Victor Ukleev, Oleg I. Utesov, Chen Luo, Florin Radu, Sebastian Wintz, Markus Weigand, Simone Finizio, Moritz Winter, Alexander Tahn, Bernd Rellinghaus, Kosuke Karube, Yoshinori Tokura, Yasujiro Taguchi, Jonathan S. White The cubic $\beta$-Mn-type alloy Co$_8$Zn$_8$Mn$_4$ is a chiral helimagnet that exhibits a peculiar temperature-dependent behavior in the spiral pitch, which decreases from 130 nm at room temperature to 70 nm below 20 K. Notably, this shortening is also accompanied by a structural transition of the metastable skyrmion texture, transforming from a hexagonal lattice to a square lattice of elongated skyrmions. The underlying mechanism of these transformations remain unknown, with interactions potentially involved including temperature-dependent Dzyaloshinskii-Moriya interaction, magnetocrystalline anisotropy, and exchange anisotropy. Here, x-ray resonant magnetic small-angle scattering in vectorial magnetic fields was employed to investigate the temperature dependence of the anisotropic properties of the helical phase in Co$_8$Zn$_8$Mn$_4$. Our results reveal quantitatively that the magnitude of the anisotropic exchange interaction increases by a factor of 4 on cooling from room temperature to 20 K, leading to a 5% variation in the helical pitch within the (001) plane at 20 K. While anisotropic exchange interaction contributes to the shortening of the spiral pitch, its magnitude is insufficient to explain the variation in the spiral periodicity from room to low temperatures. Finally, we demonstrate that magnetocrystalline and exchange anisotropies compete, favoring different orientations of the helical vector in the ground state.
Victor Ukleev, Fernando Ajejas, Anton Devishvili, Alexei Vorobiev, Nina-Juliane Steinke, Robert Cubitt, Chen Luo, Radu-Marius Abrudan, Florin Radu, Vincent Cros, Nicolas Reyren, Jonathan S. White We report investigations of the magnetic textures in periodic [Pt(1 nm)/(CoFeB(0.8 nm)/Ru(1.4 nm)]$_{10}$ multilayers using polarised neutron reflectometry (PNR) and small-angle neutron scattering (SANS). The multilayers are known to host skyrmions stabilized by Dzyaloshinskii-Moriya interactions induced by broken inversion symmetry and spin-orbit coupling at the asymmetric interfaces. From depth-dependent PNR measurements, we observe well-defined structural features, and obtain the layer-resolved magnetization profiles. The in-plane magnetization of the CoFeB layers calculated from fitting of the PNR profiles is found to be in excellent agreement with magnetometry data. Using SANS as a bulk probe of the entire multilayer, we observe long-period magnetic stripe domains and skyrmion ensembles with full orientational disorder at room temperature. No sign of skyrmions is found below 250\u2009K, which we suggest is due to an increase of a effective magnetic anisotropy in the CoFeB layer on cooling that suppresses skyrmion stability. Using polarised SANS at room temperature, we prove the existence of pure Néel-type windings in both stripe domain and skyrmion regimes. No Bloch-type winding admixture, i.e. an indication for hybrid windings, is detected within the measurement sensitivity, in good agreement with expectations according to our micromagnetic modelling of the multilayers. Our findings using neutron techniques offer valuable microscopic insights into the rich magnetic behavior of skyrmion-hosting multilayers, which are essential for the advancement of future skyrmion-based spintronic devices.
Victor Ukleev, Ludmila Leroy, Riccardo Mincigrucci, Dario Deangelis, Danny Fainozzi, Nupur Ninad Khatu, Ettore Paltanin, Laura Foglia, Filippo Bencivenga, Chen Luo, Florian Ruske, Florin Radu, Cristian Svetina, Urs Staub Surface acoustic waves (SAWs) are excited by femtosecond extreme ultraviolet (EUV) transient gratings (TGs) in a room-temperature ferrimagnetic DyCo$_5$ alloy. TGs are generated by crossing a pair of EUV pulses from a free electron laser (FEL) with the wavelength of 20.8\u2009nm matching the Co $M$-edge, resulting in a SAW wavelength of $\Lambda=44$\u2009nm. Using the pump-probe transient grating scheme in a reflection geometry the excited SAWs could be followed in the time range of -10 to 100\u2009ps in the thin film. Coherent generation of TGs by ultrafast EUV pulses allows to excite SAW in any material and to investigate their couplings to other dynamics such as spin waves and orbital dynamics. In contrast, we encountered challenges in detecting electronic and magnetic signals, potentially due to the dominance of the larger SAW signal and the weakened reflection signal from underlying layers. A potential solution for the latter challenge involves employing soft X-ray probes, albeit introducing additional complexities associated with the required grazing incidence geometry.
The helical magnetic structures of cubic chiral systems are well-explained by the competition among Heisenberg exchange, Dzyaloshinskii-Moriya interaction, cubic anisotropy, and anisotropic exchange interaction (AEI). Recently, the role of the latter has been argued theoretically to be crucial for the low-temperature phase diagram of the cubic chiral magnet Cu$_2$OSeO$_3$, which features tilted conical and disordered skyrmion states for a specific orientation of the applied magnetic field ($\mu_0 \vec{\mathrm{H}} \parallel [001]$). In this study, we exploit transmission resonant x-ray scattering ($t-$REXS) in vector magnetic fields to directly quantify the strength of the AEI in Cu$_2$OSeO$_3$, and measure its temperature dependence. We find that the AEI continuously increases below 50\u2009K, resulting in a conical spiral pitch variation of $10\%$ in the (001) plane. Our results contribute to establishing the interaction space that supports tilted cone and low-temperature skyrmion state formation, facilitating the goals for both a quantitative description and eventual design of the diverse spiral states existing amongst chiral magnets.
