arXiv subjects

Hiroki Wadati

Publications and source records attributed to Hiroki Wadati.

At least 19 recordsLinked to original sources

arXiv2026

XUV Transmission Spectroscopy Using a Tabletop High-Harmonic Source

High-harmonic generation (HHG) provides a coherent ultrashort-pulse light source in the extreme- ultraviolet (XUV) region and has potential applications in time-resolved spectroscopy and materials characterization. In this study, we constructed an HHG system using a Yb:KGW laser system (PHAROS, Light Conversion) as the driving source and Ar gas as the nonlinear medium. High-order harmonics were observed up to a photon energy of 70.6 eV, corresponding to the 59th harmonic order. As an application of the developed XUV source, we measured the transmission of a Mg thin film and a Si3N4 membrane. In addition, the surface chemical state of the Mg thin film was characterized by X-ray photoelectron spectroscopy (XPS), and the results were compared with the transmission measured using the HHG source. This comparison was used to examine the relationship between the surface condition, including surface oxidation, and the XUV transmission of the Mg thin film. These results demonstrate the applicability of the developed Ar-based HHG source to the characterization of thin-film transmission in the XUV spectral region.

cond-mat.mtrl-sci↗

arXiv2026

Bayesian model comparison of type-I and type-II ultrafast demagnetization dynamics

Ultrafast demagnetization dynamics are often phenomenologically classified into type-I and type-II responses according to their temporal evolution following femtosecond laser excitation. However, finite experimental temporal resolution and noise can substantially obscure the intrinsic dynamics and complicate this classification. In this work, we investigate the distinguishability of type-I and type-II demagnetization dynamics using Gaussian-convolved phenomenological models and Bayesian information criterion-based statistical model comparison. Synthetic datasets with varying temporal resolution and noise levels are first analyzed to evaluate the conditions under which the two classes can be reliably discriminated. We show that convolution with the instrumental response function significantly reduces the observable differences between the intrinsic responses, thereby producing broad regimes in which model discrimination becomes statistically inconclusive. The applicability of the framework is further demonstrated through analysis of representative experimental ultrafast demagnetization data from NiCo2O4 thin films. These results suggest that the apparent classification of ultrafast demagnetization dynamics can be highly sensitive to experimental resolution, noise level, and analysis methodology.

cond-mat.mtrl-sci↗

arXiv2026

Re-examination of electronic structure of dilute Kondo transition-metal ions substituted into a Heavy Fermion compound

Correlations between the localized and conductive spins/charges have been the central issue of various fascinating quantum phenomena found on itinerant electron systems. Here, the obvious multiplet structures are presented on the Mn 2$p$ to 3$d$ x-ray absorption for a heavy fermion $α$-(Yb,Lu)(Al$_{1-x}$Mn$_x$)B$_4$, indicating that the unoccupied electronic structure of the Mn site is described as the correlated high-spin 2+, even though magnetic measurements show the Mn sites to be nonmagnetic. This apparently paradoxical result demonstrates that a ligand field can effectively appear between localized Mn 3$d$ and surrounding B 2$p$ orbitals, which has been anticipated as a manifestation of a Kondo effect but not been clearly confirmed for most itinerant metals in spectroscopy. By contrast, the Mn 2$p$ photoemission indicates that the occupied Mn$^{2+}$ 3$d$ electrons still exhibit itinerant and nonlocally screened nature also owing to the Kondo-like correlation with the conductive B 2$p$, and heavier Yb 4$f$ and 5$d$ bands below the Fermi energy. The asymmetry on the particle-hole stimulates a reconsideration of the correlation and screening effects in the core-level spectroscopies.

