arXiv subjects

Kenta Kuroda

Publications and source records attributed to Kenta Kuroda.

At least 19 recordsLinked to original sources

arXiv2026

Tunable competing optical excitation pathways in the topological surface states of Bi$_2$Te$_3$

Understanding coherent optical responses of topological surface states (TSSs) requires disentangling excitation pathways from the electronic band structure. Here, using angle-resolved two-photon photoemission spectroscopy, we identify two distinct excitation pathways in the TSSs of Bi$_2$Te$_3$: an off-resonant transition via virtual states and a resonant transition via unoccupied intermediate states. A pronounced modulation of the spectral response is observed, revealing a competition between the two coherent pathways. This competition is tunable via temperature-induced shifts of the chemical potential, which selectively modify the resonant channel. These results provide microscopic insight into the optical excitation mechanisms of TSSs and highlight the potential for controlling their optical responses, relevant for future spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

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↗

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

Observation of spin splitting in the surface electronic structure of antiferromagnet NdBi

Spin splitting in electronic band structures via antiferromagnetic orders is a new route to control spin-polarized carriers that is available for spintronics applications. Here, we investigated the spin degree of freedom in the electronic band structures of the antiferromagnet NdBi using laser-based spin- and angle-resolved photoemission spectroscopy (laser-SARPES). Our laser-SARPES experiments revealed that the two surface bands that appear in the antiferromagnetic state are spin-polarized in opposite directions as a counterpart of the spin splitting. Moreover, we observed that the spin polarization is antisymmetric to the electron momentum, indicating that spin degeneracy is lifted due the breaking of inversion symmetry at the surface. These results are well reproduced by our density functional theory calculations with the single-q magnetic structure, implying that the spin-split surface state is determined by the breaking of inversion symmetry in concert with the antiferromagnetic order.

cond-mat.mtrl-sci↗

arXiv2025

Hedgehog-like spin texture in Sb-doped MnBi$_2$Te$_4$

We employ spin- and angle-resolved photoemission spectroscopy and circular-dichroism ARPES to systematically investigate the spin texture of Sb-doped MnBi$_2$Te$_4$. Our results display a hedgehog-like spin texture in this system which is signified by reversed-orienting out-of-plane spins at the Dirac gap. Our finding reveals the presence of time-reversal symmetry breaking, implying the possibility for realization of high-temperature quantum anomalous Hall effect.

cond-mat.mtrl-sci↗

arXiv2024

Emergence of high-mobility carriers in topological kagome bad metal Mn$_3$Sn by intense photoexcitation

Kagome-lattice materials offer novel playgrounds of exploring topologically nontrivial states of electrons under influence of many-body interactions. A noncollinear kagome antiferromagnet Mn$_3$Sn has attracted particular interest for application in spintronics owing to the large anomalous Hall effect related to the Weyl dispersion near the Fermi energy. In addition, strong electronic correlation suggesting the Kondo physics has also been implied. However, the effect of correlation on the band topology and their interplay remains elusive. Here, we investigate nonequilibrium Hall transport in a photoexcited Mn$_3$Sn using time-resolved terahertz Faraday rotation spectroscopy. In equilibrium, Mn$_3$Sn is a bad metal close to the Mott-Ioffe-Regal limit with low carrier mobility, and thus only the anomalous Hall effect is discerned. By contrast, intense photoexcitation beyond an approximate threshold gives rise to a clear cyclotron resonance, namely the normal Hall effect, indicating the emergence of unusual carriers with 50 times lighter effective mass and 40 times less scattering. The lifetime of high-mobility carriers as long as a few tens of picoseconds and a threshold-like behavior for the pump fluence are hardly explained by contribution of photoexcited hot carriers. Instead, the emergence of unusual carriers may be accounted for by dielectric screening of the on-site Coulomb interaction by high-density delocalized photocarriers. A possible role of electronic correlation in equilibrium transport in Mn$_3$Sn beyond the single-particle picture is discussed.