Isolated magnetic skyrmions are stable, topologically protected spin textures that are at the forefront of research interests today due to their potential applications in information technology. A distinct class of skyrmion hosts are rare earth - transition metal (RE-TM) ferrimagnetic materials. To date, the nature and the control of basic traits of skyrmions in these materials are not fully understood. We show that for an archetypal ferrimagnetic material DyCo$_3$ that exhibits a strong perpendicular anisotropy, the ferrimagnetic skyrmion size can be tuned by an external magnetic field. Moreover, by taking advantage of the high spatial resolution of scanning transmission X-ray microscopy (STXM) and utilizing a large x-ray magnetic linear dichroism (XMLD) contrast that occurs naturally at the RE resonant edges, we resolve the nature of the magnetic domain walls of ferrimagnetic skyrmions. We demonstrate that through this method one can easily discriminate between Bloch and Néel type domain walls for each individual skyrmion. For all isolated ferrimagnetic skyrmions, we observe that the domain walls are of Néel-type. This key information is corroborated with results of micromagnetic simulations and allows us to conclude on the nature of the Dzyaloshinskii-Moriya interaction (DMI) which concurs to the stabilisation of skyrmions in this ferrimagnetic system. Establishing that an intrinsic DMI occurs in RE-TM materials will also be beneficial towards a deeper understanding of chiral spin texture control in ferrimagnetic materials.
S. E. Hadjadj, C. González-Orellana, J. Lawrence, D. Bikaljević, M. Peña-Díaz, P. Gargiani, L. Aballe, J. Naumann, M. Á. Niño, M. Foerster, S. Ruiz-Gómez, S. Thakur, I. Kumberg, J. Taylor, J. Hayes, J. Torres, C. Luo, F. Radu, D. G. de Oteyza, W. Kuch, et al (3) Magnetic two-dimensional (2D) semiconductors have attracted a lot of attention because modern preparation techniques are capable of providing single crystal films of these materials with precise control of thickness down to the single-layer limit. It opens up a way to study rich variety of electronic and magnetic phenomena with promising routes towards potential applications. We have investigated the initial stages of epitaxial growth of the magnetic van der Waals semiconductor FeBr\textsubscript2 on a single-crystal Au(111) substrate by means of low-temperature scanning tunneling microscopy, low-energy electron diffraction, x-ray photoemission spectroscopy, low-energy electron emission microscopy and x-ray photoemission electron microscopy. Magnetic properties of the one- and two-layer thick films were measured via x-ray absorption spectroscopy/x-ray magnetic circular dichroism. Our findings show a striking difference in the magnetic behaviour of the single layer of FeBr\textsubscript2 and its bulk counterpart, which can be attributed to the modifications in the crystal structure due to the interaction with the substrate.
In rare-earth compounds with valence fluctuation, the proximity of the 4f level to the Fermi energy leads to instabilities of the charge configuration and the magnetic moment. Here, we provide direct experimental evidence for an induced magnetic polarization of the Eu$^{3+}$ atomic shell with J=0, due to intra-atomic exchange and spin-orbital coupling interactions with Eu$^{2+}$ atomic shell. By applying external pressure, a transition from antiferromagnetic to a fluctuating behavior in a EuNiGe$_3$ single crystals is probed. Magnetic polarization is observed for both valence states of Eu$^{2+}$ and Eu$^{3+}$ across the entire pressure range. The anomalous magnetism is discussed in terms of a homogeneous intermediate valence state where frustrated Dzyaloshinskii-Moriya couplings are enhanced by the onset of spin-orbital interaction and engender a chiral spin-liquid-like precursor.
Resonant elastic soft x-ray magnetic scattering (XRMS) is a powerful tool to explore long-periodic spin textures in single crystals. However, due to the limited momentum transfer range imposed by long wavelengths of photons in the soft x-ray region, Bragg diffraction is restricted to crystals with the large lattice parameters. Alternatively, small angle x-ray scattering has been involved in the soft energy x-ray range which, however, brings in difficulties with the sample preparation that involves focused ion beam milling to thin down the crystal to below a few hundred nm thickness. We show how to circumvent these restrictions by using XRMS in specular reflection from a sub-nanometer smooth crystal surface. The method allows observing diffraction peaks from the helical and conical spin modulations at the surface of a Cu$_2$OSeO$_3$ single crystal and probing their corresponding chirality as contributions to the dichroic scattered intensity. The results suggest a promising way to carry out XRMS studies on plethora of noncentrosymmetric systems hitherto unexplored with soft x-rays due to the absence of the commensurate Bragg peaks in the available momentum transfer range.
T. Ferté, M. Beens, G. Malinowski, K. Holldack, R. Abrudan, F. Radu, T. Kachel, M. Hehn, C. Boeglin, B. Koopmans, N. Bergeard We have studied the laser induced ultrafast quenching of Gd 4f magnetic order in ferrimagnetic Co100-xGdx alloys to highlight the role of the inter-atomic exchange coupling. We have taken advantage of the ultrashort soft X-ray pulses deliver by the femtoslicing beamline at the BESSY II synchrotron radiation source at the Helmholtz-Zentrum Berlin to perform element- and time-resolved X-ray Magnetic Circular Dichroism spectroscopy.Our results show that the laser induced quenching of Gd 4f magnetic order occurs on very different time-scales for the Co72Gd28, the Co77Gd23 and the Co79Gd21 alloys. Most of the magnetic moment losses occur within the first picosecond (ps) while the electron distribution is strongly out of equilibrium. After the equilibration of the electrons and lattice temperatures (t > 1 ps), the magnetic losses occur on slower rates that depend on the alloy composition: increasing the Co composition speeds up the demagnetization of Gd 4f sublattice. The strength of the inter-atomic exchange coupling which depends on composition, determines the efficiency of the angular momentum flow from the Gd 4f spin towards the lattice. Our results are in qualitative agreements with the predictions of the microscopic three temperatures model for ferrimagnetic alloys.
