arXiv subjects

Jun Fujii

Publications and source records attributed to Jun Fujii.

At least 19 recordsLinked to original sources

arXiv2026

Rashba engineering at van der Waals interfaces

Two-dimensional transition metal dichalcogenide (TMD) interfaces offer a versatile platform for studying emergent quantum phenomena and enabling novel device functionalities. When distinct TMD monolayers are stacked vertically or laterally stitched, their interfaces can exhibit unique electronic band alignments, giving rise to long-lived interlayer excitons, charge transfer effects, and moir\'e superlattices with correlated states. Here, we demonstrate that the interface between a large variety of two different epitaxially grown TMD monolayers controls the intensity and sign of the Rashba spin splitting, which is probed using THz spintronic emission. Optimized TMD heterobilayers, such as HfSe$_2$/PtSe$_2$, show enhanced THz emission that surpass the spin-to-charge conversion efficiency of bulk TMDs, confirming the presence of Rashba states with large spin splitting at the interface. By combining spin- and angle-resolved photoemission spectroscopy with density functional theory, we reveal that the electronic hybridization between the two different TMD monolayers gives rise to extended in-gap states with strong Rashba spin-orbit coupling. The choice of TMD layers enables to engineer the sign and strength of spin-to-charge conversion in van der Waals heterobilayers opening up perspectives to build efficient and tunable THz spintronic emitters.

cond-mat.mes-hall↗

arXiv2026

Emergent surface resonance from charge density wave symmetry breaking in TiSe2

Surface confined electronic states provide a fertile ground for discovering emergent phenomena that have no counterpart in the bulk, offering new routes to manipulate correlations, symmetry breaking, and dimensionality at the atomic scale. Here, we show that charge density wave (CDW) symmetry breaking can yield a surface states in 1T-TiSe2. Micro angle resolved photoemission spectroscopy resolves a sharp, two dimensional surface resonant state (SRS) that emerges within the CDW reconstructed low energy spectrum. The SRS exhibits notable temperature dependence and its spectral weight collapses around 160 K, while CDW transition temperature TCDW is commonly reported as 202 K. Slab DFT+U calculations reproduce a surface localized resonance when CDW folding brings valence and conduction states into near degeneracy, suggesting a correlation tuned, surface selective origin. These results point to a form of correlation-tuned surface resonance in a layered CDW compound and suggest a framework for engineering low dimensional quantum states in van der Waals materials via symmetry breaking and electronic structure tuning.

cond-mat.mtrl-sci↗

arXiv2026

Correlation-driven origin of shallow electron pocket in Co$_{1/3}$TaS$_2$ revealed by ARPES and cluster perturbation theory

We investigate the electronic structure and Fermi surface of Co$_{1/3}$TaS$_2$ using angle-resolved photoemission spectroscopy (ARPES) combined with theoretical modeling beyond standard density functional theory (DFT+U). A shallow electron pocket, the so-called $\beta$ feature, is observed at the Fermi level near the corner of the superlattice Brillouin zone, representing the first experimental observation of this feature in an intercalated TaS$_2$ compound. Similar pockets have been reported in $X_{1/3}$NbS$_2$ ($X$ = Co, Cr, Ni), where their surface versus bulk origin remains actively debated. Because conventional DFT+U does not capture this feature, we employ cluster perturbation theory (CPT) to incorporate an explicit treatment of strong electron correlations ($U$) on the Co sites. CPT successfully reproduces the $\beta$ feature, demonstrating its origin from correlation-driven bulk states rather than surface effects. To further substantiate this conclusion, we studied a reduced Co-content sample, Co$_{0.22}$TaS$_2$, where the reduced charge transfer modifies the Co-derived states near the Fermi level. Its electronic structure remains largely similar to that of pristine 2H-TaS$_2$, showing only a minor overall energy shift and lacking the $\beta$ feature, consistent with disrupted long-range Co ordering and modified orbital character near the Fermi level. We demonstrate that the $\beta$ feature arises from strong local correlations on the Co sites and requires long-range crystallographic order among intercalated Co atoms to maintain coherence. These results highlight the importance of strong electronic correlations in magnetically intercalated transition-metal dichalcogenides and provide a microscopic understanding of features not captured by conventional DFT+U.

cond-mat.str-el↗

arXiv2025

Mixed Triplet-Singlet Order Parameter in Decoupled Superconducting 1H Monolayers of Transition-Metal Dichalcogenides

