arXiv subjects

Jun Okabayashi

Publications and source records attributed to Jun Okabayashi.

15 recordsLinked to original sources

arXiv2025

Evidence for single variant in altermagnetic RuO2(101) thin films

Altermagnetism presents intriguing possibilities for spintronic devices due to its unique combination of strong spin-splitting and zero net magnetization. However, realizing its full potential hinges on fabricating single-variant altermagnetic thin films. In this work, we present definitive evidence for the formation of single-variant altermagnetic RuO2(101) thin films with fully epitaxial growth on Al2O3(1-102) r-plane substrates, confirmed through rigorous structural analyses using X-ray diffraction, atomic-resolution transmission electron microscopy and X-ray magnetic linear dichroism. The mutual correspondence of the occupancy of oxygen atoms on the surfaces of RuO2(101)[010] and Al2O3(1-102)[11-20] plays a decisive role in the formation of the single-variant RuO2, which is also supported by our first-principles density functional theory calculations. We further observed spin-splitting magnetoresistance in the single-variant RuO2(101)/CoFeB bilayers, highlighting the characteristic effect of single variant on spin transport. The demonstration of single-variant RuO2(101) films marks a significant advancement in the field of altermagnetism and paves the way for exploring their potential applications.

cond-mat.mtrl-sci↗

arXiv2023

Perpendicular magnetic anisotropy of an ultrathin Fe layer grown on NiO(001)

The magnetic anisotropy and magnetic interactions at the interface between Fe and NiO(001) were investigated. Depending on the growth conditions of the NiO(001) layers and the post-annealing temperature, the preferential magnetization direction of the ultrathin Fe layer grown on a NiO(001) layer changed from in-plane to a direction perpendicular to the film plane. The lattice constant of the NiO(001) layers parallel to the growth direction increased with O$_2$ flow rate, while that parallel to the in-plane were locked onto the MgO(001) substrate regardless of the growth conditions of the NiO layers. Moreover, perpendicular magnetization was observed only when the NiO layer was grown with O$_2$ flow rates higher than 2.0 sccm corresponding to oxygen-rich NiO. X-ray magnetic circular dichroism measurements revealed an enhancement in anisotropic orbital magnetic moments similar to the origin of perpendicular magnetic anisotropy at the Fe/MgO(001) interface. The interfacial magnetic anisotropy energies were 0.93 and 1.02 mJ/m$^2$ at room temperature and at 100 K, respectively, indicating less temperature dependence. In contrast, the coercivity $H_c$ exhibited a significant temperature dependence. Although no signature of exchange bias or unidirectional loop shift was observed, $H_c$ was strongly dependent on the NiO layer thickness, indicating that the exchange interaction at the interface between the ferromagnetic and antiferromagnetic layers was not negligible, despite the NiO(001) being a spin-compensated surface.

cond-mat.mtrl-sci↗

arXiv2023

Control of conductivity in Fe-rich cobalt-ferrite thin films with perpendicular magnetic anisotropy

We fabricated two types of cobalt-ferrite (001) thin films, insulative Fe-rich cobalt-ferrite CoxFe3-xO4+δ (I-CFO) and conductive Fe-rich cobalt-ferrite CoyFe3-yO4 (C-CFO), with perpendicular magnetic anisotropy (PMA) on MgO (001) substrates. Although the stoichiometric cobalt-ferrite is known as an insulating material, it is found that the conductivity of Fe-rich cobalt-ferrites can be controlled by changing the source materials and deposition conditions in the pulsed laser deposition technique. The I-CFO and C-CFO films exhibit PMA through the in-plane lattice distortion. We investigated the Fe-ion-specific valence states in both I-CFO and C-CFO films by Mössbauer spectroscopy and X-ray magnetic circular dichroism, and found that the difference in conductivity corresponds to the abundance ratio of Fe2+ state at the octahedral B-site (Oh) in the inverse spinel structure. Furthermore, first-principles calculations reproduce the changes in the density of states at the Fermi level depending on the cation vacancies at the B-site, which explains the difference in the conductivity between I-CFO and C-CFO.

cond-mat.mtrl-sci↗

arXiv2022

Tracing magnetic atom diffusion with annealing at the interface between CoMn alloy and MnGa layer by X-ray magnetic circular dichroism

The magnetic atom diffusion at the interface between CoMn alloy and MnGa layer with annealing is studied using x-ray magnetic circular dichroism (XMCD) analysis. We found that the spins in bcc CoMn are coupled parallel to those in perpendicularly magnetized MnGa layer under the as-grown conditions, while the post-annealing modulates the interfacial magnetic coupling to antiferromagnetic in Co. The element-specific hysteresis curves at each absorption edge revealed the large coercive fields in Mn and Co through the exchange coupling with MnGa. After the annealing process, the changes of XMCD spectral line shapes are related to the interfacial reactions promoting the formation of Mn and Co2MnGa layers, which is deduced from the analysis of transmission electron microscopy. The interfacial diffusion of Mn atoms modulates the magnetic exchange coupling between Mn and Co sites and reverses the direction of perpendicular magnetization.

