X-ray directional dichroism of a polar ferrimagnet

In a polar ferrimagnet GaFeO3, we have found a novel magneto-optical effect, termed x-ray nonreciprocal directional dichroism (XNDD), that the x-ray absorption at around the K edge of an Fe ion depends on whether the x-ray propagation vector is parallel or antiparallel to the outer product of the magnetization and electric-polarization vectors. The XNDD spectroscopy as demonstrated here can be a useful tool to probe the local magnetism in noncentrosymmetric systems such as magnetic interfaces and nanostructures.     

Soft x-ray resonant diffraction study of magnetic and orbital correlations in a manganite near half doping

We have utilized resonant x-ray diffraction at the Mn L(II,III) edges in order to directly compare magnetic and orbital correlations in Pr0.6Ca0.4MnO3. Comparing the widths of the magnetic and orbital diffraction peaks, we find that the magnetic correlation length exceeds that of the orbital order by nearly a factor of 2. Furthermore, we observe a large (approximately 3 eV) spectral weight shift between the magnetic and orbital resonant line shapes, which cannot be explained within the classic Goodenough picture of a charge-ordered ground state. To explain the shift, we calculate the orbital and magnetic resonant diffraction line shapes based on a relaxed charge-ordered model.     

Spin and orbital magnetic moments of Fe3O4

We present measurements of the spin and orbital magnetic moments of Fe3O4 by using SQUID and magnetic circular dichroism in soft x-ray absorption. The measurements show that Fe3O4 has a noninteger spin moment, in contrast to its predicted half-metallic feature. Fe3O4 also exhibits a large unquenched orbital moment. Calculations using the local density approximation including the Hubbard U method and the configuration interaction cluster-model suggest that strong correlations and spin-orbit interaction of the 3d electrons result in the noninteger spin and large orbital moments of Fe3O4.     

Enhanced optical magnetoelectric effect in a patterned polar ferrimagnet

A simple method to dramatically enhance the optical magnetoelectric (ME) effect, i.e., nonreciprocal directional birefringence, is proposed and demonstrated for a polar ferrimagnet GaFeO3 as a typical example. We patterned a simple grating with a period of 4 microm on a surface of GaFeO3 crystal and used the diffracted light as a probe. The optical ME modulation signal for the Bragg spot of the order n=1 becomes gigantic in the photon energy 1-4 eV and reaches 1-2% of the bare diffracted light intensity in a magnetic field of 500 Oe. This is amplified by more than 3 orders of magnitude compared to that for the reflection of bulk GaFeO3. Fabricating a photonic crystal will make it possible to lead the way for the practical use of the optical ME effect.     

Direct observation of orbital ordering in La0.5Sr1.5MnO4 using soft x-ray diffraction

We report the first direct resonant soft x-ray scattering observations of orbital ordering. We have studied the low temperature phase of La0.5Sr1.5MnO4, a compound that displays charge and orbital ordering. Previous claims of orbital ordering in such materials have relied on observations at the manganese K edge. These claims have been questioned in several theoretical studies. Instead we have employed resonant soft x-ray scattering at the manganese L(III) and L(II) edges which probes the orbital ordering directly. Energy scans at constant wave vector are compared to theoretical predictions and suggest that at all temperatures there are two separate contributions to the scattering: direct orbital ordering and strong cooperative Jahn-Teller distortions of the Mn3+ ions.     

Soft X-ray resonant magnetic diffraction

We have conducted the first soft x-ray diffraction experiments from a bulk single crystal, studying the bilayer manganite La2-2xSr1+2xMn2O7 with x=0.475 in which we were able to access the (002) Bragg reflection using soft x rays. The Bragg reflection displays a strong resonant enhancement at the L(III) and L(II) manganese absorption edges. We demonstrate that the resonant enhancement of the magnetic diffraction of the (001) is extremely large, indeed so large that it exceeds that of the nonresonant Bragg diffraction. Resonant soft x-ray scattering of 3d transition metal oxides is the only technique for the atomic selective measurement of spin, charge, and orbital correlations in materials, such as high temperature superconductors, colossal magnetoresistance manganites, and charge stripe nickelates.     