Understanding the emergence of unconventional superconductivity, where the order parameter deviates from simple isotropic s-wave pairing, is a central puzzle in condensed matter physics. Transition-metal dichalcogenides (TMDCs), though generally regarded as conventional superconductors, display signatures of this unusual behavior and thus provide a particularly intriguing platform to explore how exotic states arise. Here we investigate the misfit compound (SnS)$_{1.15}$(TaS$_2$), a heterostructure composed of alternating SnS and 1H-TaS$_2$ layers. Using transport, photoemission, and scanning tunneling spectroscopy, we demonstrate that the SnS layers effectively decouple the TaS$_2$ into electronically isolated 1H sheets. In this limit, the tunneling density of states reveals a clear two-gap superconducting spectrum with T$_c \sim$ 3.1 K. A theoretical model based on lack of inversion symmetry and finite-range attraction reproduces the observed multi-gap structure as a mixed singlet-triplet state. These results establish misfit compounds as a powerful platform for studying unconventional superconductivity in isolated 1H layers and for realizing multiple uncoupled superconductors within a single crystal.

cond-mat.supr-con↗

arXiv2025

Strongly Entangled Kondo and Kagome Lattices and the Emergent Magnetic Ground State in Heavy-Fermion Kagome Metal YbV$_6$Sn$_6$

Applying angle-resolved photoemission spectroscopy and density functional theory calculations, we present compelling spectroscopic evidence demonstrating the intertwining and mutual interaction between the Kondo and kagome sublattices in heavy-fermion intermetallic compound YbV$_6$Sn$_6$. We reveal the Yb 4$f$-derived states near the Fermi level, along with the presence of bulk kagome bands and topological surface states. We unveil strong interactions between the 4$f$ and itinerant electrons, where the kagome bands hosting the Dirac fermions and van Hove singularities predominate. Such findings are well described using a $c$-$f$ hybridization model. On the other hand, our systematic characterization of magnetic properties demonstrates an unusually enhanced antiferromagnetic ordering, where the kagome-derived van Hove singularities near $E_F$ play a vital role in determining the unconventional nature of the Ruderman-Kittel-Kasuya-Yosida interaction and Kondo coupling. These unique kagome-state-mediated exchange interactions have never been reported before and could lead to a novel phase diagram and various quantum critical behaviors in YbV$_6$Sn$_6$ and its siblings. Our results not only expand the family of exotic quantum phases entangled with kagome structure to the strongly correlated regime, but also establish YbV$_6$Sn$_6$ as an unprecedented platform to explore unconventional many-body physics beyond the standard Kondo picture.

cond-mat.str-el↗

arXiv2025

Spatial Control of Charge Doping in n-Type Topological Insulators

Spatially controlling the Fermi level of topological insulators and keeping its electronic states stable are indispensable processes to put this material into practical use for semiconductor spintronics devices. So far, however, such a method has not been established yet. Here we show a novel method for doping hole into n-type topological insulators Bi$_2$X$_3$ (X= Se, Te) that overcomes the shortcomings of the previous reported methods. The key of this doping is to adsorb H$_2$O on Bi$_2$X$_3$ decorated with a small amount of carbon, and its trigger is the irradiation of photon with sufficient energy to excite core-electrons of the outermost layer atoms. This method allows controlling the doping amount by the irradiation time, and acts as photolithography. Such a tunable doping makes it possible to design the electronic states at the nanometer scale, and thus paves a promising avenue toward the realization of novel spintronics devices based on topological insulators.

cond-mat.mes-hall↗

arXiv2025

Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el↗

arXiv2025

Anomalous spin-optical helical effect in Ti-based kagome metal

The kagome lattice stands as a rich platform for hosting a wide array of correlated quantum phenomena, ranging from charge density waves and superconductivity to electron nematicity and loop current states. Direct detection of loop currents in kagome systems has remained a formidable challenge due to their intricate spatial arrangements and the weak magnetic field signatures they produce. This has left their existence and underlying mechanisms a topic of intense debate. In this work, we uncover a hallmark reconcilable with loop currents: spin handedness-selective signals that surpass conventional dichroic, spin, and spin-dichroic responses. We observe this phenomenon in the kagome metal CsTi$_3$Bi$_5$ and we call it the anomalous spin-optical helical effect. This effect arises from the coupling of light' s helicity with spin-orbital electron correlations, providing a groundbreaking method to visualize loop currents in quantum materials. Our discovery not only enriches the debate surrounding loop currents but also paves the way for new strategies to exploit the electronic phases of quantum materials via light-matter interaction.

