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Y. Fujisawa

Publications and source records attributed to Y. Fujisawa.

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Realization of a parity-violating antiferromagnetic state in LaMnSi

Spontaneous symmetry breaking underlies functional electronic phenomena in quantum materials. Breaking space-inversion ($\mathcal{P}$) or time-reversal ($\mathcal{T}$) symmetry can generate spin-split electronic bands central to modern spintronics. By contrast, parity-violating antiferromagnetic (AFM) order breaks both $\mathcal{P}$ and $\mathcal{T}$ while preserving the combined $\mathcal{PT}$ symmetry, enabling spin-degenerate yet momentum-asymmetric electronic bands. This momentum asymmetry has been proposed as a microscopic origin of unconventional nonreciprocal and nonlinear responses but its experimental verification has remained challenging because it requires establishing both the symmetry-breaking magnetic order and the associated electronic structure. Here we combine soft x-ray angle-resolved photoemission spectroscopy (ARPES) and polarization-resolved optical second-harmonic generation (SHG) microscopy to study LaMnSi, a candidate parity-violating AFM metal. Soft x-ray ARPES resolves the three-dimensional bulk band structures in agreement with density functional theory calculations for the AFM phase, whereas SHG microscopy detects sign-reversing nonlinear optical responses from opposite AFM domains that carry $\mathcal{T}$-odd parity-violating order. Together, these results provide direct evidence for parity-violating AFM state in LaMnSi, establish LaMnSi as a parity-violating AFM metal, and identify this class of AFMs as a promising platform for symmetry-controlled nonreciprocal and nonlinear electronic responses.

cond-mat.mtrl-sci

Versatile multi-q antiferromagnetic charge order in correlated vdW metals

Following the discovery of graphene, interest in van der Waals (vdW) materials has surged; however, advancing physics beyond graphene requires quantum vdW materials platforms that host versatile, strongly interacting many-body states. Here, using scanning tunneling microscopy and spectroscopy at 300 mK, we uncover multiple competing electronic states in the van der Waals metal CeTe3: charge-ordered antiferromagnetic phases forming stripe and checkerboard orders. Remarkably, their competition is tuned by a modest in-plane magnetic field (~1.5 T), revealing strongly intertwined multiple frustrations involving antiferromagnetism, charge order, and Fermi-surface instabilities. Quasiparticle-interference imaging directly identifies the momentum-space origin of these competitions on the representative semimetals Fermi surface. While the observations can be understood at a basic level in terms of Kondo coupling between localized Ce 4f moments and itinerant Te 5p electrons, our results reveal a much richer phenomenology: an unusually broad electronic reconstruction extending to an energy scale of roughly 30 meV from EF, which realizes and deforms antiferromagnetic charge-ordered states and signals strongly correlated interactions beyond a weak-coupling description. Beyond establishing CeTe3 as a model platform, our results demonstrate that competing instabilities in antiferromagnetic two-dimensional metals/semimetals generate versatile electronic phases, opening a route to tunable nanoscale quantum states governed by the intertwined effects of correlation, symmetry, and topology.

cond-mat.str-el

Revealing Pronounced Electron-Hole Fermi Pockets in the Charge Density Wave Semimetal LaTe3

Rare earth tri-tellurides (RTe3) are van der Waals (vdW) coupled semimetals ideal for exploring exotic electronic phases. LaTe3 is especially important for understanding the fundamental Fermiology of the RTe3 family because it is non-magnetic and has a simpler charge density wave structure. In this study, we used spectroscopic-imaging scanning tunneling microscopy to measure the Landau levels of LaTe3 with high energy resolution at 300 mK. These measurements were taken under varying magnetic fields up to 15 T, with fine intervals of 0.02 - 0.03 T. Our results reveal a pair of pronounced electron-hole Fermi pockets of similar sizes and evidence of electron-boson coupling in both pockets. Given the strong charge susceptibility typical of low-dimensional conductors, the interactions and instabilities driven by the electron-hole Fermi pockets could be a basis for searching unexplored quantum phases in other antiferromagnetic RTe3 compounds.

cond-mat.str-el

Uncovering hidden Fermi surface instabilities through visualizing unconventional quasiparticle interference in CeTe3