Magnetization-induced second harmonic generation in a polar ferromagnet

Second harmonic generation (SHG) induced by spontaneous magnetization has been investigated for a polar ferromagnetic crystal of GaFeO3. The Kerr rotation of the second harmonic light becomes gigantic with decreasing temperature below the magnetic transition temperature (approximately =205 K), e.g., as large as 73 degrees at 100 K. The magnetic domains can be visualized by using that large nonlinear Kerr rotation. The spectrum of the magnetization-induced SHG as measured indicates the two-photon resonant electronic process on a Fe3+ ion in the crystal.     

Strongly enhanced orbital moment by reduced lattice symmetry and varying composition of Fe1-xCox alloy films

We studied tetragonally distorted Fe(1-x)Co(x) alloy films on Rh(001), which show a strong perpendicular anisotropy in a wide thickness and composition range. Analyzing x-ray magnetic circular dichroism spectra at the L_(3,2) edges we found a dependence of the Co magnetic orbital moment on the chemical composition of the Fe(1-x)Co(x) alloy films, with a maximum at x=0.6. For this composition, we observed an out-of-plane easy axis of magnetization at room temperature for film thickness up to 15 monolayers. Since both the magnetic orbital moment and the anisotropy energy show similar composition dependence, it confirms that both quantities are directly related. Our experiments show that the adjustment of the Fermi level by a proper choice of the alloy composition is decisive for the large magnetic orbital moment and for a large magnetic anisotropy in a tetragonally distorted lattice.     

Direct observation of a bulklike spin moment at the Fe/GaAs(100)-4x6 interface

We have used x-ray magnetic circular dichroism, which offers a unique capability to give element specific information at submonolayer sensitivity, to determine the spin and orbital magnetic moments at the Fe/GaAs(100) interface. The wedge samples, grown by molecular beam epitaxy at room temperature, consisted of 0.25-1 monolayer (ML) Fe on GaAs(100)-4x6 capped with 9 ML Co and have shown Fe spin moments of (1.84-1.96)micro(B) and a large orbital enhancement. Our results demonstrate unambiguously that the Fe/GaAs(100)-4x6 interface is ferromagnetic with a bulklike spin moment, which is highly promising for spintronics applications.     

Ferro-type orbital state in the Mott transition system Ca2-xSrxRuO4 studied by the resonant x-ray scattering interference technique

We have succeeded in detecting ferro-type orbital states in Ca2-xSrxRuO4, which is the first outcome in a 4d Mott transition system by the resonant x-ray scattering interference technique. For x=0 (Mott insulator), the resonant signal for d(xy) orbital ordering is observed even at room temperature, in which the Jahn-Teller distortion is negligible. The signal disappears near the metal-insulator transition. On the other hand, in a metallic phase for x=0.5, orbital polarization with d(yz/zx) character dominates. With lowering temperature, the magnitude of the resonant signal slightly decreases owing to the additional influence of the gamma band with d(xy) character.     

Determination of the orbital moment and crystal-field splitting in LaTiO3

Utilizing a sum rule in a spin-resolved photoelectron spectroscopic experiment with circularly polarized light, we show that the orbital moment in LaTiO3 is strongly reduced from its ionic value, both below and above the Ne el temperature. Using Ti L2,3 x-ray absorption spectroscopy as a local probe, we found that the crystal-field splitting in the t2g subshell is about 0.12-0.30 eV. This large splitting does not facilitate the formation of an orbital liquid.     

Measurement of a pauli and orbital paramagnetic state in bulk gold using x-ray magnetic circular dichroism spectroscopy

We show that bulk gold (Au) exhibits temperature-independent paramagnetism in an external magnetic field by x-ray magnetic circular dichroism spectroscopy at the Au L(2) and L(3) edges. Using the sum-rule analysis, we obtained a magnetic moment of 1.3 × 10(-4) μB/atom in an external magnetic field of 10 T and a paramagnetic susceptibility of 8.9 × 10(-6) for the 5d orbit. The induced paramagnetism in bulk Au is characterized by a large (≈ 30%) orbital contribution. This orbital component was retained even when Au atoms formed nanoparticles, playing an important role in stabilizing the spontaneous spin polarization in the Au nanoparticles.     

Coupling between spin and orbital degrees of freedom in KCuF3

We present the results of resonant x-ray scattering experiments on KCuF3. Structurally forbidden reflections, corresponding to magnetic and 3d-orbital long-range order, have been observed. Integrated intensities have been measured as a function of incident energy, polarization, azimuthal angle, and temperature. The results give evidence for a strong coupling between orbital and spin degrees of freedom. The interplay between magnetic and orbital order parameters is revealed by the temperature dependence of the intensity of orbital Bragg peaks.     

