SQUID measures the sum of the oppositely-aligned 4c and 4a sublattice magnetisations.

The magnetic dead layers in films a few nanometers thick are investigated for La$_{0.7}$Sr$_{0.3}$MnO$_3$ on (001)-oriented SrTiO$_3$ (STO), LaAlO$_3$ (LAO) and (LaAlO$_3$)$_{0.3}$(Sr$_2$TaAlO$_6$)$_{0.7}$ (LSAT) substrates. An anomalous moment found to persist above the Curie temperature of the La$_{0.7}$Sr$_{0.3}$MnO$_3$ films is not attributed to the films, but to oxygen vacancies at or near the surface of the substrate. The contribution to the moment from the substrate is as high as 20 $\mu$B/nm$^2$ in the case of STO or LSAT. The effect is increased by adding an STO cap layer. Taking this d-zero magnetism into account, extrapolated magnetic dead layer thicknesses of 0.8 nm, 1.5 nm and 3.0 nm are found for the manganite films grown on LSAT, STO and LAO substrates, respectively. An STO cap layer eliminates the LSMO dead layer.

Antiferromagnets and compensated ferrimagnets offer opportunities to investigate spin dynamics in the 'terahertz gap' because their resonance modes lie in the 0.3 THz to 3 THz range. Despite some inherent advantages when compared to ferromagnets, these materials have not been extensively studied due to difficulties in exciting and detecting the high-frequency spin dynamics, especially in thin films. Here we show that spin-obit torque in a single layer of the highly spin-polarized compensated ferrimagnet Mn2RuxGa is remarkably efficient at generating spin-orbit fields \mu_0H_eff, which approach 0.1x10-10 T m2/A in the low-current density limit -- almost a thousand times the Oersted field, and one to two orders of magnitude greater than the effective fields in heavy metal/ferromagnet bilayers. From an analysis of the harmonic Hall effect which takes account of the thermal contributions from the anomalous Nernst effect, we show that the antidamping component of the spin-orbit torque is sufficient to sustain self-oscillation. Our study demonstrates that spin electronics has the potential to underpin energy-frugal, chip-based solutions to the problem of ultra high-speed information transfer.

We have a choice of methods for examining domains at the surface of a ferromagnet that depend on probing the stray field distribution, but these methods do not work in antiferromagnets or compensated ferrimagnets, which produce no stray field. The discovery of compensated ferrimagnetic half-metals allows for the local magnetization state to be observed directly with polarized light. The example considered here, Mn$_{2}$Ru$_{x}$Ga, has two inequivalent but oppositely-aligned Mn sublattices with equal and opposite moments, but only one of them contributes spin polarized conduction electrons at the Fermi energy. The material looks like an antiferromagnet from the outside, but from the point of view of electronic structure it resembles a spin-polarized ferromagnetic metal. The anisotropy axis is perpendicular to the film plane, which allows domains to be imaged directly by polar magneto-optic Kerr effect. The domain structure in a film with a composition of Mn$_{2}$Ru$_{0.4}$Ga has been imaged in a Kerr microscope and hysteresis loops traced. Domains have dimensions of order 20 {\mu}m with meandering domain walls and a fractal dimension D$_{f}$ = 1.85. Our results open new direct imaging possibilities for magnetically-ordered materials with no net moment.

Electrolyte gating is a powerful means for tuning the carrier density and exploring the resultant modulation of novel properties on solid surfaces. However, the mechanism, especially its effect on the oxygen migration and electrostatic charging at the oxide heterostructures, is still unclear. Here we explore the electrolyte gating on oxygen-deficient interfaces between SrTiO3 (STO) crystals and LaAlO3 (LAO) overlayer through the measurements of electrical transport, X-ray absorption spectroscopy (XAS) and photoluminescence (PL) spectra. We found that oxygen vacancies (Ovac) were filled selectively and irreversibly after gating due to oxygen electromigration at the amorphous LAO/STO interface, resulting in a reconstruction of its interfacial band structure. Because of the filling of Ovac, the amorphous interface also showed an enhanced electron mobility and quantum oscillation of the conductance. Further, the filling effect could be controlled by the degree of the crystallinity of the LAO overlayer by varying the growth temperatures. Our results reveal the different effects induced by electrolyte gating, providing further clues to understand the mechanism of electrolyte gating on buried interfaces and also opening a new avenue for constructing high-mobility oxide interfaces., Comment: 5 figures; Supplementary materials included at the end of the main text

