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A. Hariki

Publications and source records attributed to A. Hariki.

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Nanoscale imaging of spin textures with locally varying altermagnetic response in $\alpha$-Fe$_2$O$_3$

Altermagnetism is a recently identified magnetic state in which time-reversal symmetry is broken despite a collinear compensated spin structure. The response of altermagnets is determined not only by their $d$-, $g$-, or $i$-wave spin order, but also the orientation of their N\'eel vector $\mathbf{L}$. Therefore, accessing a response that fundamentally depends on the orientation of $\mathbf{L}$, such as the anomalous Hall effect, remains experimentally challenging in particular at the nanoscale. Here, we harness nano-spectroscopic X-ray magnetic circular dichroism (XMCD) to investigate nanoscale modulated altermagnetic responses in $\alpha$-Fe$_2$O$_3$ (Hematite). By performing spectroscopy across the temperature-induced $\mathbf{L}$-reorientation Morin transition, we observe the on-and-off switching of XMCD, in agreement with our theoretical calculations. Although the bulk XMCD vanishes below the Morin temperature, we confirm the reorientation of $\mathbf{L}$ by harnessing polarization-independent X-ray absorption spectroscopy. Moreover, we observe a finite XMCD signal in nanoscale domain walls with locally modulated N\'eel vectors, while the surrounding domains exhibit no XMCD. At room temperature, we instead identify altermagnetic meron spin textures that exhibit XMCD in their planar regions but no XMCD in their nanoscopic cores. Our results establish a pathway to harness complex spin textures with nanoscale functionalities in a broader class of altermagnets with various $\mathbf{L}$-orientations and using light, earth-abundant elements.

cond-mat.mtrl-sci

Bi-altermagnetism unveiled by sublattice-specific circular dichroism in resonant inelastic X-ray scattering

An altermagnet is a recently identified class of magnets that exhibit a zero net magnetic moment but break symmetry under the combined operations of parity and time reversal. It typically consists of two magnetic sites of opposite spins related by rotation within the unit cell. Here, we use circular dichroism (CD) in resonant inelastic X-ray scattering (RIXS) to identify a new form of altermagnetism, namely bi-altermagnetism, in the correlated insulator Fe2Mo3O8, which comprises two altermagnetic sublattices: one with alternating quasi-octahedral Fe environments and the other with alternating tetrahedral Fe environments. We experimentally revealed the emergence of CD in an achiral, zero-magnetization system, thereby probing mirror-symmetry breaking associated with altermagnetic order. Notably, the CD appeared at sublattice-specific excitations of the octahedral and tetrahedral sites, indicating symmetry breaking in both altermagnetic sublattices. Calculations based on a model with the bi-altermagnetic order along the c axis successfully reproduce the observed CD. Our findings provide compelling evidence for bi-altermagnetism in Fe2Mo3O8, and showcase the use of RIXS-CD as a probe of magnetic sublattices in systems with zero net magnetization.

cond-mat.str-el

Theory of circular dichroism in resonant inelastic x-ray scattering

We analyze circular dichroism (CD) in resonant inelastic x-ray scattering (RIXS) in magnetic materials. We define RIXS-CD as the difference between scattering amplitudes for the right- and left-circularly polarized incoming photons and unpolarized (total) outgoing photons. We employ the impurity approximation, in which the interference between scattering events on different atoms is neglected. We perform the symmetry analysis of several common antiferromagnetic and altermagnetic structures and outline the general approach. The analysis is supported by numerical calculations using atomic model with realistic crystal fields obtained from first principles. We show that RIXS-CD is distinguished from first-order spectroscopies such as x-ray magnetic circular dichroism by insensitivity to the time-reversal symmetry breaking. As a result we find that RIXS-CD is present in the normal (disordered) state of materials with lower symmetry. In antiferromagnets the RIXS-CD is invariant under N\'eel vector reversal. In altermagnets and ferromagnets the RIXS-CD spectra for time-reversed states are, in general, independent except for the special case when there is a unitary symmetry of the Hamiltonian connecting the

cond-mat.mtrl-sci

Circular Dichroism in Resonant Inelastic X-ray Scattering: Probing Altermagnetic Domains in MnTe