The charge density wave (CDW) state is a widespread phenomenon in low-dimensional metals/semimetals. The spectral weight of the associated folded bands (shadow bands) can be an intriguing trigger leading to additional Fermi surface instability and unexplored phase transitions. The rare earth tri-telluride CeTe3 exhibits a single CDW stabilized below ~400 K and antiferromagnetism below ~3 K. The distinct periodicities between the Te-square net, the CeTe block layer, and the CDW give rise to rich shadow band formations. In this work, we reveal the predominant scattering between the original and shadow bands at 4 K, with the scattering within the original bands being relatively suppressed at Fermi energy. This unconventional quasi-particle scattering collectively underscores the vital role of the shadow bands' spectral weight and the hidden matrix element effect, which are crucial for controlling electronic properties in this system. Furthermore, our finding points to the existence of rich and unexplored Fermi surface instabilities, which potentially play a role in controlling the nature of long-range antiferromagnetism at lower temperatures in the presence of finite charge-spin interaction.

cond-mat.str-el

Emergent topological magnetism in Hund's excitonic insulator

Analogous to the charged electron-electron pair condensation in superconductors, an excitonic insulator (EI) represents Fermi surface instability due to spontaneous formation and condensation of charge-neutral electron-hole pair (exciton). Unlike in superconductors, however, the charge-neutral nature of exciton makes probing emergent EI phase via macroscopic physical properties generally difficult. Here, we propose a van der Waals coupled antiferromagnetic semiconductor GdGaI (GGI) as a new material category leading to emergent multi-q magnet intertwined with spontaneous exciton formation/condensation. Before excitonic band hybridization, a simple picture for the parent electronic state consists of electron (Gd-derived 5d) and hole (Ga-derived 4p) delocalized bands, together with Gd-derived 4f localized antiferromagnets with S = 7/2 classical nature. Through intra Gd atom 4f-5d Hund's coupling, a notable finding is the emergent minimum length scale (2a) Skyrmion-like spin texture resulting from spontaneous condensation/formation of spin-polarized exciton with BCS-BEC crossover phenomenology. This discovered platform is promising for realizing valuable quantum matter on the nanoscale; our finding will provide significant insight into designing the atomic scale topological magnetism out of itinerant systems.

cond-mat.str-el

Widely Tunable Berry curvature in the Magnetic Semimetal Cr1+dTe2

Magnetic semimetals have increasingly emerged as lucrative platforms hosting spin-based topological phenomena in real and momentum spaces. Of particular interest is the emergence of Berry curvature, whose geometric origin, accessibility from Hall transport experiments, and material tunability, bodes well for new physics and practical devices. Cr1+dTe2, a self-intercalated magnetic transition metal dichalcogenide, TMD, exhibits attractive natural attributes relevant to such applications, including topological magnetism, tunable electron filling, magnetic frustration etc. While recent studies have explored real-space Berry curvature effects in this material, similar considerations of momentum-space Berry curvature are lacking. Here, we systematically investigate the electronic structure and transport properties of epitaxial Cr1+dTe2 thin films over a wide range of doping, d between 0.33 and 0.71. Spectroscopic experiments reveal the presence of a characteristic semi-metallic band region near the Brillouin Zone edge, which shows a rigid band like energy shift as a function of d. Transport experiments show that the intrinsic component of the anomalous Hall effect, AHE, is sizable, and undergoes a sign flip across d. Finally, density functional theory calculations establish a causal link between the observed doping evolution of the band structure and AHE: the AHE sign flip is shown to emerge from the sign change of the Berry curvature, as the semi-metallic band region crosses the Fermi energy. Our findings underscore the increasing relevance of momentum-space Berry curvature in magnetic TMDs and provide a unique platform for intertwining topological physics in real and momentum spaces.

cond-mat.mtrl-sci

Enhanced $d$-$p$ hybridization intertwined with anomalous ground state formation in van der Waals-coupled magnetic metal Fe$_5$GeTe$_2$

Fe$_5$GeTe$_2$ is a van der Waals (vdW)-coupled unconventional ferromagnetic metal with a high Curie temperature ($T_C$) exceeding 300 K. The formation of an anomalous ground state significantly below $T_C$ has received considerable attention, resulting in increased interest in understanding the spin-polarized electronic state evolution near the Fermi energy ($E_F$) as a function of temperature. Despite recent extensive studies, a microscopic understanding of the spin-polarized electronic structure around $E_F$ has not yet been established owing to the intrinsic complexity of both the crystal and band structures. In this study, we investigate the temperature dependence of element-specific soft X-ray magnetic circular dichroism (XMCD). A systematic temperature evolution in the XMCD signal from both magnetic Fe and its ligand Te is clearly observed. More importantly, the enhancement in the hybridization between the Fe 3$d$ and Te 5$p$ states in the zero-magnetic field limit is revealed, and we discuss its implications on the possible emergence of an exotic magnetic ground state in Fe$_5$GeTe$_2$.

