Resonant Magnetic X-ray Diffraction Research Articles

4D Visualization of a Nonthermal Coherent Magnon in a Laser Heated Lattice by an X-ray Free Electron Laser.

Ultrafast optical manipulation of magnetic phenomena is an exciting achievement of mankind, expanding one's horizon of knowledge toward the functional nonequilibrium states. The dynamics acting on an extremely short timescale push the detection limits that reveal fascinating light-matter interactions for nonthermal creation of effective magnetic fields. While some cases are benchmarked by emergent transient behaviors, otherwise identifying the nonthermal effects remains challenging. Here, a femtosecond time-resolved resonant magnetic X-ray diffraction experiment is introduced, which uses an X-ray free-electron laser (XFEL) to distinguish between the effective field and the photoinduced thermal effect. It is observed that a multiferroic Y-type hexaferrite exhibits magnetic Bragg peak intensity oscillations manifesting entangled antiferromagnetic (AFM) and ferromagnetic (FM) Fourier components of a coherent AFM magnon. The magnon trajectory constructed in 3D space and time domains is decisive to evince ultrafast field formation preceding the lattice thermalization. A remarkable impact of photoexcitation across the electronic bandgap is directly unraveled, amplifying the photomagnetic coupling that is one of the highest among AFM dielectrics. Leveraging the above-bandgap photoexcitation, this energy-efficient optical process further suggests a novel photomagnetic control of ferroelectricity in multiferroics.

Spectral shape of resonant x-ray magnetic diffraction from GdAl2

We have numerically examined the spectral shape of the ratio of the intensity variation upon the magnetization reversal for the 444 reflection of the ferromagnetic intermetallic compound GdAl2 in the vicinity of the Gd L 2 edge and succeeded in roughly reproducing the experimental spectra for two different magnetization directions simultaneously. The main features of the spectral shape are described in terms of the conventional dispersion effects and the resonant magnetic scattering of electric dipole transitions.

Nanoscale Antiferromagnetic Domain Imaging using Full-Field Resonant X-ray Magnetic Diffraction Microscopy.

The physical properties of magnetic materials frequently depend not only on the microscopic spin and electronic structures, but also on the structures of mesoscopic length scales that emerge, for instance, from domain formations, or chemical and/or electronic phase separations. However, experimental access to such mesoscopic structures is currently limited, especially for antiferromagnets with net zero magnetization. Here, full-field microscopy and resonant magnetic X-ray diffraction are combined to visualize antiferromagnetic (AF) domains of the spin-orbit Mott insulator Sr2 IrO4 with area over ≈0.1 mm2 and with spatial resolution as high as ≈150nm. With the unprecedented wide field of views and high spatial resolution, an intertwining of two AF domains on a length comparable to the measured average AF domain wall width of 545nm is revealed. This mesoscopic structure comprises a substantial portion of the sample surface, and thus can result in a macroscopic response unexpected from its microscopic magnetic structure. In particular, the symmetry analysis presented in this work shows that the inversion symmetry, which is preserved by the microscopic AF order, becomes ill-defined at the mesoscopic length scale. This result underscores the importance of this novel technique for a thorough understanding of the physical properties of antiferromagnets.

Photo-induced antiferromagnetic-ferromagnetic and spin-state transition in a double-perovskite cobalt oxide thin film

Investigation of ultrafast dynamic behaviors can provide novel insights about the coupling mechanisms among multiple degrees of freedom in condensed matters, such as lattice, magnetism and electronic structure. Here we investigate both the ferromagnetic (FM) and antiferromagnetic (AFM) dynamics of a strongly correlated oxide system, GdBaCo2O5.5 thin film by time-resolved x-ray magnetic circular dichroism in reflectivity (XMCDR) and resonant magnetic x-ray diffraction (RMXD). A photo-induced AFM-FM transition characterized by an increase of the transient XMCDR (sensitive to FM order) beyond the unpumped value and a decay of RMXD (sensitive to AFM order) was observed. The photon-energy dependence of the transient XMCDR and reflectivity could be interpreted as a concomitant photo-induced spin-state transition (SST). The AFM-FM transition and SST couple with each other in the time domain, resulting in unusual dynamic behaviors of the magnetism.