cond-mat.str-el↗

arXiv2026

Type-II-like ultrafast demagnetization behavior in NiCo2O4 thin films

Rare-earth-ferrimagnetic oxides are emerging as attractive platforms for investigating ultrafast spin dynamics. Here, we study the photoinduced magnetization dynamics of epitaxial NiCo2O4 (NCO) thin films by time-resolved magneto-optical Faraday effect using two independent pump-probe configurations: 1030/515 nm and 800/400 nm. In both measurements, photoexcitation induces an immediate reduction of the magneto-optical signal within the experimental time resolution, followed by a reproducible slower demagnetization component with a characteristic timescale of approximately 5-6 ps and a subsequent recovery on the ~100 ps timescale. Importantly, this picosecond demagnetization component is observed consistently across the two experimental configurations and excitation wavelengths, demonstrating that it is an intrinsic feature of the ultrafast magnetic response of NCO thin films. Because the earliest-time dip may contain a transient optical contribution, we describe the overall response as type-II-like, rather than assigning a definitive textbook type-II classification solely on the basis of the sub-resolution signal. These results establish a robust two-step ultrafast demagnetization behavior in NCO and highlight rare-earth-free oxide ferrimagnets as promising systems for exploring Mult sublattice spin dynamics on ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2026

Teaching light absorption and the Beer-Lambert law using everyday materials: a tomato juice experiment for introductory physics

I describe a visually engaging experiment to demonstrate the Beer-Lambert law in introductory physics or general science courses. By using diluted tomato juice as a naturally colored absorber and a halogen lamp as a broadband light source, students can explore how light attenuation depends on concentration and wavelength. The activity connects the optical concept of exponential absorption with everyday materials, making it accessible for classrooms with limited resources. Transmission spectra obtained with a compact spectrometer reveal a strong absorption band around 500 nm, corresponding to the green-blue region absorbed by lycopene. Plotting absorbance against concentration allows students to confirm linear behavior at low concentrations and to discuss deviations at higher ones. The experiment emphasizes conceptual understanding of light-matter interaction, quantitative data analysis, and the limitations of ideal laws, providing a memorable learning experience in optics and spectroscopy.

physics.ed-ph↗

arXiv2026

Recent Progress in Ultrafast Dynamics of Transition-Metal Compounds Studied by Time-Resolved X-ray Techniques

X-ray absorption spectroscopy and X-ray magnetic circular dichroism have long served as indispensable tools for probing the electronic and magnetic properties of transition-metal compounds with elemental selectivity. In recent years, the emergence of femtosecond lasers has opened a new avenue for studying nonequilibrium dynamics in condensed matter. However, conventional optical techniques lack elemental and orbital specificity, making it difficult to disentangle the coupled charge, spin, and lattice responses in complex materials. The development of X-ray free-electron lasers (XFEL) and laboratory high-harmonic generation (HHG) sources has enabled the extension of X-ray absorption and scattering techniques into the femtosecond time domain. Time-resolved X-ray absorption spectroscopy, X-ray magnetic circular dichroism, and resonant soft X-ray scattering now provide direct, complementary access to element- and momentum-resolved ultrafast dynamics. This review summarizes recent progress in these techniques, focusing on pump-probe measurements of laser-induced demagnetization, spin-state transitions, and valence and structural changes in transition-metal compounds. We also discuss advances in tabletop HHG-based X-ray spectroscopy and its integration with large-scale XFEL facilities. These developments provide powerful routes for visualizing the nonequilibrium evolution of charge, spin, orbital, and lattice degrees of freedom, offering new insights into the ultrafast control of quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Raman Spectroscopic Investigation of Ferroaxial Order in Na2BaNi(PO4)2 Single Crystals

Ferroaxial order is characterized by the breaking of mirror symmetry parallel to the crystallographic principal axis, which often originates from spontaneous rotational distortions of the crystal lattice. Such rotational distortions are, by symmetry, allowed to couple to specific phonon modes. However, Raman-active phonons associated with these rotational distortions have not yet been clearly identified on a symmetry-consistent basis. Here, we perform polarization-resolved Raman spectroscopy on the ferroaxial phase of Na2BaNi(PO4)2 single crystals and combine the measurements with first-principles lattice-dynamics calculations. This symmetry-guided analysis enables a comprehensive assignment of Raman-active modes in the ferroaxial phase. Several low-frequency Ag modes exhibit finite linewidth broadening, suggesting that these phonons may be weakly affected by the underlying rotational distortion. These results establish a symmetry-based spectroscopic framework for analyzing phonons associated with rotational distortions in ferroaxial materials and provide a basis for future studies of ferroaxial order in complex oxides.