cond-mat.str-el

Itinerant ferromagnetism mediated by giant spin polarization of metallic ligand band in van der Waals magnet Fe5GeTe2

We investigate near-Fermi-energy (EF) element-specific electronic and spin states of ferromagnetic van der Waals (vdW) metal Fe5GeTe2. The soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurement provides spectroscopic evidence of localized Fe 3d band. We also find prominent hybridization between the localized Fe 3d band and the delocalized Ge/Te p bands. This picture is strongly supported from direct observation of the remarkable spin polarization of the ligand p bands near EF, using x-ray magnetic circular dichroism (XMCD) measurements. The strength of XMCD signal from ligand element Te shows the highest value, as far as we recognize, among literature reporting finite XMCD signal for none-magnetic element in any systems. Combining SX-ARPES and elemental selective XMCD measurements, we collectively point an important role of giant spin polarization of the delocalized ligand Te states for realizing itinerant long-range ferromagnetism in Fe5GeTe2. Our finding provides a fundamental elemental selective view-point for understanding mechanism of itinerant ferromagnetism in low dimensional compounds, which also leads insight for designing exotic magnetic states by interfacial band engineering in heterostructures.

cond-mat.str-el

Tailoring Magnetism in Self-intercalated Cr1+δTe2 Epitaxial Films

Magnetic transition metal dichalcogenide (TMD) films have recently emerged as promising candidates to host novel magnetic phases relevant to next-generation spintronic devices. However, systematic control of the magnetization orientation, or anisotropy, and its thermal stability, characterized by Curie temperature (Tc) remains to be achieved in such films. Here we present self-intercalated epitaxial Cr1+δTe2 films as a platform for achieving systematic/smooth magnetic tailoring in TMD films. Using a molecular beam epitaxy (MBE) based technique, we have realized epitaxial Cr1+δTe2 films with smoothly tunable over a wide range (0.33-0.82), while maintaining NiAs-type crystal structure. With increasing δ, we found monotonic enhancement of Tc from 160 to 350 K, and the rotation of magnetic anisotropy from out-of-plane to in-plane easy axis configuration for fixed film thickness. Contributions from conventional dipolar and orbital moment terms are insufficient to explain the observed evolution of magnetic behavior with δ. Instead, ab initio calculations suggest that the emergence of antiferromagnetic interactions with δ, and its interplay with conventional ferromagnetism, may play a key role in the observed trends. To our knowledge, this constitutes the first demonstration of tunable Tc and magnetic anisotropy across room temperature in TMD films, and paves the way for engineering novel magnetic phases for spintronic applications.

cond-mat.mtrl-sci

Fermionic Order by Disorder in a van der Waals Antiferromagnet

CeTe3 is a unique platform to investigate the itinerant magnetism in a van der Waals (vdW) coupled metal. Despite chemical pressure being a promising route to boost quantum fluctuation in this system, a systematic study on the chemical pressure effect on Ce3+(4f1) states is absent. Here, we report on the successful growth of a series of Se doped single crystals of CeTe3. We found a fluctuation driven exotic magnetic rotation from the usual easy-axis ordering to an unusual hard-axis ordering. Unlike in localized magnetic systems, near-critical magnetism can increase itinerancy hand-in-hand with enhancing fluctuation of magnetism. Thus, seemingly unstable hard-axis ordering emerges through kinetic energy gain, with the self-consistent observation of enhanced magnetic fluctuation (disorder). As far as we recognize, this order-by-disorder process in fermionic system is observed for the first time within vdW materials. Our finding opens a unique experimental platform for direct visualization of the rich quasiparticle Fermi surface deformation associated with the Fermionic order-by-disorder process. Also, the search for emergent exotic phases by further tuning of quantum fluctuation is suggested as a promising future challenge.