MagStREXS: crystallographic software for magnetic structure determination through resonant X-ray magnetic diffraction data

<i>MagStREXS</i>: crystallographic software for magnetic structure determination through resonant X-ray magnetic diffraction data

Approaching the quantum critical point in a highly correlated all-in–all-out antiferromagnet

Continuous quantum phase transitions involving all-in-all-out (AIAO) antiferromagnetic order in strongly spin-orbit-coupled 5d compounds could give rise to various exotic electronic phases and strongly-coupled quantum critical phenomena. Here we experimentally trace the AIAO spin order in Sm2Ir2O7 using direct resonant x-ray magnetic diffraction techniques under high pressure. The magnetic order is suppressed at a critical pressure Pc=6.30 GPa, while the lattice symmetry remains in the cubic Fd-3m space group across the quantum critical point. Comparing pressure tuning and the chemical series R2Ir2O7 reveals that the suppression of the AIAO order and the approach to the spin-disordered state is characterized by contrasting evolutions of both the pyrochlore lattice constant a and the trigonal distortion x. The former affects the 5d bandwidth, the latter the Ising anisotropy, and as such we posit that the opposite effects of pressure and chemical tuning lead to spin fluctuations with different Ising and Heisenberg character in the quantum critical region. Finally, the observed low-pressure scale of the AIAO quantum phase transition in Sm2Ir2O7 identifies a circumscribed region of P-T space for investigating the putative magnetic Weyl-semimetal state.

Field-induced spin reorientation in the antiferromagnetic Dirac material EuMnBi2 revealed by neutron and resonant x-ray diffraction

Field-dependent magnetic structure of a layered Dirac material EuMnBi$_2$ was investigated in detail by the single crystal neutron diffraction and the resonant x-ray magnetic diffraction techniques. On the basis of the reflection conditions in the antiferromagnetic phase at zero field, the Eu moments were found to be ordered ferromagnetically within the $ab$ plane and stacked antiferromagnetically along the $c$ axis in the sequence of up-up-down-down. Upon the spin-flop transition under the magnetic field parallel to the $c$ axis, the Eu moments are reoriented from the $c$ to the $a$ or $b$ directions forming two kinds of spin-flop domains, whereas the antiferromagnetic structure of the Mn sublattice remains intact as revealed by the quantitative analysis of the change in the neutron diffraction intensities. The present study provides a concrete basis to discuss the dominant role of the Eu sublattice on the enhanced two-dimensionality of the Dirac fermion transport in EuMnBi$_2$.

Mode-Resolved Detection of Magnetization Dynamics Using X-ray Diffractive Ferromagnetic Resonance.

Collective spin excitations of ordered magnetic structures offer great potential for the development of novel spintronic devices. The present approach relies on micromagnetic models to explain the origins of dynamic modes observed by ferromagnetic resonance (FMR) studies, since experimental tools to directly reveal the origins of the complex dynamic behavior are lacking. Here we demonstrate a new approach which combines resonant magnetic X-ray diffraction with FMR, thereby allowing for a reconstruction of the real-space spin dynamics of the system. This new diffractive FMR technique builds on X-ray detected FMR that allows for element-selective dynamic studies, giving unique access to specific wave components of static and dynamic coupling in magnetic heterostructures. In combination with diffraction, FMR is elevated to the level of a modal spectroscopy technique, potentially opening new pathways for the development of spintronic devices.

Itinerancy-dependent noncollinear spin textures in SrFeO3, CaFeO3 , and CaFeO3/SrFeO3 heterostructures probed via resonant x-ray scattering

Non-collinear, multi-q spin textures can give rise to exotic, topologically protected spin structures such as skyrmions, but the reason for their formation over simple single-q structures is not well understood. While lattice frustration and the Dzyaloshinskii-Moriya interaction are known to produce non-collinear spin textures, the role of electron itinerancy in multi-q formation is much less studied. Here we investigated the non-collinear, helical spin structures in epitaxial films of the perovskite oxides SrFeO3 and CaFeO3 using magnetotransport and resonant soft x-ray magnetic diffraction. Metallic SrFeO3 exhibits features in its magnetoresistance that are consistent with its recently proposed multi-q structure. Additionally, the magnetic Bragg peak of SrFeO3 measured at the Fe L edge resonance energy asymmetrically broadens with decreasing temperature in its multi-q state. In contrast, insulating CaFeO3 has a symmetric scattering peak with an intensity 10x weaker than SrFeO3. Enhanced magnetic scattering at O K edge prepeak energies demonstrates the role of a negative charge transfer energy and the resulting oxygen ligand holes in the magnetic ordering of these ferrates. By measuring magnetic diffraction of CaFeO3/SrFeO3 superlattices with thick CaFeO3 layers, we find that the CaFeO3 helical ordering is coherent across 1 unit cell-thick SrFeO3 layers but not 6 unit cell-thick layers. We conclude that insulating CaFeO3 supports only a simple single-q helical structure in contrast to metallic SrFeO3 that hosts multi-q structures. Our results provide important insight into the role of electron itinerancy in the formation of multi-q spin structures.

X-ray magnetic diffraction under high pressure.