cond-mat.mtrl-sci↗

arXiv2022

Understanding magnetocrystalline anisotropy based on orbital and quadrupole moments

Understanding magnetocrystalline anisotropy (MCA) is fundamentally important for developing novel magnetic materials. Therefore, clarifying the relationship between MCA and local physical quantities observed by spectroscopic measurements, such as the orbital and quadrupole moments, is necessary. In this review, we discuss MCA and the distortion effects in magnetic materials with transition metals (TMs) based on the orbital and quadrupole moments, which are related to the spin-conserving and spin-flip terms in the second-order perturbation calculations, respectively. We revealed that orbital moment stabilized the spin moment in the direction of the larger orbital moment, while the quadrupole moment stabilized the spin moment along the longitudinal direction of the spin-density distribution. The MCA of the magnetic materials with TMs and their interfaces can be determined from the competition between these two contributions. We showed that the perpendicular MCA of the face-centered cubic (fcc) Ni with tensile tetragonal distortion arose from the orbital moment anisotropy, whereas that of Mn-Ga alloys originated from the quadrupole moment of spin density. In contrast, in the Co/Pd(111) multilayer and Fe/MgO(001), both the orbital moment anisotropy and quadrupole moment of spin density at the interfaces contributed to the perpendicular MCA. Understanding the MCA of magnetic materials and interfaces based on orbital and quadrupole moments is essential to design MCA of novel magnetic applications.

cond-mat.mtrl-sci↗

arXiv2022

Origin of Perpendicular Magnetic Anisotropy in Co$_x$Fe$_{3-x}$O$_{4+δ}$ Thin Films Studied by X-ray Magnetic Circular and Linear Dichroisms

We investigate the element-specific spin and orbital states and their roles on magnetic anisotropy in the Co-ferrite (Co$_x$Fe$_{3-x}$O$_{4+δ}$ (001)) thin films which exhibit perpendicular magnetic anisotropy (PMA). The origin of PMA in the low $x$ region ($x$ $<$ 1) can be mainly explained by the large perpendicular orbital magnetic moments in the Co$^{2+}$ (3$d^7$) states detected by X-ray magnetic circular and linear dichroisms (XMCD/XMLD). The XMLD for a PMA film ($x=0.2$) with square hysteresis curve shows the oblate charge distribution in the Co$^{2+}$ site, which is consistent with the change in local nearest neighbor distance in Co detected by extended X-ray absorption fine structure analysis. Our finding reveals that the microscopic origin of PMA in Co-ferrite comes from the enhanced orbital magnetic moments along out-of-plane [001] direction through in-plane charge distribution by tensile strain, which adds the material functionalities in spinel ferrite thin films from the viewpoint of strain and orbital magnetic moments.

cond-mat.mtrl-sci↗

arXiv2021

Perpendicular magnetic anisotropy at Fe/Au(111) interface studied by Mössbauer, x-ray absorption, and photoemission spectroscopies

The origin of the interfacial perpendicular magnetic anisotropy (PMA) induced in the ultrathin Fe layer on the Au(111) surface was examined using synchrotron-radiation-based Mössbauer spectroscopy (MS), X-ray magnetic circular dichroism (XMCD), and angle-resolved photoemission spectroscopy (ARPES). To probe the detailed interfacial electronic structure of orbital hybridization between the Fe 3$d$ and Au 6$p$ bands, we detected the interfacial proximity effect, which modulates the valence-band electronic structure of Fe, resulting in PMA. MS and XMCD measurements were used to detect the interfacial magnetic structure and anisotropy in orbital magnetic moments, respectively. $In$-$situ$ ARPES also confirms the initial growth of Fe on large spin-orbit coupled surface Shockley states under Au(111) modulated electronic states in the vicinity of the Fermi level. This suggests that PMA in the Fe/Au(111) interface originates from the cooperation effects among the spin, orbital magnetic moments in Fe, and large spin-orbit coupling in Au. These findings pave the way to develop interfacial PMA using $p$-$d$ hybridization with a large spin-orbit interaction.

cond-mat.mtrl-sci↗

arXiv2020

High tunnel magnetoresistance and magnetism in metastable bcc Co$_{1-x}$Mn$_x$-based magnetic tunnel junctions