cond-mat.str-el↗

arXiv2024

Charge transfer and Spin-Valley locking in 4Hb-TaS$_{2}$

4Hb-TaS$_2$ is a superconductor that exhibits unique characteristics such as time-reversal symmetry breaking, hidden magnetic memory, and topological edge modes. It is a naturally occurring heterostructure comprising of alternating layers of 1H-TaS$_2$ and 1T-TaS$_2$. The former is a well-known superconductor, while the latter is a correlated insulator with a possible non-trivial magnetic ground state. In this study, we use angle resolved photoemission spectroscopy to investigate the normal state electronic structure of this unconventional superconductor. Our findings reveal that the band structure of 4H-TaS$_2$ fundamentally differs from that of its constituent materials. Specifically, we observe a significant charge transfer from the 1T layers to the 1H layers that drives the 1T layers away from half-filling. In addition, we find a substantial reduction in inter-layer coupling in 4Hb-TaS$_2$ compared to the coupling in 2H-TaS$_2$ that results in a pronounced spin-valley locking within 4Hb-TaS$_2$

cond-mat.supr-con↗

arXiv2024

Three-dimensional mapping of the altermagnetic spin splitting in CrSb

Altermagnetism, a kind of collinear magnetism that is characterized by a momentum-dependent band and spin splitting without net magnetization, has recently attracted considerable interest. Finding altermagnetic materials with large splitting near the Fermi level necessarily requires three-dimensional k-space mapping. While this is crucial for spintronic applications and emergent phenomena, it remains challenging. Here, using synchrotron-based angle-resolved photoemission spectroscopy (ARPES), spin-resolved ARPES and model calculations, we uncover a large altermagnetic splitting, up to ~1.0 eV, near the Fermi level in CrSb. We verify its bulk-type g-wave altermagnetism through systematic three-dimensional k-space mapping, which unambiguously reveals the altermagnetic symmetry and associated nodal planes. Spin-resolved ARPES measurements further verify the spin polarizations of the split bands near Fermi level. Tight-binding model analysis indicates that the large altermagnetic splitting arises from strong third-nearest-neighbor hopping mediated by Sb ions. The large band/spin splitting near Fermi level in metallic CrSb, together with its high TN (up to 705 K) and simple spin configuration, paves the way for exploring emergent phenomena and spintronic applications based on altermagnets.

cond-mat.mtrl-sci↗

arXiv2024

Uncovering the lowest thickness limit for room-temperature ferromagnetism of Cr$_{1.6}$Te$_{2}$

Metallic ferromagnetic transition metal dichalcogenides have emerged as important building blocks for scalable magnonics and memory applications. Downscaling such systems to the ultra-thin limit is critical to integrate them into technology. Here, we achieved layer-by-layer control over the transition metal dichalcogenide Cr$_{1.6}$Te$_{2}$ by using pulsed laser deposition, and we uncovered the minimum critical thickness above which room temperature magnetic order is maintained. The electronic and magnetic structure is explored experimentally and theoretically and it is shown that the films exhibit strong in-plane magnetic anisotropy as a consequence of large spin-orbit effects. Our study elucidates both magnetic and electronic properties of Cr$_{1.6}$Te$_{2}$, and corroborates the importance of intercalation to tune the magnetic properties of nanoscale materials architectures.

cond-mat.mtrl-sci↗

arXiv2024

Signatures of a surface spin-orbital chiral metal

The relation between crystal symmetries, electron correlations, and electronic structure steers the formation of a large array of unconventional phases of matter, including magneto-electric loop currents and chiral magnetism. Detection of such hidden orders is a major goal in condensed matter physics. However, to date, nonstandard forms of magnetism with chiral electronic ordering have been experimentally elusive. Here, we develop a theory for symmetry-broken chiral ground states and propose a methodology based on circularly polarized spin-selective angular-resolved photoelectron spectroscopy to probe them. We exploit the archetypal quantum material Sr2RuO4 and reveal spectroscopic signatures which, even though subtle, may be reconciled with the formation of spin-orbital chiral currents at the material surface. As we shed light on these chiral regimes, our findings pave the way for a deeper understanding of ordering phenomena and unconventional magnetism.

cond-mat.str-el↗

arXiv2023

Observation of termination-dependent topological connectivity in a magnetic Weyl kagome-lattice

Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designer, with the opportunity of driving new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co$_3$Sn$_2$S$_2$ and show how for different sample's terminations the Weyl-points connect also differently, still preserving the bulk-boundary correspondence. Scanning-tunnelling microscopy has suggested such a scenario indirectly. Here, we demonstrate this directly for the fermiology of Co$_3$Sn$_2$S$_2$, by linking it to the system real space surfaces distribution. By a combination of micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co$_3$Sn$_2$S$_2$ for different surface terminations and show the existence of topological features directly depending on the top-layer electronic environment. Our work helps to define a route to control bulk-derived topological properties by means of surface electrostatic potentials, creating a realistic and reliable methodology to use Weyl kagome metals in responsive magnetic spintronics.

cond-mat.str-el↗

arXiv2023

The electronic structure of intertwined kagome, honeycomb, and triangular sublattices of the intermetallics MCo$_2$Al$_9$