cond-mat.str-el↗

arXiv2024

GdAlSi: An antiferromagnetic topological Weyl semimetal with non-relativistic spin splitting

Spintronics has emerged as a viable alternative to traditional electronics based technologies in the past few decades. While on one hand, the discovery of topological phases of matter with protected spin-polarized states has opened up exciting prospects, recent revelation of intriguing non-relativistic spin splitting in collinear antiferromagnetic materials with unique symmetries facilitate a wide possibility of realizing both these features simultaneously. In this work, we report the co-existence of these two intriguing properties within a single material: GdAlSi. It crystallizes in a body-centered tetragonal structure with a non-centrosymmetric space group $I4_{1}md$ ($109$), which is confirmed using detailed structural analysis through X-ray diffraction (XRD) and optical second harmonic generation (SHG) measurements. The magnetization data indicates AFM ordering with an ordering temperature ($T_N$) $\sim$ 32 K. Ab-initio calculations reveal GdAlSi to be a collinear antiferromagnetic Weyl semimetal with an unconventional, momentum-dependent spin splitting, also referred to as altermagnet. Angle-resolved photoemission spectroscopy measurements on GdAlSi single crystals subsequently confirm the presence of Fermi arcs, a distinctive hallmark of Weyl semimetals. Electric and magnetic multipole analysis provides a deeper understanding of the symmetry-mediated, momentum-dependent spin splitting, which has strictly non-relativistic origin. To the best of our knowledge, such co-existence of unconventional antiferromagnetic order and non-trivial topology is unprecedented and has never been observed before in a single material, rendering GdAlSi a special and promising candidate material. We propose a device harnessing these features, poised to enable practical and efficient topotronic applications.

cond-mat.str-el↗

arXiv2024

Fermi Surface Nesting Driving the RKKY Interaction in the Centrosymmetric Skyrmion Magnet Gd2PdSi3

The magnetic skyrmions generated in a centrosymmetric crystal were recently first discovered in Gd2PdSi3. In light of this, we observe the electronic structure by angle-resolved photoemission spectroscopy (ARPES) and unveil its direct relationship with the magnetism in this compound. The Fermi surface and band dispersions are demonstrated to have a good agreement with the density functional theory (DFT) calculations carried out with careful consideration of the crystal superstructure. Most importantly, we find that the three-dimensional Fermi surface has extended nesting which matches well the q-vector of the magnetic order detected by recent scattering measurements. The consistency we find among ARPES, DFT, and the scattering measurements suggests the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction involving itinerant electrons to be the formation mechanism of skyrmions in Gd2PdSi3.

cond-mat.mtrl-sci↗

arXiv2024

Photoemission angular distribution beyond the single wavevector description of photoelectron final states

We develop a simulation procedure for angle-resolved photoemission spectroscopy (ARPES), where a photoelectron wave function is set to be an outgoing plane wave in a vacuum associated with the emitted photoelectron wave packet. ARPES measurements on the transition metal dichalcogenide $1T$-$\mathrm{Ti}\mathrm{S}_2$ are performed, and our simulations exhibit good agreement with experiments. Analysis of our calculated final state wave functions quantitatively visualizes that they include various waves due to the boundary condition and the uneven crystal potential. These results show that a more detailed investigation of the photoelectron final states is necessary to fully explain the photon-energy- and light-polarization-dependent ARPES spectra.

cond-mat.mtrl-sci↗

arXiv2024

Zone-selection effect of photoelectron intensity distributions in a nonsymmorphic system RAlSi (R : Ce and Nd)

We investigate the electronic structures of noncentrosymmetric Weyl semimetals RAlSi (R: Ce and Nd) using soft x-ray angle-resolved photoemission spectroscopy. We find that the photoelectron intensity distribution observed in the momentum-resolved electronic bands is highly sensitive to the covered Brillouin zone (BZ) due to the zone-selection effect arising from the nonsymmorphic crystal structure of RAlSi. Our data reconstruct the photoelectron distributions varied according to the zone-selection effect, and reveal comprehensive information about the electronic band structures reproduced by band calculations. This detailed information enables us to experimentally trace the Weyl-cone dispersion throughout three-dimensional momentum space, providing valuable insights into the unique properties of RAlSi.