Nanna Zhou Hagström, Michael Schneider, Nico Kerber, Alexander Yaroslavtsev, Erick Burgos Parra, Marijan Beg, Martin Lang, Christian M. Günther, Boris Seng, Fabian Kammerbauer, Horia Popescu, Matteo Pancaldi, Kumar Neeraj, Debanjan Polley, Rahul Jangid, Stjepan B. Hrkac, Sheena K. K. Patel, Sergei Ovcharenko, Diego Turenne, Dmitriy Ksenzov, et al (80) The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence, and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, we present the results from the first megahertz repetition rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL. We illustrate the experimental capabilities that the SCS instrument offers, resulting from the operation at MHz repetition rates and the availability of the novel DSSC 2D imaging detector. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.
K. Prokeš, Chen Luo, H. Ryll, E. Schierle, D. Marchenko, E. Weschke, F. Radu, R. Abrudan, V. V. Volobuev, G. Springholz, O. Rader Enhanced magnetism has recently been reported for the topological-insulator/ferromagnet interface Bi$_2$Se$_3$/EuS with Curie temperatures claimed to be raised above room temperature from the bulk EuS value of 16 K. Here we investigate the analogous interface Bi$_2$Se$_3$/EuSe. EuSe is a low-temperature layered ferrimagnet that is particularly sensitive to external perturbations. We find that superconducting quantum interference device (SQUID) magnetometry of Bi$_2$Se$_3$/EuSe heterostructures reveals precisely the magnetic phase diagram known from EuSe, including the ferrimagnetic phase below 5 K, without any apparent changes from the bulk behavior. Choosing a temperature of 10 K to search for magnetic enhancement, we determine an upper limit for a possible magnetic coercive field of 3 mT. Using interface sensitive x-ray absorption spectroscopy we verify the magnetic divalent configuration of the Eu at the interface without contamination by Eu3+, and by x-ray magnetic circular dichroism (XMCD) we confirm at the interface the magnetic hysteresis obtained by SQUID. XMCD data obtained at 10 K in a magnetic field of 6 T indicate a magnetic spin moment of mz,spin = 7 $\mu$B/Eu$^{2+}$, in good agreement with the SQUID data and the expected theoretical moment of Eu2+. Subsequent XMCD measurements in zero field show, however, that sizable remanent magnetization is absent at the interface for temperatures down to about 10 K.
Boris Seng, Daniel Schönke, Javier Yeste, Robert M. Reeve, Nico Kerber, Daniel Lacour, Jean-Loïs Bello, Nicolas Bergeard, Fabian Kammerbauer, Mona Bhukta, Tom Ferté, Christine Boeglin, Florin Radu, Radu Abrudan, Torsten Kachel, Stéphane Mangin, Michel Hehn, Mathias Kläui The evolution of chiral spin structures is studied in ferrimagnet Ta/Ir/Fe/GdFeCo/Pt multilayers as a function of temperature using scanning electron microscopy with polarization analysis (SEMPA). The GdFeCo ferrimagnet exhibits pure right-hand Néel-type domain wall (DW) spin textures over a large temperature range. This indicates the presence of a negative Dzyaloshinskii-Moriya interaction (DMI) that can originate from both the top Fe/Pt and the Co/Pt interfaces. From measurements of the DW width, as well as complementary magnetic characterization, the exchange stiffness as a function of temperature is ascertained. The exchange stiffness is surprisingly mostly constant, which is explained by theoretical predictions. Beyond single skyrmions, we find by direct imaging a pure Néel-type skyrmionium, which due to the absence of a skyrmion Hall angle is a promising topological spin structure to enable high impact potential applications in the next generation of spintronic devices.
Tom S. Seifert, Ulrike Martens, Florin Radu, Mirkow Ribow, Marco Berritta, Lukas Nádvorník, Ronald Starke, Tomas Jungwirth, Martin Wolf, Ilie Radu, Markus Münzenberg, Peter M. Oppeneer, Georg Woltersdorf, Tobias Kampfrath The anomalous Hall effect (AHE) is a fundamental spintronic charge-to-charge-current conversion phenomenon and closely related to spin-to-charge-current conversion by the spin Hall effect. Future high-speed spintronic devices will crucially rely on such conversion effects at terahertz (THz) frequencies. Here, we reveal that the AHE remains operative from DC up to 40 THz with a flat frequency response in thin films of three technologically relevant magnetic materials: DyCo$_{5}$, Co$_{32}$Fe$_{68}$ and Gd$_{27}$Fe$_{73}$. We measure the frequency-dependent conductivity-tensor elements ${\sigma}_{xx}$ and ${\sigma}_{yx}$ and find good agreement with DC measurements. Our experimental findings are fully consistent with ab-initio calculations of ${\sigma}_{yx}$ for CoFe and highlight the role of the large Drude scattering rate (~100 THz) of metal thin films, which smears out any sharp spectral features of the THz AHE. Finally, we find that the intrinsic contribution to the THz AHE dominates over the extrinsic mechanisms for the Co$_{32}$Fe$_{68}$ sample. The results imply that the AHE and related effects such as the spin Hall effect are highly promising ingredients of future THz spintronic devices reliably operating from DC to 40 THz and beyond.
E. Golias, E. Weschke, T. Flanagan, E. Schierle, A. Richardella, E. D. L. Rienks, P. S. Mandal, A. Varykhalov, J. Sánchez-Barriga, F. Radu, N. Samarth, O. Rader V-doped (Bi,Sb)$_2$Te$_3$ has a ten times higher magnetic coercivity than its Cr-doped counterpart and therefore is believed to be a superior system for the quantum anomalous Hall effect (QAHE). The QAHE requires the opening of a magnetic band gap at the Dirac point. We do not find this gap by angle-resolved photoelectron spectroscopy down to 1 K. By x-ray magnetic circular dichroism (XMCD) we directly probe the magnetism at the V site and in zerofield. Hysteresis curves of the XMCD signal show a strong dependence of the coercivity on the ramping velocity of the magnetic field. The XMCD signal decays on a time scale of minutes which we conclude contributes to the absence of a detectable magnetic gap at the Dirac point.