Intermetallics are an important playground to stabilize a large variety of physical phenomena, arising from their complex crystal structure. The ease of their chemical tuneabilty makes them suitable platforms to realize targeted electronic properties starting from the symmetries hidden in their unit cell. Here, we investigate the family of the recently discovered intermetallics MCo$_2$Al$_9$ (M: Sr, Ba) and we unveil their electronic structure for the first time. By using angle-resolved photoelectron spectroscopy and density functional theory calculations, we discover the existence of Dirac-like dispersions as ubiquitous features in this family, coming from the hidden kagome and honeycomb symmetries embedded in the unit cell. Finally, from calculations, we expect that the spin-orbit coupling is responsible for opening energy gaps in the electronic structure spectrum, which also affects the majority of the observed Dirac-like states. Our study constitutes the first experimental observation of the electronic structure of MCo$_2$Al$_9$ and proposes these systems as hosts of Dirac-like physics with intrinsic spin-orbit coupling. The latter effect suggests MCo$_2$Al$_9$ as a future platform for investigating the emergence of non-trivial topology.

cond-mat.str-el↗

arXiv2023

Flat band separation and robust spin-Berry curvature in bilayer kagome metals

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV$_6$Sn$_6$ kagome family (where X is a rare earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin-orbit coupling gaps. These states would carry a finite spin-Berry curvature, and topological surface states. Here, we investigate the spin and electronic structure of the XV$_6$Sn$_6$ kagome family. We obtain evidence for a finite spin-Berry curvature contribution at the center of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin-orbit coupling. In addition, the spin-Berry curvature is further investigated in the charge density wave regime of ScV$_6$Sn$_6$, and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin-Berry curvature of topological kagome metals, and helps to define its spectroscopic fingerprint.

cond-mat.str-el↗

arXiv2023

Dynamics and Resilience of the Charge Density Wave in a bilayer kagome metal

Long-range electronic order descending from a metallic parent state constitutes a rich playground to study the intricate interplay of structural and electronic degrees of freedom. With dispersive and correlation features as multifold as topological Dirac-like itinerant states, van-Hove singularities, correlated flat bands, and magnetic transitions at low temperature, kagome metals are located in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave (CDW) transition, and the van-Hove singularities, which are intrinsic to the kagome tiling, have been conjectured to play a key role in mediating such an instability. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the topological bilayer kagome metal ScV6Sn6 as a platform to investigate this puzzling problem, since it features both kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a CDW phase that affects the susceptibility, the neutron scattering, and the specific heat, similarly to the siblings AV3Sb5 (A = K, Rb, Cs) and FeGe. We report on our findings from high-resolution angle-resolved photoemission, density functional theory, and time-resolved optical spectroscopy to unveil the dynamics of its CDW phase. We identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order. Along with a comprehensive analysis of the subdominant impact from electronic correlations, we find ScV6Sn6 to feature an instance of charge density wave order that predominantly originates from phonons. As we shed light on the emergent phonon profile in the low-temperature ordered regime, our findings pave the way for a deeper understanding of ordering phenomena in all CDW kagome metals.

cond-mat.str-el↗

arXiv2023

Observation of highly anisotropic bulk dispersion and spin-polarized topological surface states in CoTe2

We present CoTe2 as a new type-II Dirac semimetal supporting Lorentz symmetry violating Dirac fermions in the vicinity of the Fermi energy. By combining first principle ab-initio calculations with experimental angle-resolved photo-emission spectroscopy results, we show the CoTe2 hosts a pair of type-II Dirac fermions around 90 meV above the Fermi energy. In addition to the bulk Dirac fermions, we find several topological band inversions in bulk CoTe2, which gives rise to a ladder of spin-polarized surface states over a wide range of energies. In contrast to the surface states which typically display Rashba-type in-plane spin splitting, we find that CoTe2 hosts novel out-of-plane spin polarization as well. Our work establishes CoTe2 as a potential candidate for the exploration of Dirac fermiology and applications in spintronic devices, infrared plasmonics, and ultrafast optoelectronics.

cond-mat.mtrl-sci↗

arXiv2023

Discovery of a magnetic Dirac system with large intrinsic non-linear Hall effect

Magnetic materials exhibiting topological Dirac fermions are attracting significant attention for their promising technological potential in spintronics. In these systems, the combined effect of the spin-orbit coupling and magnetic order enables the realization of novel topological phases with exotic transport properties, including the anomalous Hall effect and magneto-chiral phenomena. Herein, we report experimental signature of topological Dirac antiferromagnetism in TaCoTe2 via angle-resolved photoelectron spectroscopy (ARPES) and first-principles density functional theory (DFT) calculations. In particular, we find the existence of spin-orbit coupling-induced gaps at the Fermi level, consistent with the manifestation of a large intrinsic non-linear Hall conductivity. Remarkably, we find that the latter is extremely sensitive to the orientation of the N\'eel vector, suggesting TaCoTe2 a suitable candidate for the realization of non-volatile spintronic devices with an unprecedented level of intrinsic tunability.

cond-mat.str-el↗