cond-mat.str-el↗

arXiv2024

Broken Screw Rotational Symmetry in the Near-Surface Electronic Structure of $AB$-Stacked Crystals

We investigate the electronic structure of $2H$-$\mathrm{Nb}\mathrm{S}_2$ and $h$-$\mathrm{BN}$ by angle-resolved photoemission spectroscopy (ARPES) and photoemission intensity calculations. Although in bulk form, these materials are expected to exhibit band degeneracy in the $k_z=π/c$ plane due to screw rotation and time-reversal symmetries, we observe gapped band dispersion near the surface. We extract from first-principles calculations the near-surface electronic structure probed by ARPES and find that the calculated photoemission spectra from the near-surface region reproduce the gapped ARPES spectra. Our results show that the near-surface electronic structure can be qualitatively different from the bulk one due to partially broken nonsymmorphic symmetries.

cond-mat.mtrl-sci↗

arXiv2023

Anomalously large spin-dependent electron correlation in nearly half-metallic ferromagnet CoS$_2$

The spin-dependent band structure of CoS$_2$ which is a candidate for a half-metallic ferromagnet was investigated by both spin- and angle-resolved photoemission spectroscopy and theoretical calculations, in order to reappraise the half-metallicity and electronic correlations. We determined the three-dimensional Fermi surface and the spin-dependent band structure. As a result, we found that a part of the minority spin bands is on the occupied side in the vicinity of the Fermi level, providing spectroscopic evidence that CoS$_2$ is not but very close to a half-metal. Band calculations using density functional theory with generalized gradient approximation showed a good agreement with the observed majority spin $e_g$ bands, while it could not explain the observed band width of the minority-spin eg bands. On the other hand, theoretical calculations using dynamical mean field theory could better reproduce the strong mass renormalization in the minority-spin $e_g$ bands. All those results strongly suggest the presence of anomalously enhanced spin-dependent electron correlation effects on the electronic structure in the vicinity of the half-metallic state. We also report the temperature dependence of the electronic structure across the Curie temperature and discuss the mechanism of the thermal demagnetization. Our discovery of the anomalously large spin-dependent electronic correlations not only demonstrates a key factor in understanding the electronic structure of half-metals but also provides a motivation to improve theoretical calculations on spin-polarized strongly correlated systems.

cond-mat.str-el↗

arXiv2023

Laser-based angle-resolved photoemission spectroscopy with micrometer spatial resolution and detection of three-dimensional spin vector

We have developed a state-of-the-art apparatus for laser-based spin- and angle-resolved photoemission spectroscopy with micrometer spatial resolution (micro-SARPES). This equipment is achieved through the combination of a high-resolution photoelectron spectrometer, a 6-eV laser with high photon flux that is focused down to a few micrometers, a high-precision sample stage control system, and a double very-low-energy-electron-diffraction spin detector. The setup achieves an energy resolution of 1.5 (5.5) meV without (with) the spin detection mode, compatible with a spatial resolution better than 10 micrometers. This enables us to probe both spatially-resolved electronic structures and vector information of spin polarization in three dimensions. The performance of micro-SARPES apparatus is demonstrated by presenting ARPES and SARPES results from topological insulators and Au photolithography patterns on a Si (001) substrate.

cond-mat.mtrl-sci↗

arXiv2023

SPADExp: A photoemission angular distribution simulator directly linked to first-principles calculations

We develop a software package SPADExp (simulator of photoemission angular distribution for experiments) to calculate the photoemission angular distribution (PAD), which is the momentum dependence of spectrum intensity in angle-resolved photoemission spectroscopy (ARPES). The software can directly load the output of the first-principles software package OpenMX, so users do not need to construct tight-binding models as previous studies did for PAD calculations. As a result, we can calculate the PADs of large systems such as quasicrystals and slab systems. We calculate the PADs of sublattice systems (graphene and graphite) to reproduce characteristic intensity distributions, which ARPES has experimentally observed. After that, we investigate twisted bilayer graphene, a quasicrystal showing 12-fold rotational symmetric spectra in ARPES, and the surface states of the topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$. Our calculations show good agreement with previous ARPES measurements, showing the correctness of our calculation software and further potential to investigate the photoemission spectra of novel quantum materials.