Owing to the experimental discovery of magnetic skyrmions stabilized by the Dzyaloshinskii-Moriya and/or dipolar interactions in thin films, there is a recent upsurge of interest in magnetic skyrmions with antiferromagnetic spins in order to overcome the fundamental limitations inherent with skyrmions in ferromagnetic materials. Here, we report on the observation of compact ferrimagnetic skyrmions for the class of amorphous alloys consisting of 4f rare-earth and 3d transition-metal elements with perpendicular magnetic anisotropy, using a DyCo$_3$ film, that are identified by combining x-ray magnetic scattering, scanning transmission x-ray microscopy, and Hall transport technique. These skyrmions, with antiparallel aligned Dy and Co magnetic moments and a characteristic core radius of about 40~nm, are formed during the nucleation and annihilation of the magnetic maze-like domain pattern exhibiting a topological Hall effect contribution. Our findings provide a promising route for fundamental research in the field of ferrimagnetic/antiferromagnetic spintronics towards practical applications.
Long before the recent fascination with two-dimensional materials, the critical behaviour and universality scaling of phase transitions in low-dimensional systems has been a topic of great interest. Particularly intriguing is the case of long-range magnetic order in two dimensions, once considered to be excluded in systems with continuous symmetry by the Hohenberg-Mermin-Wagner theorem. While an out-of-plane anisotropy has been shown to stabilize 2D magnetic order, this proof has remained elusive for a 2D magnet with in-plane rotational symmetry. Here, we construct a nearly ideal easy-plane system, a CrCl3 monolayer grown on Graphene/6H-SiC (0001), and unambiguously demonstrate robust in-plane ferromagnetic ordering with a critical scaling behaviour characteristic of a 2D-XY system. These observations suggest the first realization of a finite-size Berezinskii-Kosterlitz-Thouless (BKT) phase transition in a large-area, quasi-freestanding, van der Waals monolayer magnet with a XY universality class; and further constitute an ideal platform to study exotic phenomena like superfluid spin transport or 2D topological in-plane spin textures -- such as merons.
Charge transfer induced interfacial ferromagnetism and its impact on the exchange bias effect in La0.7Sr0.3MnO3/NdNiO3 correlated oxide heterostructures were investigated by soft x-ray ab?sorption and x-ray magnetic circular dichroism spectra in a temperature range from 10 to 300 K. Besides the antiferromagnetic Ni3+ cations which are naturally part of the NdNiO3 layer, Ni2+ ions are formed at the interface due to a charge transfer mechanism involving the Mn element of the adjacent layer. They exhibit a ferromagnetic behavior due to the exchange coupling to the Mn4+ ions in the La0.7Sr0.3MnO3 layer. This can be seen as detrimental to the strength of the unidirec?tional anisotropy since a significant part of the interface does not contribute to the pinning of the ferromagnetic layer. By analyzing the line shape changes of the x-ray absorption at the Ni L2,3 edges, the metal-insulator transition of the NdNiO3 layer is resolved in an element specific manner. This phase transition is initiated at about 120 K, way above the paramagnetic to antiferromagnetic transition of NdNiO3 layer which measured to be 50 K. Exchange bias and enhanced coercive fields were observed after field cooling the sample through the Neel temperature of the NdNiO3 layer. Different from La0.7Sr0.3MnO3/LaNiO3, the exchange bias observed in La0.7Sr0.3MnO3/NdNiO3 is due to the antiferromagnetism of NdNiO3 and the frustration at the interface. These results suggest that reducing the interfacial orbital hybridization may be used as a tunable paramater for the strength of the exchange bias effect in all-oxide heterostructures which exhibit a charge transfer mechanism.
Noncollinear antiferromagnets with a D0$_{19}$ (space group = 194, P6$_{3}$/mmc) hexagonal structure have garnered much attention for their potential applications in topological spintronics. Here, we report the deposition of continuous epitaxial thin films of such a material, Mn$_{3}$Sn, and characterize their crystal structure using a combination of x-ray diffraction and transmission electron microscopy. Growth of Mn$_{3}$Sn films with both (0001) c-axis orientation and (40$\bar{4}$3) texture is achieved. In the latter case, the thin films exhibit a small uncompensated Mn moment in the basal plane, quantified via magnetometry and x-ray magnetic circular dichroism experiments. This cannot account for the large anomalous Hall effect simultaneously observed in these films, even at room temperature, with magnitude $\sigma_{\mathrm{xy}}$ ($\mu_{0}H$ = 0 T) = 21 $\mathrm{\Omega}^{-1}\mathrm{cm}^{-1}$ and coercive field $\mu_{0}H_{\mathrm{C}}$ = 1.3 T. We attribute the origin of this anomalous Hall effect to momentum-space Berry curvature arising from the symmetry-breaking inverse triangular spin structure of Mn$_{3}$Sn. Upon cooling through the transition to a glassy ferromagnetic state at around 50 K, a peak in the Hall resistivity close to the coercive field indicates the onset of a topological Hall effect contribution, due to the emergence of a scalar spin chirality generating a real-space Berry phase. We demonstrate that the polarity of this topological Hall effect, and hence the chiral-nature of the noncoplanar magnetic structure driving it, can be controlled using different field cooling conditions.
Cubic chiral magnets, such as Cu$_{2}$OSeO$_{3}$, exhibit a variety of non-collinear spin textures, including a trigonal lattice of spin whirls, so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at GHz frequencies, we probe the ferromagnetic resonance modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS-FMR, is carried out at distinct positions in reciprocal space, it allows to distinguish contributions originating from different magnetic states, providing information on the precise character, weight and mode mixing as a prerequisite of tailored excitations for applications.