Advances in both non-resonant and resonant X-ray magnetic diffraction since the 1980s have provided researchers with a powerful tool for exploring the spin, orbital and ion degrees of freedom in magnetic solids, as well as parsing their interplay. Here, we discuss key issues for performing X-ray magnetic diffraction on single-crystal samples under high pressure (above 40 GPa) and at cryogenic temperatures (4 K). We present case studies of both non-resonant and resonant X-ray magnetic diffraction under pressure for a spin-flip transition in an incommensurate spin-density-wave material and a continuous quantum phase transition of a commensurate all-in-all-out antiferromagnet. Both cases use diamond-anvil-cell technologies at third-generation synchrotron radiation sources. In addition to the exploration of the athermal emergence and evolution of antiferromagnetism discussed here, these techniques can be applied to the study of the pressure evolution of weak charge order such as charge-density waves, antiferro-type orbital order, the charge anisotropic tensor susceptibility and charge superlattices associated with either primary spin order or softened phonons.

Magnetic structure and magnetoelastic coupling of GdNiSi3 and TbNiSi3

The series of intermetallic compounds $R$NiSi$_3$ ($R$ = rare earth) shows interesting magnetic properties evolving with $R$ and metamagnetic transitions under applied magnetic field for some of the compounds. The microscopic magnetic structures must be determined to rationalize such rich behavior. Here, resonant x-ray magnetic diffraction experiments are performed on single crystals of GdNiSi$_{3}$ and TbNiSi$_{3}$ at zero field. The primitive magnetic unit cell matches the chemical cell below the N\'eel temperatures $T_{N}$ = 22.2 and 33.2 K, respectively. The magnetic structure is determined to be the same for both compounds (magnetic space group $Cmmm'$). It features ferromagnetic {\it ac} planes that are stacked in an antiferromagnetic $+-+-$ pattern, with the rare-earth magnetic moments pointing along the $\vec{a}$ direction, which contrasts with the $+--+$ stacking and moment direction along the $\vec{b}$ axis previously reported for YbNiSi$_3$. This indicates a sign reversal of the coupling constant between second-neighbor $R$ planes as $R$ is varied from Gd and Tb to Yb. The long {\it b} lattice parameter of GdNiSi$_{3}$ and TbNiSi$_{3}$ shows a magnetoelastic expansion upon cooling below $T_N$, pointing to the conclusion that the $+-+-$ stacking is stabilized under lattice expansion. A competition between distinct magnetic stacking patterns with similar exchange energies tuned by the size of $R$ sets the stage for the magnetic ground state instability observed along this series.

Strongly-coupled quantum critical point in an all-in-all-out antiferromagnet

Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Here, using newly-developed, high-pressure resonant X-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd2Os2O7 as the all-in-all-out antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound.

Imaging and manipulation of skyrmion lattice domains in Cu2OSeO3

Nanoscale chiral skyrmions in noncentrosymmetric helimagnets are promising binary state variables in high-density, low-energy nonvolatile memory. Skyrmions are ubiquitous as an ordered, single-domain lattice phase, which makes it difficult to write information unless they are spatially broken up into smaller units, each representing a bit. Thus, the formation and manipulation of skyrmion lattice domains is a prerequisite for memory applications. Here, using an imaging technique based on resonant magnetic x-ray diffraction, we demonstrate the mapping and manipulation of skyrmion lattice domains in Cu2OSeO3. The material is particularly interesting for applications owing to its insulating nature, allowing for electric field-driven domain manipulation.

Itinerant and Localized Magnetization Dynamics in Antiferromagnetic Ho.

Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L_{3} absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Tuning the x-ray energy to the electric dipole (E1, 2p→5d) or quadrupole (E2, 2p→4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3-τ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similar spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f-5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magneto-striction leads to a transient shift of the magnetic satellite peak.

Noncoplanar and counterrotating incommensurate magnetic order stabilized by Kitaev interactions in γ-Li(2)IrO(3).

Materials that realize Kitaev spin models with bond-dependent anisotropic interactions have long been searched for, as the resulting frustration effects are predicted to stabilize novel forms of magnetic order or quantum spin liquids. Here, we explore the magnetism of γ-Li(2)IrO(3), which has the topology of a three-dimensional Kitaev lattice of interconnected Ir honeycombs. Using magnetic resonant x-ray diffraction, we find a complex, yet highly symmetric incommensurate magnetic structure with noncoplanar and counterrotating Ir moments. We propose a minimal Kitaev-Heisenberg Hamiltonian that naturally accounts for all key features of the observed magnetic structure. Our results provide strong evidence that γ-Li(2)IrO(3) realizes a spin Hamiltonian with dominant Kitaev interactions.

