X-ray Resonant Magnetic Reflectivity Research Articles

Non-uniform Gd distribution and magnetization profiles within GdCoFe alloy thin films

Rare earth (RE):transition metal (TM) ferrimagnetic alloys continue to attract significant attention for spintronics. This work focuses on the elemental distribution of RE and TM elements throughout the thickness of nominally uniform films and the resulting spatial variations of the magnetization within these layers. Samples of CoFe alloyed with Gd were studied using secondary ion mass spectroscopy, polarized neutron reflectometry, and x-ray resonant magnetic reflectivity. The samples were grown by magnetron co-sputtering to control the RE:TM alloy ratio of the ferrimagnetic layer, which was combined with W and Pt layers as either under or over-layers to create sample structures such as W/Gdx(Co70Fe30)100−x/Pt, where x = 0, 8, and 23 at. %. Results show that uniformly deposited thin-films have a significant variation in the distribution of the TM and RE through the film thickness, and this leads to a spatial distribution in the net magnetization profile and a non-uniform Gd magnetization profile within the layer. These findings have implications for the application RE:TM alloys in spintronics as they may impact the perpendicular magnetic anisotropy, the ferrimagnetic compensation temperature, and interfacial spin transport.

Ferromagnetic order controlled by the magnetic interface of LaNiO3/La2/3Ca1/3MnO3 superlattices

Interface engineering in complex oxide superlattices is a growing field, enabling manipulation of the exceptional properties of these materials, and also providing access to new phases and emergent physical phenomena. Here we demonstrate how interfacial interactions can induce a complex charge and spin structure in a bulk paramagnetic material. We investigate a superlattice (SLs) consisting of paramagnetic LaNiO3 (LNO) and highly spin-polarized ferromagnetic La2/3Ca1/3MnO3 (LCMO), grown on SrTiO3 (001) substrate. We observed emerging magnetism in LNO through an exchange bias mechanism at the interfaces in X-ray resonant magnetic reflectivity. We find non-symmetric interface induced magnetization profiles in LNO and LCMO which we relate to a periodic complex charge and spin superstructure. High resolution scanning transmission electron microscopy images reveal that the upper and lower interfaces exhibit no significant structural variations. The different long range magnetic order emerging in LNO layers demonstrates the enormous potential of interfacial reconstruction as a tool for tailored electronic properties.

Depth-resolved magnetization profile of MgO/CoFeB/W perpendicular half magnetic tunnel junctions

In this work, we used the soft X-ray resonant magnetic reflectivity to study the depth-resolved out-of-plane (oop) magnetization profile of a CoFeB/MgO sample with W/Ta cap layer after annealing at 400°C. It is a powerful technique to probe buried magnetic interfaces of ultra-thin films by combining the depth-resolved information of X-ray reflectivity with the species selectivity of X-ray magnetic circular dichroism. It allowed us to resolve the oop magnetization within a 1.36 nm thick CoFeB layer by the measurement of angle-dependent specular reflectivity at large scattering angles (up to 80°). We determined a graded magnetic distribution for both Fe and Co with a 20% increase at the interface with MgO, decreasing slightly over a thickness of 0.7 nm from MgO before it rapidly decreases to 50% at the interface with W. After applying a non-saturating magnetic field in the plane of the sample, we also quantified a similar magnetization profile with an inclined moment configuration. This indicates that the magnetization gradient is a robust property of the CoFeB layer in the studied sample.

Interplay between chemical and magnetic roughness of Pt in a Pt/Co bilayer investigated with X-ray resonant magnetic reflectometry

Abstract The magnetization depth profiles of Pt have been investigated by X-ray resonant magnetic reflectivity measurements of sputtered Pt/Co bilayer systems with different chemical roughness values at the Pt/Co interface. The asymmetry ratio as a function of the angle of incidence has been measured at the Pt L3 near-edge absorption region at the maximum of the X-ray magnetic circular dichroism effect. The observed asymmetry ratios in the order of 0.5% are described quantitatively on the basis of a magnetically modified optical approach. The curves of the extracted magnetization profiles in the Pt layer show a different behavior corresponding to chemical roughness, while the magnetic saturation moment of Pt at the Pt/Co interface remains unaltered.