Magnetotransport is investigated in thin films of the half-metallic ferrimagnet Mn$_2$Ru$_x$Ga in pulsed magnetic fields of up to 58 T. A non-vanishing Hall signal is observed over a broad temperature range, spanning the compensation temperature 155 K, where the net magnetic moment is strictly zero, the anomalous Hall conductivity is 6673 $\Omega^{-1}.m^{-1}$ and the coercivity exceeds 9 T. Molecular field modelling is used to determine the intra- and inter-sublattice exchange constants and from the spin-flop transition we infer the anisotropy of the electrically active sublattice to be 216 kJ/m$^3$ and predict the magnetic resonances frequencies. Exchange and anisotropy are comparable and hard-axis applied magnetic fields result in a tilting of the magnetic moments from their collinear ground state. Our analysis is applicable to collinear ferrimagnetic half-metal systems.

The magneto-optical Kerr effect (MOKE) is often assumed to be proportional to the magnetisation of a magnetically ordered metallic sample; in metallic ferrimagnets with chemically distinct sublattices, such as rare-earth transition-metal alloys, it depends on the difference between the sublattice contributions. Here we show that in a highly spin polarized, fully compensated ferrimagnet, where the sublattices are chemically similar, MOKE is observed even when the net moment is strictly zero. We analyse the spectral ellipsometry and MOKE of Mn 2 Ru x Ga, and show that this behaviour is due to a highly spin-polarized conduction band dominated by one of the two manganese sublattices which creates helicity-dependent reflectivity determined by a broad Drude tail. Our findings open new prospects for studying spin dynamics in the infra-red., Comment: 7 pages, 7 figures

Nanoporous alumina membranes produced by mild or hard anodisation in oxalic acid at potentials ranging from 5 - 140 V have a controllable pore surface area of up to 200 times the membrane area. They exhibit a saturating magnetic response that is temperature-independent and almost anhysteretic below room temperature. The magnetism cannot be explained by the ~1 ppm of transition-metal impurities present in the membranes. The magnetic moment increases with the area of the open nanopores, reaching values of 0.6 Bohr magnetons per square nanometer for mild anodisation and 8 muB/nm2 for hard anodisation where the growth rate is faster. Crystallization of the membrane or chemical treatment with salicylic acid reduces the effect by up to 90 %. The magnetism is therefore associated with the open pore surfaces of the amorphous Al2O3, and it is independent of the orientation of the applied field with respect to the membrane surface. Possible explanations in terms of electrons associated with oxygen vacancies (F or F+ centres) are discussed and it is concluded that the effect is due to giant orbital paramagnetism rather than collective ferromagnetic spin order.

The magnetization of thin films of cobalt ferrite frequently falls far below the bulk value of 455 kAm-1, which corresponds to an inverse cation distribution in the spinel structure with a significant orbital moment of about 0.6 muB that is associated with the octahedrally-coordinated Co2+ ions. The orbital moment is responsible for the magnetostriction and magnetocrystalline anisotropy, and its sensitivity to imposed strain. We have systematically investigated the structure and magnetism of films produced by pulsed-laser deposition on different substrates (TiO2, MgO, MgAl2O4, SrTiO3, LSAT, LaAlO3) and as a function of temperature (500-700 C) and oxygen pressure (10-4 - 10 Pa). Magnetization at room-temperature ranges from 60 to 440 kAm-1, and uniaxial substrate-induced anisotropy ranges from +220 kJm-3 for films on deposited on MgO (100) to -2100 kJm-3 for films deposited on MgAl2O4 (100), where the room-temperature anisotropy field reaches 14 T. No rearrangement of high-spin Fe3+ and Co2+ cations on tetrahedral and octahedral sites can reduce the magnetization below the bulk value, but a switch from Fe3+ and Co2+ to Fe2+ and low-spin Co3+ on octahedral sites will reduce the low-temperature magnetization to 120 kAm-1, and a consequent reduction of Curie temperature can bring the room-temperature value to near zero. Possible reasons for the appearance of low-spin cobalt in the thin films are discussed. Keywords; Cobalt ferrite, thin films, pulsed-laser deposition, low-spin Co3+, strain engineering of magnetization.