James M. Taylor, Edouard Lesne, Anastasios Markou, Fasil Kidane Dejene, Pranava Keerthi Sivakumar, Simon Pöllath, Kumari Gaurav Rana, Neeraj Kumar, Chen Luo, Hanjo Ryll, Florin Radu, Florian Kronast, Peter Werner, Christian H. Back, Claudia Felser, Stuart S. P. Parkin Non-collinear antiferromagnets, with either an L1$_{2}$ cubic crystal lattice (e.g. Mn$_{3}$Ir and Mn$_{3}$Pt) or a D0$_{19}$ hexagonal structure (e.g. Mn$_{3}$Sn and Mn$_{3}$Ge), exhibit a number of novel phenomena of interest to topological spintronics. Amongst the cubic systems, for example, tetragonally distorted Mn$_{3}$Pt exhibits an intrinsic anomalous Hall effect (AHE). However, Mn$_{3}$Pt only enters a non-collinear magnetic phase close to the stoichiometric composition and at suitably large thicknesses. Therefore, we turn our attention to Mn$_{3}$Ir, the material of choice for use in exchange bias heterostructures. In this paper, we investigate the magnetic and electrical transport properties of epitaxially grown, face-centered-cubic $\gamma$-Mn$_{3}$Ir thin films with (111) crystal orientation. Relaxed films of 10 nm thickness exhibit an ordinary Hall effect, with a hole-type carrier concentration of (2.24 $\pm$ 0.08) $\times$ 10$^{23}$ cm$^{-3}$. On the other hand, TEM characterization demonstrates that ultrathin 3 nm films grow with significant in-plane tensile strain. This may explain a small remanent moment, observed at low temperatures, shown by XMCD spectroscopy to arise from uncompensated Mn spins. Of the order 0.02 $\mu_{B}$ / atom, this dominates electrical transport behavior, leading to a small AHE and negative magnetoresistance. These results are discussed in terms of crystal microstructure and chiral domain behavior, with spatially resolved XML(C)D-PEEM supporting the conclusion that small antiferromagnetic domains, < 20 nm in size, of differing chirality account for the absence of observed Berry curvature driven magnetotransport effects.
Ferrimagnetic alloys are extensively studied for their unique magnetic properties leading to possible applications in perpendicular magnetic recording, due to their deterministic ultrafast switching and heat assisted magnetic recording capabilities. On a prototype ferrimagnetic alloy we demonstrate fascinating properties that occur close to a critical temperature where the magnetization is vanishing, just as in an antiferromagnet. From the X-ray magnetic circular dichroism measurements, an anomalous 'wing shape' hysteresis loop is observed slightly above the compensation temperature. This bears the characteristics of an intrinsic exchange bias effect, referred to as atomic exchange bias. We further exploit the X-ray magnetic linear dichroism (XMLD) contrast for probing non-collinear states which allows us to discriminate between two main reversal mechanisms, namely perpendicular domain wall formation versus spin-flop transition. Ultimately, we analyze the elemental magnetic moments for the surface and the bulk parts, separately, which allows to identify in the phase diagram the temperature window where this effect takes place. Moreover, we suggests that this effect is a general phenomenon in ferrimagnetic thin films which may also contribue to the understanding of the mechanism behind the all optical switching effect.
We describe a new sensitive method for the investigation of weakly magnetic films placed inside a tri-layer planar waveguide. Polarized neutrons tunnel into the waveguide through the surface, channel along the layers and are emitted from the end face as a narrow and slightly divergent microbeam. Polarization analysis permits to detect very small magnetization in the order of a few 10 Gauss. The magnetic film containing the rare-earth element Tb was investigated using both fixed wavelength and time-of-flight polarized neutron reflectometers. The experimental results are presented and discussed.
Neutron planar waveguides are focusing devices generating a narrow neutron beam of submicron width. Such a neutron microbeam can be used for the investigation of local microstructures with high spatial resolution. The essential parameter of the microbeam is its angular width. The main contribution to the microbeam angular divergence is Fraunhofer diffraction on a narrow slit. We review and discuss various ways to characterize the angular divergence of the neutron microbeam using time-of-flight and fixed wavelength reflectometers.
The triangular spin lattice of NiBr$_{2}$ is a canonical example of a frustrated helimagnet that shows a temperature-driven phase transition from a collinear commensurate antiferromagnetic structure to an incommensurate spin helix on cooling. Employing neutron diffraction, bulk magnetization, and magnetic susceptibility measurements, we have studied the f\hspace*.5ptield-induced magnetic states of the NiBr$_{2}$ single crystal. Experimental f\hspace*.5ptindings enable us to recapitalize the driving forces of the spin spiral ordering in the triangular spin-lattice systems, in general. Neutron diffraction data conf\hspace*.5ptirms, at low temperature below T$_{{\rm m}}$ = 22.8(1) K, the presence of diffraction satellites characteristic of an incommensurate magnetic state, which are symmetrically arranged around main magnetic reflections that evolve just below T$_{{\rm N}}$ = 44.0(1) K. Interestingly, a f\hspace*.5ptield-induced transition from the incommensurate to commensurate spin phase has been demonstrated that enforces spin helix to restore the high temperature compensated antiferromagnetic structure. This spin reorientation can be described as a spin-flop transition in the (\hbox$a$--$b$) basal plane of a triangular spin lattice system. These f\hspace*.5ptindings offer a new pathway to control the spin helix in incommensurate phases that are currently considered having high technical implications in the next-generation data storage devices.
We investigate neutron propagation in a middle layer of a planar waveguide which is a tri-layer thin film. A narrow divergent microbeam emitted from the end face of the film is registered. The neutron channeling length is experimentally measured as a function of the guiding channel width. Experimental results are compared with calculations.
Mn$_2$Au is an important antiferromagnetic (AF) material for spintronics applications. Due to its very high Néel temperature of about 1500 K, some of the basic properties are difficult to explore, such as the AF susceptibility and the exchange constants. Experimental determination of these properties is further complicated in thin films by unavoidable presence of uncompensated and quasiloose spins on antisites and at interfaces. Using x-ray magnetic circular dichroism (XMCD), we have measured the spin and orbital contribution to the susceptibility in the direction perpendicular to the in-plane magnetic moments of a Mn$_2$Au(001) film and in fields up to 8 T. By performing these measurements at a low temperature of 7 K and at room temperature, we were able to separate the loose spin contribution from the susceptibility of AF coupled spins. The value of the AF exchange constant obtained with this method for a 10 nm thick Mn$_2$Au(001) film equals to (24 $\pm$ 5) meV.