Depth Profile of Induced Magnetic Polarization in Au Layers of Fe/Au(001) Metallic Superlattice by Resonant X-ray Magnetic Scattering at High Angle Region

Spin polarization of 5d conduction electrons induced in the Au layers of antiferromagnetically coupled Fe/Au metallic superlattice was investigated by resonant X-ray magnetic diffraction at the Au L3 absorption edge. Superlattice reflections around the Au 002 Bragg peak were measured in the magnetic saturation state with circularly polarized synchrotron radiation X-rays of 11921 eV. The magnetic diffraction profile was extracted with the combination of helicity switching and reversing the direction of magnetic field applied along the line of intersection between the film surface and the scattering plane. The depth distribution of resonant magnetic scattering length in the Au layers was estimated from the magnetic diffraction profile. Both resonant magnetic diffraction from the Au layer and non-resonant magnetic diffraction from the Fe layer were considered in the analysis. We demonstrated that the depth distribution of the Au magnetic scattering length was expressed with sum of the interface-concentrated ...

Time and momentum resolved resonant magnetic x-ray diffraction on EuTe

We used fs- and ps- resonant magnetic x-ray diffraction to probe the laser-induced changes to the magnetic profile in thin films of the antiferromagnetic semicon-ductor EuTe.

Weak antiferromagnetism ofJeff=12band in bilayer iridate Sr3Ir2O7

The antiferromagnetic structure of Sr${}_{3}$Ir${}_{2}$O${}_{7}$, the bilayer analog of a spin-orbital Mott insulator Sr${}_{2}$IrO${}_{4}$, was revealed by resonant magnetic x-ray diffraction. Contrasting intensities of the magnetic diffraction at the Ir ${L}_{\mathrm{III}}$ and ${L}_{\mathrm{II}}$ edges show a ${J}_{\mathrm{eff}}=1/2$ character of the magnetic moment as is argued in Sr${}_{2}$IrO${}_{4}$. The magnitude of moment, however, was found to be smaller than that of Sr${}_{2}$IrO${}_{4}$ by a factor of 5 to 6, implying that Sr${}_{3}$Ir${}_{2}$O${}_{7}$ is no longer a Mott insulator but a weak antiferromagnet. An evident change of the temperature dependence of the resistivity at ${T}_{\mathrm{N}}$, from almost temperature-independent resistivity to insulating, strongly suggests that the emergent weak magnetism controls the charge gap. The magnetic structure was found to be an out-of-plane collinear antiferromagnetic ordering in contrast to the in-plane canted antiferromagnetism in Sr${}_{2}$IrO${}_{4}$, originating from the strong bilayer antiferromagnetic coupling.

Interface effects on Gd induced disordering of Co films on Pt(111)

Amorphization of epitaxial Co thin films grown on top of a Pt(111) surface has been studied by surface X-ray diffraction after deposition of Gd overlayers. The results indicate strong differences of the disordering process depending on the thickness of the Co film. First basic difference is that thick Co films (15 atomic layers) are only partially amorphized by 4 atomic layers of Gd on top of them, whereas thinner Co films (5 atomic layers) are completely disordered by just 2 atomic layers of Gd. Moreover, amorphization by Gd overlayers induces different stress relaxation processes in both cases. For 15 atomic layers thick Co films a preferential amorphization of the more strained Co grains is observed, leading to an effective relaxation of about −0.5% of the in-plane lattice parameter during amorphization, approaching its relaxed value. On the contrary, for 5 atomic layers thick Co films, the initial steps of disordering are accompanied by a stronger increase of the in-plane lattice constant, by about 1.4%, typical of Co–Pt interface alloy formation, followed by a complete amorphization. Furthermore, the magnetic characterization, carried out by magneto-optical Kerr effect and resonant magnetic surface X-ray diffraction, strongly supports that the amorphization of thin Co films is changing the nature of the Co/Pt interface. In particular, as Gd overlayers are deposited, and the amorphization proceeds, the structural disordering of the Co/Pt interface flips its characteristic perpendicular magnetic anisotropy toward in-plane orientation before the complete magnetic depolarization of the interface Pt atoms is reached. All these results confirm a marked dependence of amorphization processes on film thickness, which can be related to the enhanced influence of the nearby film/substrate interface.

Depth-resolved magnetic structure across the ferromagnetic to helical-antiferromagnetic phase transition in Dy/W(110)

We investigated the magnetic depth profile during the transition from the ferromagnetic (FM) to the helical-antiferromagnetic (AFM) phase in Dy-metal films grown on W(110). To this purpose, we used the strongly varying photon penetration depth across the $\text{Dy}\text{ }{M}_{5}$ absorption threshold in resonant magnetic soft x-ray diffraction. Unlike in earlier studies on Dy films with two equivalent interfaces, we find a gradual growth of the AFM part of the film with temperature. The near-surface magnetic structure does not become FM and appears to serve as seed layer for the growth of the AFM order.