The quasi two-dimensional electron gas (q-2DEG) at oxide interfaces provides a platform for investigating quantum phenomena in strongly correlated electronic systems. Here, we study the transport properties at the high-mobility (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)O$_{0.3}$/SrTiO$_{0.3}$ (LSAT/STO) interface. Before oxygen annealing, the as-grown interface exhibits a high electron density and electron occupancy of two subbands: higher-mobility electrons ($\mu_1\approx{10^4}$ cm$^2$V$^{-1}$s$^{-1}$ at 2 K) occupy the lower-energy $3d_{xy}$ subband, while lower-mobility electrons ($\mu_1\approx{10^3}$ cm$^{2}$V$^{-1}$s$^{-1}$ at 2 K) propagate in the higher-energy $3d_{xz/yz}$-dominated subband. After removing oxygen vacancies by annealing in oxygen, only a single type of 3dxy electrons remain at the annealed interface, showing tunable Shubnikov-de Haas (SdH) oscillations below 9 T at 2 K and an effective mass of $0.7m_e$. By contrast, no oscillation is observed at the as-grown interface even when electron mobility is increased to $50,000$ cm$^{2}$V$^{-1}$s$^{-1}$ by gating voltage. Our results reveal the important roles of both carrier mobility and subband occupancy in tuning the quantum transport at oxide interfaces., Comment: 22 pages, 4 figures

A thin Hafnium film is shown to act both as an effective diffusion barrier for manganese at a thickness of 0.7 nm, and as an effective exchange coupling layer in a sandwich structure with perpendicular magnetic anisotropy. The magnetic layers are Co$_{20}$Fe$_{60}$B$_{20}$ and the low moment ferrimagnet Mn$_2$Ru$_x$Ga (MRG). The coupling changes sign at the compensation temperature of MRG and the exchange energy reaches 0.11 mJm$^{-2}$ for the thinnest Hf interlayers. Ruthenium, the usual metal of choice for coupling ferromagnetic layers in thin film heterostructures, cannot be used with the zero-moment half metal MRG because of Ru interdiffusion. Due to its large coercivity near compensation, the MRG can act as an effective source of exchange pinning.

Ferrimagnetic Mn$_2$Fe$_x$Ga $(0.26 \leq x \leq 1.12)$ thin films have been characterised by X-ray diffraction, SQUID magnetometry, X-ray absorption spectroscopy, X-ray magnetic circular dichroism and M\"{o}ssbauer spectroscopy with the aim of determining the structure and site-specific magnetism of this tetragonal, D0$_{22}$-structure Heusler compound. High-quality epitaxial films with low RMS surface roughness ($\sim 0.6$ nm) are grown by magnetron co-sputtering. The tetragonal distortion induces strong perpendicular magnetic anisotropy along the $c$-axis with a typical coercive field $\mu_0 H\sim 0.8$ T and an anisotropy field ranging from $6$ to $8$ T. Upon increasing the Fe content $x$, substantial uniaxial anisotropy, $K_\mathrm{u} \geq 1.0$ MJ/m$^3$ can be maintained over the full $x$ range, while the magnetisation of the compound is reduced from $400$ to $280$ kA/m. The total magnetisation is almost entirely given by the sum of the spin moments originating from the ferrimagnetic Mn and Fe sublattices, with the latter being coupled ferromagnetically to one of the former. The orbital magnetic moments are practically quenched, and have negligible contributions to the magnetisation. The films with $x=0.73$ exhibit a high anomalous Hall angle of $2.5$ % and a high Fermi-level spin polarisation, above $51$ %, as measured by point contact Andreev reflection. The Fe-substituted Mn$_2$Ga films are highly tunable with a unique combination of high anisotropy, low magnetisation, appreciable spin polarisation and low surface roughness, making them very strong candidates for thermally-stable spin-transfer-torque switching nanomagnets with lateral dimensions down to $10$ nm., Comment: 11 pages, 11 figures