X-ray magnetic circular dichroism provides a means to identify ferromagnetic, chiral, and altermagnetic orders via their time-reversal-symmetry ($\mathcal{T}$) breaking. However, differentiating magnetic domains related by crystallographic symmetries remains a technical challenge. Here we reveal a circular dichroism (CD) in the resonant inelastic x-ray scattering (RIXS) spectra from the altermagnetic MnTe. The azimuthal dependence of the RIXS-CD intensity of the magnon excitations indicates a dominant occupation of a single altermagnetic domain. The RIXS-CD in our scattering geometry is ascribed to the mirror-symmetry breaking associated with the $\mathcal{T}$-broken altermagnetic order. Our results establish RIXS-CD as a domain-sensitive probe of elementary excitations in quantum materials.

cond-mat.str-el

Magnetic Dichroism in Rutile NiF$_2$: Separating Altermagnetic and Ferromagnetic Effects

We present numerical simulations of x-ray magnetic circular dichroism (XMCD) at the L$_{2,3}$ edge of Ni in the weakly ferromagnetic altermagnet NiF$_2$. Our results predict a significant XMCD signal for light propagating perpendicular to the magnetic moments, which are approximately aligned along the [100] easy-axis direction. The analysis shows that the altermagnetic and ferromagnetic contributions to the XMCD signal can be uniquely distinguished by their dependence on an applied magnetic field. By varying the angle of the field relative to the easy axis, the in-plane orientation of both the N\'eel vector and the net magnetization can be systematically controlled. We further demonstrate that the XMCD signal, even under fields as strong as 40 T and for any in-plane orientation, can be accurately described as a linear combination of two spectral components, with geometrical prefactors determined by the field magnitude and direction. This insight enables experimental validation of the distinctive relationship between the N\'eel vector orientation and the x-ray Hall vector in the rutile structure. Quantitative simulations supporting these findings are provided.

cond-mat.mtrl-sci

Determination of the N\'eel vector in rutile altermagnets through x-ray magnetic circular dichroism: the case of MnF$_2$

We present a numerical simulation of the X-ray magnetic circular dichroism (XMCD) at the $L_{2,3}$ edge of Mn in altermagnetic MnF$_2$ using a combination of density functional + exact diagonlization of an atomic model. We explore how the dichroic spectra vary with the light propagation vector and the N\'eel vector. We show how XMCD in rutile structures can be employed to determine the orientation of the N\'eel vector. An exact relationship between the XMCD spectra for different orientation of the N\'eel vector valid in the absence on the valence spin-orbit coupling and core-valence multipole interaction is derived and its approximate validity demonstrated by numerical calculation for the full Hamiltonian.

cond-mat.str-el

Fingerprints of Mott and Slater gaps in the core-level photoemission spectra of antiferromagnetic iridates

We present Ir $4f$ core-level hard-x-ray photoemission spectroscopy (HAXPES) experiments conducted across antiferromagnetic (AFM) ordering transition in Ruddlesden-Popper iridates Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$. The Ir $4f$ spectra exhibit distinct changes between the AFM and paramagnetic (PM) phases, with the spectral difference $I_\text{PM}-I_\text{AFM}$ showing a contrasting behavior in the two compounds. By employing computational simulations using the local-density approximation combined with the dynamical mean-field theory method, we elucidate that $I_\text{PM}-I_\text{AFM}$ primary reflects the Slater or Mott-Hubbard character of the AFM insulating state rather than material specific details. This sensitivity to fine low-energy electronic structure arises from the dependence of charge-transfer responses to the sudden creation of a localized core hole on both metal-insulator transitions and long-range AFM ordering. Our result broadens the applications of core-level HAXPES as a tool for characterization of electronic structure.

cond-mat.str-el

X-ray Magnetic Circular Dichroism in RuO$_2$

We present numerical simulation of the X-ray magnetic circular dichroism (XMCD) of the $L_{2,3}$ and $M_{2,3}$ edges of Ru in antiferromagnetic RuO$_2$ using a combination of density functional + dynamical mean-field theory and configuration interaction treatment of Anderson impurity model. We study the dependence of the dichroic spectra on the orientation of the Néel vector and discuss it in the context of altermagnetism. Approximate equivalence between the XMCD spectra for geometries with X-rays propagating parallel and perpendicular to the Néel vector is found and shown to be exact in absence of valence spin-orbit coupling and core-valence multipolar interaction.