Co-rich Co$_{1-x}$Mn$_x$ alloys have hcp or fcc disordered phases and those ferromagnetic orderings are significantly deteriorated with increasing Mn concentration $x$ in bulk. On the other hand, those metastable bcc phases show properties attractive to spintronics, e.g., high tunnel magnetoresistance (TMR) ratio of more than 200% (600%) at 300 K (10 K) in magnetic tunnel junctions (MTJs) with the $x$ = 0.25 bcc alloy electrodes [Kunimatsu et al., Appl. Phys. Express 13, 083007 (2020)]. Here, we report systematic study of structure and magnetism for epitaxial thin films as well as the TMR effect in MgO(001)-barrier MTJs with electrodes comprising those bcc films. The single phase bcc Co$_{1-x}$Mn$_x$(001) films were pseudomorphically grown on Cr(001) for 0.14 < $x$ < 0.50 with a sputtering technique. The magnetization was larger than that of pure Co for $x$ = 0.14-0.25 and deceased with further increasing $x$. This behavior mainly stemmed from the composition dependence of magnetic moment of Mn that exceeded 2 $μ_B$ at the maximum, unveiled by X-ray magnetic circular dichroism. Correspondingly, within the range of 0.25 < $x$ < 0.37, the TMR ratio decreased from 620% (229%) to 450% (194%) at 10 K (300 K) as $x$ increased. We discussed the relationship between the magnetism and high TMR ratio with different $x$ with the aid of the ab-initio band structure calculations.

cond-mat.mtrl-sci↗

arXiv2020

Detecting quadrupole: a hidden source of magnetic anisotropy for Manganese alloys

Mn-based alloys exhibit unique properties in the spintronics materials possessing perpendicular magnetic anisotropy (PMA) beyond the Fe and Co-based alloys. It is desired to figure out the quantum physics of PMA inherent to Mn-based alloys, which have never been reported. Here, the origin of PMA in ferrimagnetic Mn$_{3-δ}$Ga ordered alloys is investigated to resolve antiparallel-coupled Mn sites using x-ray magnetic circular and linear dichroism (XMCD/XMLD) and a first-principles calculation. We found that the contribution of orbital magnetic moments in PMA is small from XMCD and that the finite quadrupole-like orbital distortion through spin-flipped electron hopping is dominant from XMLD and theoretical calculations. These findings suggest that the spin-flipped orbital quadrupole formations originate from the PMA in Mn$_{3-δ}$Ga and bring the paradigm shift in the researches of PMA materials using x-ray magnetic spectroscopies.

cond-mat.mtrl-sci↗

arXiv2019

Magnetic tunnel junctions with a B2-ordered CoFeCrAl equiatomic Heusler alloy

The equiatomic quaternary Heusler alloy CoFeCrAl is a candidate material for spin-gapless semiconductors (SGSs). However, to date, there have been no experimental attempts at fabricating a junction device. This paper reports a fully epitaxial (001)-oriented MgO barrier magnetic tunnel junction (MTJ) with CoFeCrAl electrodes grown on a Cr buffer. X-ray and electron diffraction measurements show that the (001) CoFeCrAl electrode films with atomically flat surfaces have a $B2$-ordered phase. The saturation magnetization is 380 emu/cm$^3$, almost the same as the value given by the Slater--Pauling--like rule, and the maximum tunnel magnetoresistance ratios at 300 K and 10 K are 87% and 165%, respectively. Cross-sectional electron diffraction analysis shows that the MTJs have MgO interfaces with fewer dislocations. The temperature- and bias-voltage-dependence of the transport measurements indicates magnon-induced inelastic electron tunneling overlapping with the coherent electron tunneling. X-ray magnetic circular dichroism (XMCD) measurements show a ferromagnetic arrangement of the Co and Fe magnetic moments of $B2$-ordered CoFeCrAl, in contrast to the ferrimagnetic arrangement predicted for the $Y$-ordered state possessing SGS characteristics. Ab-initio calculations taking account of the Cr-Fe swap disorder qualitatively explain the XMCD results. Finally, the effect of the Cr-Fe swap disorder on the ability for electronic states to allow coherent electron tunneling is discussed.

cond-mat.mtrl-sci↗

arXiv2019

Strain-Induced Reversible Manipulation of Orbital Magnetic Moments in Ni/Cu Multilayers on Ferroelectric BaTiO3