M. Kopte, U. K. Rößler, R. Schäfer, T. Kosub, A. Kákay, O. Volkov, H. Fuchs, E. Y. Vedmedenko, F. Radu, O. G. Schmidt, J. Lindner, J. Faßbender, D. Makarov The magnetic properties of ferromagnetic thin films down to the nanoscale are ruled by the exchange stiffness, anisotropies and the effects of magnetic fields. As surfaces break inversion symmetry, an additional effective chiral exchange is omnipresent in any magnetic nanostructure. These so-called Dzyaloshinskii-Moriya interactions (DMI) affect all inhomogeneous magnetic states either subtly or spectacularly. E.g., DMIs cause a chirality selection of the rotation sense and can fix the local rotation axis for the magnetization in domain walls (DW). But, they can stabilize also entirely different twisted magnetic structures. The chiral skyrmions a two-dimensional particle-like topological soliton is the ultimately smallest of these objects, which currently is targetted as a possible information carrier in novel spintronic devices. Observation and quantification of the chiral exchange effects provide for the salient point in understanding magnetic properties in ultrathin films and other nanostructures. An easy and reliable method to determine the DMI constant as materials parameter of asymmetric thin films is the crucial problem. Here, we put forth an experimental approach for the determination of the complete set of the micromagnetic parameters. Quasi-static Kerr microcopy observations of DW creep motion and equilibrium sizes of circular magnetic objects in combination with standard magnetometry are used to derive a consistent set of these materials parameters in polycrystalline ultrathin film systems, namely CrOx/Co/Pt stacks. The quantified micromagnetic model for these films identifies the circular magnetic objects, as seen by the optical microscopy, as ordinary bubble domains with homochiral walls. From micromagnetic calculations, the chiral skyrmions stabilized by the DMI in these films are shown to have diameters in the range 40-200nm, too small to be observed by optical microscopy.
T. Seifert, U. Martens, S. Günther, M. A. W. Schoen, F. Radu, X. Z. Chen, I. Lucas, R. Ramos, M. H. Aguirre, P. A. Algarabel, A. Anadón, H. Körner, J. Walowski, C. Back, M. R. Ibarra, L. Morellón, E. Saitoh, M. Wolf, C. Song, K. Uchida, et al (3) Terahertz emission spectroscopy of ultrathin multilayers of magnetic and heavy metals has recently attracted much interest. This method not only provides fundamental insights into photoinduced spin transport and spin-orbit interaction at highest frequencies but has also paved the way to applications such as efficient and ultrabroadband emitters of terahertz electromagnetic radiation. So far, predominantly standard ferromagnetic materials have been exploited. Here, by introducing a suitable figure of merit, we systematically compare the strength of terahertz emission from X/Pt bilayers with X being a complex ferro-, ferri- and antiferromagnetic metal, that is, dysprosium cobalt (DyCo$_5$), gadolinium iron (Gd$_{24}$Fe$_{76}$), Magnetite (Fe$_3$O$_4$) and iron rhodium (FeRh). We find that the performance in terms of spin-current generation not only depends on the spin polarization of the magnet's conduction electrons but also on the specific interface conditions, thereby suggesting terahertz emission spectroscopy to be a highly surface-sensitive technique. In general, our results are relevant for all applications that rely on the optical generation of ultrafast spin currents in spintronic metallic multilayers.
Neutron Zeeman spatial beam-splitting is considered at reflection from magnetically noncollinear films. Two applications of Zeeman beam-splitting phenomenon in polarized neutron reflectometry are discussed. One is the construction of polarizing devices with high polarizing efficiency. Another one is the investigations of magnetically noncollinear films with low spin-flip probability. Experimental results are presented for illustration.
Results of experimental investigations of a neutron resonances width in planar waveguides using the time-of-flight reflectometer REMUR of the IBR-2 pulsed reactor are reported and comparison with theoretical calculations is presented. The intensity of the neutron microbeam emitted from the waveguide edge was registered as a function of the neutron wavelength and the incident beam angular divergence. The possible applications of this method for the investigations of layered nanostructures are discussed.
We present and apply a new method to measure directly weak magnetization in thin films. The polarization of a neutron beam channeling through a thin film structure is measured after exiting the structure edge as a microbeam. We have applied the method to a tri-layer thin film structure acting as a planar waveguide for polarized neutrons. The middle guiding layer is a rare earth based ferrimagnetic material TbCo5 with a low magnetization of about 20 mT. We demonstrate that the channeling method is more sensitive than the specular neutron reflection method.
We review different neutron methods which allow extracting directly the value of the magnetic induction in thick films: Larmor precession, Zeeman spatial beam-splitting and neutron spin resonance. Resulting parameters obtained by the neutron methods and standard magnetometry technique are presented and compared. The possibilities and specificities of the neutron methods are discussed.
Increasing the magnetic data recording density requires reducing the size of the individual memory elements of a recording layer as well as employing magnetic materials with temperature-dependent functionalities. Therefore, it is predicted that the near future of magnetic data storage technology involves a combination of energy-assisted recording on nanometer-scale magnetic media. We present the potential of heat-assisted magnetic recording on a patterned sample; a ferrimagnetic alloy composed of a rare earth and a transition metal, DyCo$_5$, which is grown on a hexagonal-ordered nanohole array membrane. The magnetization of the antidot array sample is out-of-plane oriented at room temperature and rotates towards in-plane upon heating above its spin-reorientation temperature (T$_R$) of ~350 K, just above room temperature. Upon cooling back to room temperature (below T$_R$), we observe a well-defined and unexpected in-plane magnetic domain configuration modulating with ~45 nm. We discuss the underlying mechanisms giving rise to this behavior by comparing the magnetic properties of the patterned sample with the ones of its extended thin film counterpart. Our results pave the way for novel applications of ferrimagnetic antidot arrays of superior functionality in magnetic nano-devices near room temperature.