Fragile magnetic ground state in half-doped LaSr2Mn2O7

We investigated the orbital and antiferromagnetic ordering behaviors of the half-doped bilayer manganite La(2-2x)Sr(1+2x)Mn2O7 (x ? 0.5) by using Mn L(2,3)-edge resonant soft x-ray scattering. Resonant soft x-ray scattering reveals the CE-type orbital order below T(oo) ? 220 K, which shows partial melting behavior below T(m) ? 165 K. We also found coexistence CE- and A-type antiferromagnetic orders. Both orders involve the CE-type orbital order with nearly the same orbital character and are coupled with each other. These results manifest that the ground state with the CE-type antiferromagnetic order is easily susceptible to destabilization into the A-type one even with a small fluctuation of the doping level, as suggested by the extremely narrow magnetic phase boundaries at x ? 0.5±0.005.     

X-ray magnetochiral dichroism: a new spectroscopic probe of parity nonconserving magnetic solids

We report the first experimental detection of x-ray magnetochiral dichroism in magnetoelectric Cr2O3. This dichroism, which does not require any polarized x-ray beam, is related to the time-reversal odd part of the optical activity tensor dominated by electric dipole-electric quadrupole E1E2 interference terms. The experiments were carried out using either a single crystal or a powdered pellet required to grow a single antiferromagnetic domain by magnetoelectric annealing. This new element (edge) specific spectroscopy offers unique access to the atomic orbital anapole moment Omega-z.     

Orbitally driven spin-singlet dimerization in S=1 La4Ru2O10

Using x-ray absorption spectroscopy at the Ru-L2,3 edge we reveal that the Ru4+ ions remain in the S=1 spin state across the rare 4d-orbital ordering transition and spin-gap formation. We find using local spin density approximation + Hubbard U band structure calculations that the crystal fields in the low-temperature phase are not strong enough to stabilize the S=0 state. Instead, we identify a distinct orbital ordering with a significant anisotropy of the antiferromagnetic exchange couplings. We conclude that La4Ru2O10 appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi-two-dimensional S=1 system.     

Direct observation of orbital magnetism in cubic solids

We present x-ray magnetic circular dichroism determinations of the orbital/spin magnetic moment ratios of dilute 3d-series impurities in Au (and Cu) host matrices. This is the first direct measurement of considerable orbital moments in cubic symmetry for a localized impurity in a bulk metal host. It is shown that the unquenching of orbital magnetism depends on a delicate balance of hybridization effects between the local impurity with the host and the filling of the 3d states of the impurity. The results are accompanied by ab initio calculations that support our experimental findings.     

Optical magnetoelectric effect in the polar GaFeO3 ferrimagnet

The optical magnetoelectric (ME) effect, i.e., the change of optical absorption upon the reversal of the light propagation direction, has been investigated for a polar ferrimagnet GaFeO3. For dipole- and spin-forbidden d-d transition bands located at 1.2-2.3 eV, a clear signal of the optical ME effect (Deltaalphat approximately 3x10(-3)) is observed with an applied magnetic field as low as 500 Oe and a sample thickness (t) of 50 microm. The observation of a large ME effect in the present compound suggests a possible route to magnification of this novel phenomenon for application.     

Spin state transition in LaCoO3 studied using soft x-ray absorption spectroscopy and magnetic circular dichroism

Using soft x-ray absorption spectroscopy and magnetic circular dichroism at the Co-L(2,3) edge, we reveal that the spin state transition in LaCoO3 can be well described by a low-spin ground state and a triply degenerate high-spin first excited state. From the temperature dependence of the spectral line shapes, we find that LaCoO3 at finite temperatures is an inhomogeneous mixed-spin state system. It is crucial that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low- or intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance, and inelastic neutron data.     

Evidence for electronic phase separation between orbital orderings in SmVO3

We report evidence for phase coexistence of orbital orderings of different symmetry in SmVO3 by high resolution x-ray powder diffraction. The phase coexistence is triggered by an antiferromagnetic ordering of the vanadium spins near 130 K, below an initial orbital ordering near 200 K. The phase coexistence is the result of the intermediate ionic size of samarium coupled to exchange striction at the vanadium spin ordering.