X-ray reflectivity data analysis using Bayesian inference: The study of induced Pt magnetization in Pt/Co/Pt

The induced Pt magnetization in a Pt/Co/Pt thin film structure is studied. The normally nonmagnetic Pt acquires a magnetic moment due to the magnetic proximity effect at the Co–Pt interfaces. Element specific Pt structural and magnetic properties are characterized by synchrotron-based resonant x-ray reflectivity and x-ray resonant magnetic reflectivity measurements. An advanced analysis method based on Bayesian inference is used for model fitting of the x-ray data. Using this method, we retrieve the best fit values of material parameters (e.g., thickness, interfacial roughness) from the data. Analysis of x-ray reflectivity data of this specific system shows that the Pt magnetization and Co–Pt interfacial roughness is significantly different between the top and bottom Pt layers, with both values being larger in the top Pt. The successful application of this Bayesian method to study the magnetic and structural properties of a thin film system demonstrates its effectiveness for x-ray reflectivity data analysis.

Toward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity.

During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump–probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm (), we were able to probe close to the Fe L3 edge () of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization.

Quantitative comparison of the magnetic proximity effect in Pt detected by XRMR and XMCD

X-ray resonant magnetic reflectivity (XRMR) allows for the simultaneous measurement of structural, optical, and magneto-optic properties and depth profiles of a variety of thin film samples. However, a same-beamtime same-sample systematic quantitative comparison of the magnetic properties observed using XRMR and x-ray magnetic circular dichroism (XMCD) is still pending. Here, the XRMR results (Pt L3 absorption edge) for the magnetic proximity effect in Pt deposited on the two different ferromagnetic materials Fe and Co33Fe67 are compared with quantitatively analyzed XMCD results. The obtained results are in very good quantitative agreement between the absorption-based (XMCD) and reflectivity-based (XRMR) techniques, taking into account an ab initio calculated magneto-optic conversion factor for the XRMR analysis. Thus, it is shown that XRMR provides quantitative reliable spin depth profiles important for spintronic and spin caloritronic transport phenomena at this type of magnetic interfaces.

Static magnetic proximity effects and spin Hall magnetoresistance in Pt/Y3Fe5O12 and inverted Y3Fe5O12/Pt bilayers

The magnetic state of heavy metal Pt thin films in proximity to the ferrimagnetic insulator Y$_{3}$Fe$_{5}$O$_{12}$ has been investigated systematically by means of x-ray magnetic circular dichroism and x-ray resonant magnetic reflectivity measurements combined with angle-dependent magnetotransport studies. To reveal intermixing effects as the possible cause for induced magnetic moments in Pt, we compare thin film heterostructures with different order of the layer stacking and different interface properties. For standard Pt layers on Y$_{3}$Fe$_{5}$O$_{12}$ thin films, we do not detect any static magnetic polarization in Pt. These samples show an angle-dependent magnetoresistance behavior, which is consistent with the established spin Hall magnetoresistance. In contrast, for the inverted layer sequence, Y$_{3}$Fe$_{5}$O$_{12}$ thin films grown on Pt layers, Pt displays a finite induced magnetic moment comparable to that of all-metallic Pt/Fe bilayers. This magnetic moment is found to originate from finite intermixing at the Y$_{3}$Fe$_{5}$O$_{12}$/Pt interface. As a consequence, we found a complex angle-dependent magnetoresistance indicating a superposition of the spin Hall and the anisotropic magnetoresistance in these type of samples. Both effects can be disentangled from each other due to their different angle dependence and their characteristic temperature evolution.

Cation- and lattice-site-selective magnetic depth profiles of ultrathin Fe3O4 (001) films