SrTiO3 plays a central role in oxide electronics. It is the substrate of choice for functional oxide heterostructures based on perovskite-structure thin-film stacks, and its surface or interface with a polar oxide such as LaAlO3 can become a two-dimensional conductor because of electronic reconstruction or the presence of oxygen defects. Inconsistent reports of magnetic order in SrTiO3 abound in the literature. Here we report a systematic experimental study aimed at establishing how and when SrTiO3 can develop a magnetic moment at room temperature. Polished 100, 110 or 111 crystal slices from four different suppliers are characterized before and after vacuum annealing at 750 {\deg}C, both in single-crystal and powdered form. Impurity content is analysed at the surface and in the bulk. Besides the underlying intrinsic diamagnetism of SrTiO3, magnetic signals are of three types-a Curie law susceptibility due to dilute magnetic impurities at the ppm level, a hysteretic, temperature-dependent ferromagnetic impurity contribution, and a practically-anhysteretic, defect-related temperature-independent component that saturates in about 200 mT. The latter component is intrinsic. It is often the largest, reaching 10 Bohr magnetons per nm2 of surface area or more and dominating the magnetic response in low fields at room temperature. It is associated with defects near the surface, and can be destroyed by treatment with Tiron (C6H4Na2O8S2), an electron donor molecule that forms a strong complex with titanium at the surface. The origin of this unusual high-temperature ferromagnetic-like response is discussed.

The magnetism of nanoparticles and thin films of wide-bandgap oxides that include no magnetic cations is an unsolved puzzle. Progress has been hampered both by the irreproducibility of much of the experimental data, and the lack of any generally-accepted theoretical explanation. The characteristic signature is a virtually anhysteretic, temperature-independent magnetization curve which saturates in an applied field that is several orders of magnitude greater than the magnetization. It appears as if a tiny volume fraction, < 0.1%, of the samples is magnetic and that the energy scale of the problem is unusually high for spin magnetism. Here we investigate the effect of dispersing 4 nm CeO2 nanoparticles with powders of gamma-Al2O3, sugar or latex microspheres. The saturation magnetization, Ms ~ 60 A/m for compact samples, is maximized by 1 wt% lanthanum doping. Dispersing the CeO2 nanopowder reduces its magnetic moment by up to an order of magnitude. There is a characteristic length scale of order 100 nm for the magnetism to appear in CeO2 nanoparticle clusters. The phenomenon is explained in terms of a giant orbital paramagnetism that appears in coherent mesoscopic domains due to resonant interaction with zero-point fluctuations of the vacuum electromagnetic field. The theory explains the observed temperature-independent magnetization curve and its doping and dispersion dependence, based on a length scale of 300 nm that corresponds to the wavelength of a maximum in the UV absorption spectrum of the magnetic CeO2 nanoparticles. The coherent domains occupy roughly ten percent of the sample volume.

When current flows through a magnetic tunnel junction (MTJ), there is spin accumulation at the electrode-barrier interfaces if the magnetic moments of the two ferromagnetic electrodes are not aligned. Here we report that such nonequilibrium spin accumulation generates its own characteristic low frequency noise (LFN). Past work viewed the LFN in MTJs as an equilibrium effect arising from resistance fluctuations ($S_R$) which a passively applied current ($I$) converts to measurable voltage fluctuations ($S_{V}=I^{2}S_{R}$). We treat the LFN associated with spin accumulation as a nonequilibrium effect, and find that the noise power can be fitted in terms of the spin-polarized current by $S_{I}f=aI\coth(\frac{I}{b})-ab$, resembling the form of the shot noise for a tunnel junction, but with current now taking the role of the bias voltage, and spin-flip probability taking the role of tunneling probability., Comment: 6 pages, 5 figures

Recent experimental work on Mn2RuxGa demonstrates its potential as a compensated ferrimagnetic half-metal (CFHM).Here we present a set of high-throughput ab initio density functional theory calculations and detailed experimental characterisation, that enable us to correctly describe the nominal Mn2RuxGa thin films, in particular with regard to site-disorder and defects. We then construct models that accurately capture all the key features of the Mn-Ru-Ga system, including magnetic compensation and the spin gap at the Fermi level. We find that electronic doping is neccessary, which is achieved with a Mn/Ga ratio smaller than two. Our study shows how composition and substrate-induced biaxial strain can be combined to design the first room-temperature CFHM., Comment: 5 pages + 4 pages supplementary material

Since the discovery of two-dimensional electron gas (2DEG) at the oxide interface of LaAlO3/SrTiO3, improving carrier mobility has become an important issue for device applications. In this paper, by using an alternate polar perovskite insulator (La0.3Sr0.7)(Al0.65Ta0.35)O3 (LSAT) for reducing lattice mismatch from 3.0% to 1.0%, the low-temperature carrier mobility has been increased 30 fold to 35,000 cm2V-1s-1. Moreover, two critical thicknesses for the LSAT/SrTiO3 (001) interface are found: one at 5 unit cell for appearance of the 2DEG, the other at 12 unit cell for a peak in the carrier mobility. By contrast, the conducting (110) and (111) LSAT/STO interfaces only show a single critical thickness of 8 unit cells. This can be explained in terms of polar fluctuation arising from LSAT chemical composition. In addition to lattice mismatch and crystal symmetry at the interface, polar fluctuation arising from composition has been identified as an important variable to be tailored at the oxide interfaces to optimise the 2DEG transport., Comment: 17 pages, 4 figures