Controlling magnetic anisotropy by orbital magnetic moments related to interfacial strains has considerable potential for the development of future devices using spins and orbitals. For the fundamental physics, the relationship between strain and orbital magnetic moment is still unknown, because there are few tools to probe changes of orbital magnetic moment. In this study, we developed an electric-field- (E)-induced X-ray magnetic circular dichroism (EXMCD) technique to apply E to a ferroelectric BaTiO3 substrate. We reversibly tuned the interfacial lattice constants of Ni/Cu multilayers on BaTiO3 using this technique. As the domain structures in BaTiO3 are modulated by E, EXMCD measurements reveal that the changes in the magnetic anisotropy of Ni/Cu films are induced through the modulation of orbital magnetic moments in Ni with magneto-elastic contributions. The strained Ni layer that induces the perpendicular magnetic anisotropy without E is released at E = 8 kV/cm, and in-plane magnetization also occurs. We observed that EXMCD measurements clarified the origin of the reversible changes in perpendicular magnetic anisotropy and established the relationship between macroscopic inverse magnetostriction effects and microscopic orbital moment anisotropy.

cond-mat.mtrl-sci↗

arXiv2018

Anatomy of interfacial spin-orbit coupling in Co/Pd multilayers using X-ray magnetic circular dichroism and first-principles calculations

Element-specific orbital magnetic moments and their anisotropies in perpendicularly magnetised Co/Pd multilayers are investigated using Co L-edge and Pd M-edge angle-dependent x-ray magnetic circular dichroism. We show that the orbital magnetic moments in Co are anisotropic, whereas those in Pd are isotropic. The first-principles density-functional-theory calculations also suggest that the Co/Pd interfacial orbital magnetic moments in Co are anisotropic and contribute to the perpendicular magnetic anisotropy (PMA), and that the isotropic ones in Pd manipulates the Co orbitals at the interface through proximity effects. Orbital-resolved anatomy of Co/Pd interfaces reveals that the orbital moment anisotropy in Co and spin-flipped transition related to the magnetic dipoles in Pd are essential for the appearance of PMA.

cond-mat.mtrl-sci↗

arXiv2017

Pressure-induced two-step spin crossover in double-layered elastic model

We study the two-step spin crossover in a double-layered elastic model based on transition metal complexes each taking high spin (HS) and low spin (LS) states. Here, only the simplest elastic interactions between adjacent molecules are considered and the system is exposed to the external pressure within the framework of $NPT$-Monte Carlo method. As a certain amount of pressure is applied, the first order thermal transition between uniform HS and LS phases transforms to a two-step transition with an emergent intermediate spin (IS) phase, where the HS and LS molecules are paired face to face between layers and form diagonally striped clusters within the layer. The difference in the size of HS and LS molecules is reflected both in the elastic interactions and in the enthalpy, and the IS phase could gain the latter over the loss of the former by significantly reducing its volume. The present pressure effect is interpreted to the chemical one in double-layered transition metal materials, which actually reveals a variety of multistep spin crossover transitions relevant to our numerical result.

cond-mat.mtrl-sci↗

arXiv2017

Detection of induced paramagnetic moments in Pt on Y$_3$Fe$_5$O$_{12}$ via x-ray magnetic circular dichroism

Magnetic moments in an ultra-thin Pt film on a ferrimagnetic insulator Y$_3$Fe$_5$O$_{12}$ (YIG) have been investigated at high magnetic fields and low temperatures by means of X-ray magnetic circular dichroism (XMCD). We observed an XMCD signal due to the magnetic moments in a Pt film at the Pt $L_{3}$- and $L_{2}$-edges. By means of the element-specific magnetometry, we found that the XMCD signal at the Pt $L_{3}$-edge gradually increases with increasing the magnetic field even when the field is much greater than the saturation field of YIG. Importantly, the observed XMCD intensity was found to be much greater than the intensity expected from the Pauli paramagnetism of Pt when the Pt film is attached to YIG. These results imply the emergence of induced paramagnetic moments in Pt on YIG and explain the characteristics of the unconventional Hall effect in Pt/YIG systems.

cond-mat.mtrl-sci↗

arXiv2016

Interdiffusion in epitaxial ultrathin Co2FeAl/MgO heterostructures with interface-induced perpendicular magnetic anisotropy

The structures of epitaxial ultrathin Co2FeAl/MgO(001) heterostructures relating to the interface-induced perpendicular magnetic anisotropy (PMA) were investigated using scanning transmission electron microscopy, energy dispersive x-ray spectroscopy, and x-ray magnetic circular dichroism. We found that Al atoms from the Co2FeAl layer significantly interdiffuse into MgO, forming an Al-deficient Co-Fe-Al/Mg-Al-O structure near the Co2FeAl/MgO interface. This atomic replacement may play an additional role for enhancing PMA, which is consistent with the observed large perpendicular orbital magnetic moments of Fe atoms at the interface. This work suggests that control of interdiffusion at ferromanget/barrier interfaces is critical for designing an interface-induced PMA system.

cond-mat.mtrl-sci↗