J. Herrero-Martín, J. L. García-Muñoz, S. Valencia, C. Frontera, J. Blasco, A.J. Barón-González, G. Subías, R. Abrudan, F. Radu, E. Dudzik, R. Feyerherm X-ray absorption spectroscopy measurements in Pr0.5Ca0.5CoO3 were performed at the Pr M4,5, Pr L3, and Ca L2,3 absorption edges as a function of temperature below 300 K. Ca spectra show no changes down to 10 K while a noticeable thermally dependent evolution takes place at the Pr edges across the metal-insulator transition. Spectral changes are analyzed by different methods, including multiple scattering simulations, which provide quantitative details on an electron loss at Pr 4f orbitals. We conclude that in the insulating phase a fraction [15(+5)%] of Pr3+ undergoes a further oxidation to adopt a hybridized configuration composed of an admixture of atomic-like 4f1 states (Pr4+) and f- symmetry states on the O 2p valence band (Pr3+L states) indicative of a strong 4f- 2p interaction.
X-ray absorption spectroscopy measurements in Pr0.5Ca0.5CoO3 and (Pr,Y)0.55Ca0.45CoO3 compositions reveal that the valence of praseodymium ions is stable and essentially +3 (Pr [4f 2]) in the metallic state, but abruptly changes when carriers localize approaching the oxidation state +4 (Pr [4f 1]). This mechanism appears to be the driving force of the metal-insulator transition. The ground insulating state of Pr0.5Ca0.5CoO3 is an homogeneous Co3.5-d state stabilized by a charge transfer from Pr to Co sites: 1/2Pr3+ + Co3.5 \to 1/2Pr3+2d + Co3.5-d, with 2d ≈0.26 e-.
We present a comprehensive study of the exchange bias effect in a model system. Through numerical analysis of the exchange bias and coercive fields as a function of the antiferromagnetic layer thickness we deduce the absolute value of the averaged anisotropy constant of the antiferromagnet. We show that the anisotropy of IrMn exhibits a finite size effect as a function of thickness. The interfacial spin disorder involved in the data analysis is further supported by the observation of the dual behavior of the interfacial uncompensated spins. Utilizing soft x-ray resonant magnetic reflectometry we have observed that the antiferromagnetic uncompensated spins are dominantly frozen with nearly no rotating spins due to the chemical intermixing, which correlates to the inferred mechanism for the exchange bias.
We report on the magnetic properties and the crystallographic structure of the cobalt nanowire arrays as a function of their nanoscale dimensions. X-ray diffraction measurements show the appearance of an in-plane HCP-Co phase for nanowires with 50 nm diameter, suggesting a partial reorientation of the magnetocrystalline anisotropy axis along the membrane plane with increasing pore diameter. No significant changes in the magnetic behavior of the nanowire system are observed with decreasing temperature, indicating that the effective magnetoelastic anisotropy does not play a dominant role in the remagnetization processes of individual nanowires. An enhancement of the total magnetic anisotropy is found at room temperature with a decreasing nanowire diameter-to-length ratio (d/L), a result that is quantitatively analyzed on the basis of a simplified shape anisotropy model.
Positive exchange bias has been observed in the Ni$_{81}$Fe$_{19}$/Ir$_{20}$Mn$_{80}$ bilayer system via soft x-ray resonant magnetic scattering. After field cooling of the system through the blocking temperature of the antiferromagnet, an initial conventional negative exchange bias is removed after training i. e. successive magnetization reversals, resulting in a positive exchange bias for a temperature range down to 30 K below the blocking temperature (450 K). This new manifestation of magnetic training is discussed in terms of metastable magnetic disorder at the magnetically frustrated interface during magnetization reversal.
F. Radu, S. K. Mishra, I. Zizak, A. I. Erko, H. A. Durr, W. Eberhardt, G. Nowak, S. Buschhorn, K. Zhernenkov, M. Wolff, H. Zabel, D. Schmitz, E. Schierle, E. Dudzik, R. Feyerherm We have employed Soft and Hard X-ray Resonant Magnetic Scattering and Polarised Neutron Diffraction to study the magnetic interface and the bulk antiferromagnetic domain state of the archetypal epitaxial Ni$_{81}$Fe$_{19}$(111)/CoO(111) exchange biased bilayer. The combination of these scattering tools provides unprecedented detailed insights into the still incomplete understanding of some key manifestations of the exchange bias effect. We show that the several orders of magnitude difference between the expected and measured value of exchange bias field is caused by an almost anisotropic in-plane orientation of antiferromagnetic domains. Irreversible changes of their configuration lead to a training effect. This is directly seen as a change in the magnetic half order Bragg peaks after magnetization reversal. A 30 nm size of antiferromagnetic domains is extracted from the width the (1/2 1/2 1/2) antiferromagnetic magnetic peak measured both by neutron and x-ray scattering. A reduced blocking temperature as compared to the measured antiferromagnetic ordering temperature clearly corresponds to the blocking of antiferromagnetic domains. Moreover, an excellent correlation between the size of the antiferromagnetic domains, exchange bias field and frozen-in spin ratio is found, providing a comprehensive understanding of the origin of exchange bias in epitaxial systems.
The exchange bias (EB) effect was discovered 60 years ago by Meiklejohn and Bean. Meanwhile the EB effect has become an integral part of modern magnetism with implications for basic research and for numerous device applications. The EB effect was the first of its kind which relates to an interface effect between two different classes of materials, here between a ferromagnet and an antiferromagnet. Here we review fundamental aspects of the exchange bias effect.
An experiment which describes the quantum states of neutrons in magnetic thin films and superlattices is reviewed.
We have used soft X-ray Resonant Magnetic Scattering (XRMS) to search for the presence of an effective ferromagnetic moment belonging to the antiferromagnetic (AF) layer which is in close contact with a ferromagnetic (F) layer. Taking advantage of the element specificity of the XRMS technique, we have measured hysteresis loops of both Fe and CoO layers of a CoO(40 Å)/Fe(150 Å) exchange bias bilayer. From these measurements we have concluded that the proximity of the F layer induces a magnetic moment in the AF layer. The F moment of the AF layer has two components: one is frozen and does not follow the applied magnetic field and the other one follows in phase the ferromagnetic magnetization of the F layer. The temperature dependence of the F components belonging to the AF layer is shown and discussed.