A detailed understanding of ultrathin film surface properties is crucial for the proper interpretation of spectroscopic, catalytic, and spin-transport data. We present x-ray magnetic circular dichroism (XMCD) and x-ray resonant magnetic reflectivity (XRMR) measurements on ultrathin ${\mathrm{Fe}}_{3}{\mathrm{O}}_{4}$ films to obtain magnetic depth profiles for the three resonant energies corresponding to the different cation species ${\mathrm{Fe}}_{\mathrm{oct}}^{2+}$, ${\mathrm{Fe}}_{\mathrm{tet}}^{3+}$, and ${\mathrm{Fe}}_{\mathrm{oct}}^{3+}$ located on octahedral and tetrahedral sites of the inverse spinel structure of ${\mathrm{Fe}}_{3}{\mathrm{O}}_{4}$. By analyzing the XMCD spectrum of ${\mathrm{Fe}}_{3}{\mathrm{O}}_{4}$ using multiplet calculations, the resonance energy of each cation species can be isolated. Performing XRMR on these three resonant energies yields magnetic depth profiles that each correspond to one specific cation species. The depth profiles of both kinds of ${\mathrm{Fe}}^{3+}$ cations reveal a $\left(3.9\ifmmode\pm\else\textpm\fi{}1.0\right)\text{\ensuremath{-}}\AA{}$-thick surface layer of enhanced magnetization, which is likely due to an excess of these ions at the expense of the ${\mathrm{Fe}}_{\mathrm{oct}}^{2+}$ species in the surface region. The magnetically enhanced ${\mathrm{Fe}}_{\mathrm{tet}}^{3+}$ layer is additionally shifted about $2.9\ifmmode\pm\else\textpm\fi{}0.4\phantom{\rule{4pt}{0ex}}\AA{}$ farther from the surface than the ${\mathrm{Fe}}_{\mathrm{oct}}^{3+}$ layer.

Asymmetric modification of the magnetic proximity effect in Pt/Co/Pt trilayers by the insertion of a Ta buffer layer

The magnetic proximity effect in top and bottom Pt layers induced by Co in Ta/Pt/Co/Pt multilayers has been studied by interface sensitive, element specific x-ray resonant magnetic reflectivity. The asymmetry ratio for circularly polarized x-rays of left and right helicity has been measured at the Pt $L_3$ absorption edge (11567 eV) with an in-plane magnetic field ($\pm158$ mT) to verify its magnetic origin. The proximity-induced magnetic moment in the bottom Pt layer decreases with the thickness of the Ta buffer layer. Grazing incidence x-ray diffraction has been carried out to show that the Ta buffer layer induces the growth of Pt(011) rather than Pt(111) which in turn reduces the induced moment. A detailed density functional theory study shows that an adjacent Co layer induces more magnetic moment in Pt(111) than in Pt(011). The manipulation of the magnetism in Pt by the insertion of a Ta buffer layer provides a new way of controlling the magnetic proximity effect which is of huge importance in spin-transport experiments across similar kind of interfaces.

Advanced data analysis procedure for hard x-ray resonant magnetic reflectivity discussed for Pt thin film samples of various complexity

X-ray resonant magnetic reflectivity (XRMR) is a powerful method to determine the optical, structural and magnetic depth profiles of a variety of thin film systems. Here, we investigate samples of different complexity all measured at the Pt absorption edge to determine the optimal procedure for the analysis of the experimental XRMR curves, especially for nontrivial bi- and multilayer samples that include differently bonded Pt from layer to layer. The software tool ReMagX is used to fit these data and model the magnetooptic depth profiles based on a highly adaptable layer stack which is modified to be a more precise and physically consistent representation of the real multilayer system. Various fitting algorithms, iterative optimization approaches and a detailed analysis of the asymmetry ratio features as well as χ2 (goodness of fit) landscapes are utilized to improve the agreement between measurements and simulations. We present a step-by-step analysis procedure tailored to the Pt thin film systems to take advantage of the excellent magnetic sensitivity and depth resolution of XRMR.

Impact of the magnetic proximity effect in Pt on the total magnetic moment of Pt/Co/Ta trilayers studied by x-ray resonant magnetic reflectivity

In this work, we study the influence of the magnetic proximity effect (MPE) in Pt on the total magnetic moment of thin film trilayer systems consisting of the ferromagnet (FM) Co adjacent to the heavy metals (HMs) Pt and Ta. We investigate the trilayer systems HM1/FM/HM2 with different stacking order as well as a reference bilayer without any MPE. X-ray resonant magnetic reflectivity (XRMR) is a powerful tool to probe induced magnetism, especially when buried at interfaces in a multilayer. By using XRMR, we are able to obtain magnetic depth profiles of the structural, optical and magnetic parameters. By fitting the experimental data with a Gaussian-like magnetooptic profile taking the structural roughness at the interface into account, we can extract the magnetic moment of the spin-polarized layer. Comparing the obtained moments to the measured total moment of the sample, we can determine the impact of the MPE on the total magnetic moment of the system. Such information can be critical for analyzing spin transport experiments, including spin-orbit torque and spin Hall angle measurements, where the saturation magnetization Ms has to be taken into account. Therefore, by combining magnetization measurements and XRMR methods we were able to get a complete picture of the magnetic moment distribution in these trilayer systems containing spin-polarized Pt.