cond-mat.str-el

X-ray Magnetic Circular Dichroism in Altermagnetic $α$-MnTe

Altermagnetism is a recently identified magnetic symmetry class combining characteristics of conventional collinear ferromagnets and antiferromagnets, that were regarded as mutually exclusive, and enabling phenomena and functionalities unparalleled in either of the two traditional elementary magnetic classes. In this work we use symmetry and ab initio theory to explore X-ray magnetic circular dichroism (XMCD) in the altermagnetic class. Our results highlight the distinct phenomenology in altermagnets of this time-reversal symmetry breaking response, and its potential utility for element-specific spectroscopy and microscopy in altermagnets. As a representative material for our XMCD study we choose $α$-MnTe with the compensated antiparallel magnetic order in which an anomalous Hall effect has been already demonstrated both in theory and experiment. The predicted magnitude of XMCD lies well within the resolution of existing experimental techniques.

cond-mat.mtrl-sci

Hidden covalent insulator and spin excitations in SrRu$_2$O$_6$

The density functional plus dynamical mean-field theory is used to study the spin excitation spectra of SrRu$_2$O$_6$. A good quantitative agreement with experimental spin excitation spectra is found. Depending on the size of the Hund's coupling $J_H$ the systems chooses either Mott insulator or covalent insulator state when magnetic ordering is not allowed. We find that the nature of the paramagnetic state has negligible influence on the charge and spin excitation spectra. We find that antiferromagnetic correlations hide the covalent insulator state for realistic choices of the interaction parameters.

cond-mat.str-el

Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd$_3$ to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature - the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

cond-mat.str-el

CaCu$_3$Ru$_4$O$_{12}$: a high Kondo-temperature transition metal oxide

We present a comprehensive study of CaCu$_3$Ru$_4$O$_{12}$ using bulk sensitive hard and soft x-ray spectroscopy combined with local-density approximation (LDA) + dynamical mean-field theory (DMFT) calculations. Correlation effects on both the Cu and Ru ions can be observed. From the Cu $2p$ core level spectra we deduce the presence of magnetic Cu$^{2+}$ ions hybridized with a reservoir of itinerant electrons. The strong photon energy dependence of the valence band allows us to disentangle the Ru, Cu, and O contributions and thus to optimize the DMFT calculations. The calculated spin and charge susceptibilities show that the transition metal oxide CaCu$_3$Ru$_4$O$_{12}$ must be classified as a Kondo system and that the Kondo temperature is in the range of 500-1000 K.

cond-mat.str-el

Hard x-ray photoemission study on strain effect in LaNiO$_3$ thin films

The strain effect from a substrate is an important experimental route to control electronic and magnetic properties in transition-metal oxide (TMO) thin films. Using hard x-ray photoemission spectroscopy, we investigate the strain dependence of the valence states in LaNiO$_{3}$ thin films, strongly correlated perovskite TMO, grown on four substrates: LaAlO$_{3}$, (LaAlO$_{3}$)$_{0.3}$(SrAl$_{0.5}$Ta$_{0.5}$O$_{3}$)$_{0.7}$, SrTiO$_{3}$, and DyScO$_{3}$. A Madelung potential analysis of core-level spectra suggests that the point-charge description is valid for the La ions while it breaks down for Ni and O ions due to a strong covalent bonding between the two. A clear x-ray photon-energy dependence of the valence spectra is analyzed by the density functional theory, which points to a presence of the La 5$p$ state near the Fermi level.

cond-mat.str-el

Collective Modes in Excitonic Magnets: Dynamical Mean-Field Study

We present a dynamical mean-field study of dynamical susceptibilities in two-band Hubbard model. Varying the model parameters we analyze the two-particle excitations in the normal as well as in the ordered phase, an excitonic condensate. The two-particle DMFT spectra in the ordered phase reveal the gapless Goldstone modes arising from spontaneous breaking of continuous symmetries. We also observe gapped Higgs mode, characterized by vanishing of the gap at the phase boundary. Qualitative changes observed in the spin susceptibility can be used as an experimental probe to identify the excitonic condensation.

cond-mat.str-el

Excitonic magnet in external field: complex order parameter and spin currents

We investigate spin-triplet exciton condensation in the two-orbital Hubbard model close to half filling by means of dynamical mean-field theory. Employing an impurity solver that handles complex off-diagonal hybridization functions, we study the behavior of excitonic condensate in stoichiometric and doped systems subject to external magnetic field. We find a general tendency of the triplet order parameter to lay perpendicular with the applied field and identify exceptions from this rule. For solutions exhibiting k-odd spin textures, we discuss the Bloch theorem which, in the absence of spin-orbit coupling, forbids the appearance of spontaneous net spin current. We demonstrate that the Bloch theorem is not obeyed by the dynamical mean-field theory.

cond-mat.str-el