While the principal features of the exchange bias between a ferromagnet and an antiferromagnet are believed to be understood, a quantitative description is still lacking. We show that interface spin disorder is the main reason for the discrepancy of model calculations versus experimental results. Taking into account spin disorder at the interface between the ferromagnet and the antiferromagnet by modifying the well known Meiklejohn and Bean model, an almost perfect agreement can be reached. As an example this is demonstrated for the CoFe/IrMn exchange biased bilayer by analyzing the azimuthal dependence of magnetic hysteresis loops from MOKE measurements. Both, exchange bias and coercive fields for the complete 360$^\circ$ angular range are reproduced by our model.
We performed a detailed study of the training effect in exchange biased CoO/Co bilayers. High-resolution measurements of the anisotropic magnetoresistance (AMR) are consistent with nucleation of magnetic domains in the antiferromagnetic CoO layer during the first magnetization reversal. This accounts for the enhanced spin rotation observed in the ferromagnetic Co layer for all subsequent reversals. Surprisingly, the AMR measurements as well as magnetization measurements reveal that it is possible to partially reinduce the untrained state by performing a hysteresis measurement with an in plane external field perpendicular to the cooling field. Indeed, the next hysteresis loop obtained in a field parallel to the cooling field resembles the initial asymmetric hysteresis loop, but with a reduced amount of spin rotation occurring at the first coercive field. This implies that the antiferromagnetic domains, which are created during the first reversal after cooling, can be partially erased.
We have studied experimentally and theoretically the interaction of polarized neutrons with magnetic thin films and magnetic multilayers. In particular, we have analyzed the behavior of the critical edges for total external reflection in both cases. For a single film we have observed experimentally and theoretically a simple behavior: the critical edges remain fixed and the intensity varies according to the angle between the polarization axis and the magnetization vector inside the film. For the multilayer case we find that the critical edges for spin up and spin down polarized neutrons move towards each other as a function of the angle between the magnetization vectors in adjacent ferromagnetic films. Although the results for multilayers and single thick layers appear to be different, in fact the same spinor method explains both results. An interpretation of the critical edges behavior for the multilyers as a superposition of ferromagnetic and antifferomagnetic states is given.
The spin-density wave (SDW) state in thin chromium films is well known to be strongly affected by proximity effects from neighboring layers. To date the main attention has been given to effects arising from exchange interactions at interfaces. In the present work we report on combined neutron and synchrotron scattering studies of proximity effects in Cr/V films where the boundary condition is due to the hybridization of Cr with paramagnetic V at the interface. We find that the V/Cr interface has a strong and long-range effect on the polarization, period, and the Néel temperature of the SDW in rather thick Cr films. This unusually strong effect is unexpected and not predicted by theory.
Magnetic domain walls in thin films can be well analyzed using polarized neutron reflectometry. Well defined streaks in the off-specular spin-flip scattering maps are explained by neutron refraction at perpendicular Néel walls. The position of the streaks depends only on the magnetic induction within the domains, whereas the intensity of the off-specular magnetic scattering depends on the spin-flip probability at the domain walls and on the average size of the magnetic domains. This effect is fundamentally different and has to be clearly distinguished from diffuse scattering originating from the size distribution of magnetic domains. Polarized neutron reflectivity experiments were carried out using a $^3$He gas spin-filter with a analyzing power as high as 96% and a neutron transmission of approx 35%. Furthermore, the off-specular magnetic scattering was enhanced by using neutron resonance and neutron standing wave techniques.
We report on the use of the polarized $^3$He gas filter and neutron resonant enhancement techniques for the measurement of spin-polarized diffuse neutron scattering due to ferromagnetic domains. A CoO/Co exchange biased bilayer was grown on a Ti/Cu/$Al_2O_3$ neutron resonator template. The system is cooled in an applied magnetic field of $H_a=2000$ Oe through the Néel temperature of the antiferromagnet to 10 K where the applied magnetic field is swept as to measure the magnetic hysteresis loop. After the second magnetization reversal at the coercive field $H_{c2}=+ 230$ Oe, the system is supposed to approach the original magnetic configuration. In order to prove that this is not the case for our exchange biased bilayer, we have measured four off-specular maps I++, I+-, I-+, I-- at $H_a \approx + 370$ Oe, where the Co magnetic spins were mostly reversed. They show a striking behavior in the total reflection region: while the nonspin-flip scattering exhibits no diffuse reflectivity, the spin-flip scattering shows strong diffuse scattering at incident angles which satisfy the resonance conditions. Moreover the spin-flip off-specular part of the reflectivity is asymmetric. The I-+ intensity occurs at higher exit angles than the specularly reflected neutrons, and the I+- intensity is shifted to lower angles. Their intensities are noticeably different and there is a splitting of the resonance positions for the up and down neutron spins ($\alpha_{n} ^{+} \ne \alpha_{n} ^{-}$) . Additionally, a strong influence of the stray fields from magnetic domains to the resonance splitting is observed.
We have carried out detailed experimental studies of the exchange bias effect of a series of CoO/Co(111) textured bilayers with different Co layer thickness, using the magneto-optical Kerr effect, SQUID magnetometry, polarized neutron reflectivity, x-ray diffraction, and atomic force microscopy. All samples exhibit a pronounced asymmetry of the magnetic hysteresis at the first magnetization reversal as compared to the second reversal. Polarized neutron reflectivity measurements show that the first reversal occurs via nucleation and domain wall motion, while the second reversal is characterized by magnetization rotation. Off-specular diffuse spin-flip scattering indicates the existence of interfacial magnetic domains. All samples feature a small positive exchange bias just below the blocking temperature, followed by a dominating negative exchange bias field with decreasing temperature. For very thin Co-films the coexistence of ferromagnetic domains with parallel and perpendicular magnetization directions leads to a peculiar shape of the hysteresis with an extended plateau like region of almost zero magnetization.