cond-mat.mtrl-sci↗

arXiv2023

Semiconducting Electronic Structure of the Ferromagnetic Spinel $\mathbf{Hg}\mathbf{Cr}_2\mathbf{Se}_4$ Revealed by Soft-X-Ray Angle-Resolved Photoemission Spectroscopy

We study the electronic structure of the ferromagnetic spinel $\mathrm{Hg}\mathrm{Cr}_2\mathrm{Se}_4$ by soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) and first-principles calculations. While a theoretical study has predicted that this material is a magnetic Weyl semimetal, SX-ARPES measurements give direct evidence for a semiconducting state in the ferromagnetic phase. Band calculations based on the density functional theory with hybrid functionals reproduce the experimentally determined band gap value, and the calculated band dispersion matches well with ARPES experiments. We conclude that the theoretical prediction of a Weyl semimetal state in $\mathrm{Hg}\mathrm{Cr}_2\mathrm{Se}_4$ underestimates the band gap, and this material is a ferromagnetic semiconductor.

cond-mat.mtrl-sci↗

arXiv2023

Time-, spin-, and angle-resolved photoemission spectroscopy with a 1-MHz 10.7-eV pulse laser

We describe a setup of time-, spin-, and angle-resolved photoemission spectroscopy (tr-SARPES) employing a 10.7-eV ($λ$=115.6 nm) pulse laser at 1-MHz repetition rate as a probe photon source. This equipment effectively combines technologies of a high-power Yb:fiber laser, ultraviolet-driven harmonic generation in Xe gas, and a SARPES apparatus equipped with very-low-energy-electron-diffraction (VLEED) spin detectors. A high repetition rate (1 MHz) of the probe laser allows experiments with the photoemission space-charge effects significantly reduced, despite a high flux of 10$^{13}$ photons/s on the sample. The relatively high photon energy (10.7 eV) also brings the capability of observing a wide momentum range that covers the entire Brillouin zone of many materials while ensuring high momentum resolution. The experimental setup overcomes a low efficiency of spin-resolved measurements, which gets even more severe for the pump-probed unoccupied states, and affords for investigating ultrafast electron and spin dynamics of modern quantum materials with energy and time resolutions of 25 meV and 360 fs, respectively.

cond-mat.mtrl-sci↗

arXiv2023

Spin-polarized saddle points in the topological surface states of the elemental Bismuth revealed by a pump-probe spin-resolved ARPES

We use a pump-probe, spin-, and angle-resolved photoemission spectroscopy (ARPES) with a 10.7 eV laser accessible up to the Brillouin zone edge, and reveal for the first time the entire band structure, including the unoccupied side, for the elemental bismuth (Bi) with the spin-polarized surface states. Our data identify Bi as in a strong topological insulator phase ($Z_2$=1) against the prediction of most band calculations. We unveil that the unoccupied topological surface states possess spin-polarized saddle points yielding the van Hove singularity, providing an excellent platform for the future development of opto-spintronics.

cond-mat.mtrl-sci↗

arXiv2023

A robust weak topological insulator in a bismuth halide Bi4Br2I2

We apply a topological material design concept for selecting a bulk topology of 3D crystals by different van-der-Waals stacking of 2D topological insulator layers, and find a bismuth halide Bi4Br2I2 to be an ideal weak topological insulator (WTI) with the largest band gap (~230 meV) among all the WTI candidates, by means of angle-resolved photoemission spectroscopy (ARPES), density functional theory (DFT) calculations, and resistivity measurements. Our results vastly expand future opportunities for fundamental research and device applications with a robust WTI.

cond-mat.mtrl-sci↗