Standing wave approach in the theory of X-ray magnetic reflectivity.

An extension of the exact X-ray resonant magnetic reflectivity theory has been developed, taking into account the small value of the magnetic terms in the X-ray susceptibility tensor. It is shown that squared standing waves (fourth power of the total electric field) determine the output of the magnetic addition to the total reflectivity from a magnetic multilayer. The obtained generalized kinematical approach essentially speeds up the calculation of the asymmetry ratio in the magnetic reflectivity. The developed approach easily explains the peculiarities of the angular dependence of the reflectivity with the rotated polarization (such as the peak at the critical angle of the total external reflection). The revealed dependence of the magnetic part of the total reflectivity on the squared standing waves means that the selection of the reflectivity with the rotated polarization ensures higher sensitivity to the depth profiles of magnetization than the secondary radiation at the specular reflection condition.

Thickness Dependence of the Dzyaloshinskii-Moriya Interaction in Co2FeAl Ultrathin Films: Effects of Annealing Temperature and Heavy-Metal Material

Interfacial Dzyaloshinskii-Moriya interaction (iDMI) has been investigated in Co2FeAl (CFA) ultrathin films of various thicknesses (0.8 nm<tCFA<2 nm) grown on Si substrates, using Pt, W, Ir and MgO buffer or/and capping layers. Vibrating sample magnetometry revealed that magnetization at saturation (Ms) for the Pt and Ir buffered films is higher than the usual Ms of CFA due to the proximity induced magnetization (PIM) in Ir and Pt, estimated to be 19% and 27%, respectively. The presence of PIM in these materials is confirmed using x-ray resonant magnetic reflectivity. Moreover, while no PIM is induced in W, higher PIM is obtained with Pt when it is used as buffer layer rather than capping layer. Brillouin light scattering (BLS) in the Damon-Eshbach geometry has been used to investigate iDMI constants and the perpendicular anisotropy field versus the annealing temperature. The DMI sign has been found to be negative for Pt/CFA and Ir/CFA while it is positive for W/CFA. The thickness dependence of the effective iDMI constant for stacks involving Pt and W shows the existence of two regimes similarly to that of the perpendicular anisotropy constant due to the degradation of the interfaces as the CFA thickness approaches the nanometer. The surface iDMI and anisotropy constants of each stack have been determined for the thickest samples where a linear thickness dependence of the effective iDMI constant and the effective magnetization has been observed. The interface anisotropy and iDMI constants, investigated for Pt/CFA/MgO system, showed different trends with the annealing temperature. The decrease of iDMI constant with increasing annealing temperature is probably due to the electronic structure changes at the interfaces, while the increase of the interface anisotropy constant is coherent the interface quality and disorder enhancement.

Quantitative Disentanglement of the Spin Seebeck, Proximity-Induced, and Ferromagnetic-Induced Anomalous Nernst Effect in Normal-Metal-Ferromagnet Bilayers.

We identify and investigate thermal spin transport phenomena in sputter-deposited Pt/NiFe_{2}O_{x} (4≥x≥0) bilayers. We separate the voltage generated by the spin Seebeck effect from the anomalous Nernst effect (ANE) contributions and even disentangle the ANE in the ferromagnet (FM) from the ANE produced by the Pt that is spin polarized due to its proximity to the FM. Further, we probe the dependence of these effects on the electrical conductivity and the band gap energy of the FM film varying from nearly insulating NiFe_{2}O_{4} to metallic Ni_{33}Fe_{67}. A proximity-induced ANE could only be identified in the metallic Pt/Ni_{33}Fe_{67} bilayer in contrast to Pt/NiFe_{2}O_{x} (x>0) samples. This is verified by the investigation of static magnetic proximity effects via x-ray resonant magnetic reflectivity.

Surface pinning effect of an antiferromagnetic interlayer exchange coupling in (Ga1−x Mn x As/GaAs:Be)10 multilayer

The depth-resolved magnetic configuration of a Ga0.97Mn0.03As/GaAs:Be multilayer with an antiferromagnetic interlayer exchange coupling was investigated using surface-sensitive soft x-ray resonant magnetic reflectivity (XRMR). We observed intriguing opposite increments in the XRMR intensities at the half-Bragg peak position between two different remanent states with opposite field sweep directions. A quantitative analysis shows that these opposite intensity increments result from two different anti-parallel spin configurations in such a way that the magnetization of top-most magnetic layer is pinned along the saturation magnetization direction before the remanent state. This surface pinning effect is important for understanding spin-dependent transport in semiconducting magnetic multilayers.