cond-mat.str-el

Effect of Lead Substitution on LaO0.5F0.5BiS2

We examined Lead (Pb) Substitution effect on a single crystal of a layered superconductor LaO0.5F0.5BiS2. Pb concentration dependence of the lattice constant showed slight anomaly at about 8% and 9% substitution of Pb for Bi. These samples showed the enhancement of the superconducting transition temperature and the superconducting volume fraction. Furthermore, these samples showed the anomaly in the temperature dependence of the resistivity at about 150K. These results were not observed in Pb substituted NdO0.7F0.3BiS2. Therefore, the enhancement of the superconducting properties by Pb substitution is related to the structural instability for the pale perturbation in LaO0.5F0.5BiS2.

cond-mat.supr-con

Enhancement of Tc in BiS2 based superconductors NdO0.7F0.3BiS2 by substitution of Pb for Bi

We succeed in enhancement of a superconducting transition temperature (Tc) for NdO0.7F0.3BiS2 single crystal by partial substitution of Pb for Bi. The Tc increases with increasing Pb concentration until 6%. The maximum Tczero is 5.6 K, which is the highest value among BiS2 based superconductors synthesized under an ambient pressure. Pb substitution for Bi induces lattice shrinkage along the c axis. These results reflect that superconductivity in this system is responsive to the lattice strain.

cond-mat.supr-con

Visualizing the Pt doping effect on surface and electronic structure in Ir_{1-x}Pt_{x}Te_{2} by scanning tunneling microscopy and spectroscopy

We report on the Pt doping effect on surface and electronic structure in Ir$_{\mathrm{1-x}}$Pt$_{\mathrm{x}}$Te$_ {\mathrm{2}}$ by scanning tunneling microscopy (STM) and spectroscopy (STS). The surface prepared by cleavage at 4.2 K shows a triangular lattice of topmost Te atoms. The compounds that undergo structural transition have supermodulation with a fixed wave vector $q = \frac{2π}{5a_m}$ (where $a_m$ is the lattice constant in the monoclinic phase) despite the different Pt concentrations. The superconducting compounds show patch structures. The surface of the compound that exhibits neither the superconductivity nor the structural transition shows no superstructure. In all doped samples, the dopant is observed as a dark spot in STM images. The tunneling spectra near the dopant show the change in the local density of state at approximately -200 mV. Such microscopic effects of the dopant give us the keys for establishing a microscopic model of this material.

cond-mat.supr-con

Checkerboard stripe electronic state on cleaved surface of NdO$_{0.7}$F$_{0.3}$BiS$_{2}$ probed by scanning tunneling microscope

We present scanning tunneling microscopy measurements on a cleaved surface of the recently discovered superconductor NdO$_{0.7}$F$_{0.3}$BiS$_{2}$ with a transition temperature ($T_{\mathrm{c}}$) of 5.1 K.Tunneling spectra at 4.2 K (below $T_{\mathrm{c}}$) and 22 K (above $T_{\mathrm{c}}$) show a large spectroscopic gap ($\sim$40 mV), which is inconsistent with the metallic nature demonstrated in bulk measurements. Moreover, we find two interesting real-space electronic features. The first feature is a `checkerboard stripe' electronic state characterized by an alternating arrangement of two types of nanocluster. In one cluster, one-dimensional electronic stripes run along one Bi-Bi direction, whereas, in the other cluster, the stripes run along the other Bi-Bi direction. The second feature is a nanoscale electronic inhomogeneity whose microscopic source seems to be atomic defects on the cleaved surface or dopant F atoms.

cond-mat.supr-con

Visualization of the effect of structural supermodulation on electronic structure in IrTe$_{2}$ by scanning tunneling spectroscopy

We report on the scanning tunneling spectroscopy experiments on single crystals of IrTe$_{2}$. A structural supermodulation and a local density-of-states (LDOS) modulation with a wave vector of $q$ = 1/5$\times$$2π/a_{0}$ ($a_{0}$ is the lattice constant in the $ab$-plane) have been observed at 4.2K where the sample is in the monoclinic phase. %We cannot find an energy gap emerging reproducibly.% on the region where the supermodulation resides. As synchronized with the supermodulation, the LDOS spatially modulates within two energy ranges (below -200 meV and around -100 meV). We further investigated the effect of the local perturbations including the antiphase boundaries and the twin boundaries on the LDOS. These perturbations also modify the LDOS below -200 meV and around -100 meV, even though the lattice distortions induced by these perturbations appear to be different from those by the supermodulation. Our results indicating several microscopic structural effects on the LDOS seem to offer crucial keys for the establishment of the microscopic model describing the parent state.

cond-mat.str-el