The discovery of materials with improved functionality can be accelerated by rational material design. Heusler compounds with tunable magnetic sublattices allow to implement this concept to achieve novel magnetic properties. Here, we have designed a family of Heusler alloys with a compensated ferrimagnetic state. In the vicinity of the compensation composition in Mn-Pt-Ga, a giant exchange bias (EB) of more than 3 T and a similarly large coercivity are established. The large exchange anisotropy originates from the exchange interaction between the compensated host and ferrimagnetic clusters that arise from intrinsic anti-site disorder. We demonstrate the applicability of our design concept on a second material, Mn-Fe-Ga, with a magnetic transition above room temperature, exemplifying the universality of the concept and the feasibility of room-temperature applications. Our study points to a new direction for novel magneto-electronic devices. At the same time it suggests a new route for realizing rare-earth free exchange-biased hard magnets, where the second quadrant magnetization can be stabilized by the exchange bias., Comment: Four figures

We report on the low frequency (LF) noise measurements in magnetic tunnel junctions (MTJs) below 4 K and at low bias, where the transport is strongly affected by scattering with magnons emitted by hot tunnelling electrons, as thermal activation of magnons from the environment is suppressed. For both CoFeB/MgO/CoFeB and CoFeB/AlO$_{x}$/CoFeB MTJs, enhanced LF noise is observed at bias voltage around magnon emission energy, forming a peak in the bias dependence of noise power spectra density, independent of magnetic configurations. The noise peak is much higher and broader for unannealed AlO$_{x}$-based MTJ, and besides Lorentzian shape noise spectra in the frequency domain, random telegraph noise (RTN) is visible in the time traces. During repeated measurements the noise peak reduces and the RTN becomes difficult to resolve, suggesting defects being annealed. The Lorentzian shape noise spectra can be fitted with bias-dependent activation of RTN, with the attempt frequency in the MHz range, consistent with magnon dynamics. These findings suggest magnon-assisted activation of defects as the origin of the enhanced LF noise., Comment: 6 pages, 5 figures

We provide conclusive experimental evidence that zero bias anomaly in the differential resistance of magnetic tunnel junctions (MTJs) is due to electron-electron interaction (EEI), clarifying a long standing issue. Magnon effect that caused confusion is now excluded by measuring at low temperatures down to 0.2 K and with reduced AC measurement voltages down to 0.06 mV. The normalized change of conductance is proportional to $\ln{(eV/k_{B}T)}$, consistent with the Altshuler-Aronov theory of tunneling that describes the reduction of density of states due to EEI, but inconsistent with magnetic impurity scattering. The slope of the $\ln{(eV/k_{B}T)}$ dependence is symmetry dependent: the slopes for P and AP states are different for coherent tunnel junctions with symmetry filtering, while nearly the same for those without symmetry filtering (amorphous barriers). This observation may be helpful for verifying symmetry preserved filtering in search of new coherent tunneling junctions, and for probing and separating electron Bloch states of different symmetries in other correlated systems., Comment: preprint, 22 pages, 7 figures, expanded introduction

Atomically sharp oxide heterostructures often exhibit unusual physical properties that are absent in the constituent bulk materials. The interplay between electrostatic boundary conditions, strain and dimensionality in ultrathin epitaxial films can result in monolayer-scale transitions in electronic or magnetic properties. Here we report an atomically sharp antiferromagnetic-to-ferromagnetic phase transition when atomically growing polar antiferromagnetic LaMnO3 (001) films on SrTiO3 substrates. For a thickness of five unit cells or less, the films are antiferromagnetic, but for six unit cells or more, the LaMnO3 film undergoes a phase transition to a ferromagnetic state over its entire area, which is visualized by scanning superconducting quantum interference device microscopy. The transition is explained in terms of electronic reconstruction originating from the polar nature of the LaMnO3 (001) films. Our results demonstrate how new emergent functionalities can be visualized and engineered in atomically thick oxide films at the atomic level.