Structural dynamics during laser-induced ultrafast demagnetization

The mechanism underlying femtosecond laser pulse induced ultrafast magnetization dynamics remains elusive despite two decades of intense research on this phenomenon. Most experiments focused so far on characterizing magnetization and charge carrier dynamics, while first direct measurements of structural dynamics during ultrafast demagnetization were reported only very recently. We here present our investigation of the infrared laser pulse induced ultrafast demagnetization process in a thin Ni film, which characterizes simultaneously magnetization and structural dynamics. This is achieved by employing femtosecond time resolved X-ray resonant magnetic reflectivity (tr-XRMR) as probe technique. The experimental results reveal unambiguously that the sub-picosecond magnetization quenching is accompanied by strong changes in non-magnetic X-ray reflectivity. These changes vary with reflection angle and changes up to 30$\%$ have been observed. Modeling the X-ray reflectivity of the investigated thin film, we can reproduce these changes by a variation of the apparent Ni layer thickness of up to 1$\%$. Extending these simulations to larger incidence angles we show that tr-XRMR can be employed to discriminate experimentally between currently discussed models describing the ultrafast demagnetization phenomenon.

Static Magnetic Proximity Effect in Pt Layers on Sputter-Deposited NiFe2O4and on Fe of Various Thicknesses Investigated by XRMR

The longitudinal spin Seebeck effect is detected in sputter-deposited NiFe2O4 films using Pt as a spin detector and compared to previously investigated NiFe2O4 films prepared by chemical vapor deposition. Anomalous Nernst effects induced by the magnetic proximity effect in Pt can be excluded for the sputter-deposited NiFe2O4 films down to a certain limit, since x-ray resonant magnetic reflectivity measurements show no magnetic response down to a limit of 0.04 {\mu}B per Pt atom comparable to the case of the chemicallydeposited NiFe2O4 films. These differently prepared films have various thicknesses. Therefore, we further studied Pt/Fe reference samples with various Fe thicknesses and could confirm that the magnetic proximity effect is only induced by the interface properties of the magnetic material.

Static magnetic proximity effect inPt/Ni1−xFexbilayers investigated by x-ray resonant magnetic reflectivity

We present x-ray resonant magnetic reflectivity (XRMR) as a very sensitive tool to detect proximity induced interface spin polarization in Pt/Fe, Pt/Ni$_{33}$Fe$_{67}$, Pt/Ni$_{81}$Fe$_{19}$ (permalloy), and Pt/Ni bilayers. We demonstrate that a detailed analysis of the reflected x-ray intensity gives insight in the spatial distribution of the spin polarization of a non-magnetic metal across the interface to a ferromagnetic layer. The evaluation of the experimental results with simulations based on optical data from ab initio calculations provides the induced magnetic moment per Pt atom in the spin polarized volume adjacent to the ferromagnet. We find the largest spin polarization in Pt/Fe and a much smaller magnetic proximity effect in Pt/Ni. Additional XRMR experiments with varying photon energy are in good agreement with the theoretical predictions for the energy dependence of the magnetooptic parameters and allow identifying the optical dispersion $\delta$ and absorption $\beta$ across the Pt L3-absorption edge.

Asymmetric magnetic proximity effect in a Pd/Co/Pd trilayer system.

In spintronic devices consisting of ferromagnetic/nonmagnetic systems, the ferromagnet-induced magnetic moment in the adjacent nonmagnetic material significantly influences the spin transport properties. In this study, such magnetic proximity effect in a Pd/Co/Pd trilayer system is investigated by x-ray magnetic circular dichroism and x-ray resonant magnetic reflectivity, which enables magnetic characterizations with element and depth resolution. We observe that the total Pd magnetic moments induced at the top Co/Pd interface are significantly larger than the Pd moments at the bottom Pd/Co interface, whereas transmission electron microscopy and reflectivity analysis indicate the two interfaces are nearly identical structurally. Such asymmetry in magnetic proximity effects could be important for understanding spin transport characteristics in ferromagnetic/nonmagnetic systems and its potential application to spin devices.