cond-mat.mtrl-sci↗

arXiv2025

Development of a Ferromagnetic Resonance Measurement System Using NanoVNA

Ferromagnetic resonance (FMR) is a fundamental technique for probing magnetization dynamics in spintronic and magnetic materials. However, conventional FMR measurements rely on broadband vector network analyzers (VNAs), whose high cost limits accessibility for small laboratories and educational environments. To overcome this barrier, we have developed a compact and low-cost FMR measurement platform - the NanoVNA-FMR system-based on a commercially available NanoVNA. The setup integrates an electromagnet and a coplanar waveguide (CPW) and is fully automated using Python scripts. This enables synchronized magnetic-field sweeping, S-parameter acquisition, and real-time visualization. The system successfully captures clear FMR spectra that exhibit systematic shifts in resonance frequency with increasing magnetic field. The results are in excellent agreement with those obtained using a conventional VNA-based FMR system, confirming the quantitative reliability of the NanoVNA approach. Additionally, a 3D-printed sample holder further reduces overall system cost. These results demonstrate that the NanoVNA-FMR system provides a practical, accurate, and accessible alternative for quantitative magnetic characterization and educational applications.

cond-mat.mtrl-sci↗

arXiv2025

Fe contribution to the magnetic anisotropy of $L{1_0}$-ordered FePt thin films studied by angle-dependent x-ray magnetic circular dichroism

Among magnetic thin films with perpendicular magnetic anisotropy (PMA), $L1_0$-ordered FePt has attracted significant attention because of its exceptionally strong PMA. However, the microscopic origin of its strong PMA has not been elucidated experimentally. We have investigated the contribution of the Fe $3d$ electrons to its magnetic anisotropy energy by angle-dependent x-ray magnetic circular dichroism at the Fe $L_{2,3}$ edge. By this technique, one can deduce the magnetic dipole moment $m_\text{T}$, which represents the anisotropic spatial distribution of spin-polarized electrons, and the orbital moment anisotropy (OMA) of Fe $3d$ electrons. Detected finite $m_\text{T}$ indicates that the spin-polarized Fe $3d$ electrons are distributed preferentially in the out-of-plane direction of the films. This $m_\text{T}$ of Fe overwhelms the positive contribution of OMA to PMA, and reduces the PMA of $L1_0$-ordered FePt thin films, consistent with a previous first-principles calculation. The present result implies that a large positive contribution of the non-magnetic element Pt rather than Fe governs the PMA of $L1_0$-ordered FePt thin films.

cond-mat.mtrl-sci↗

arXiv2025

Synthesis, crystal and electronic structures, and second harmonic generation of La 4Ge 3S12

The crystal structure of La 4 Ge 3S 12 has been known to be noncentrosymmetric for almost four decades. This characteristic inversion symmetry breaking suggests the presence of nonlinear optical properties. Yet only recently have nonlinear optical phenomena such as second harmonic generation (SHG) been reported in this material. In this study, we synthesized La4Ge3S12 using the direct reaction method and characterized the composition, crystal structure, and electronic structure using electron probe microanalysis, powder and single-crystal X-ray diffraction, and X-ray photoelectron spectroscopy. The experimentally measured electronic structure is in line with that obtained using first-principles calculations. In addition, we observed the nonlinear optical properties of La4Ge3S12 in response to an ultrashort infrared pulsed laser. We found that the intensity of the SHG depends quadratically on the intensity of the incident light, mirroring the intrinsic nature of nonlinear optics.

cond-mat.mtrl-sci↗

arXiv2025

All-optical helicity-dependent switching in NiCo$_2$O$_4$ thin films

All-optical switching (AOS) involves manipulating magnetization using only pulsed laser, presenting a promising approach for next-generation magnetic recording devices. NiCo2O4 (NCO) thin films, a rare-earth-free ferrimagnetic oxide, exhibit a high Curie temperature and strong perpendicular magnetic anisotropy. This study demonstrates AOS in NCO thin films at room temperature using long-duration laser pulses and high repetition rates. Unlike previous findings, the AOS phenomena we report here are helicity-dependent and observable with an ultrashort pulsed laser. Consequently, two distinct types of AOS can be observed in a single NCO thin film, contingent on the characteristics of the laser pulses and temperature.

cond-mat.mtrl-sci↗

arXiv2024

Photo-induced phase transition on black samarium monosulfide

To investigate the role of the excitons for the origin of the pressure-induced phase transition (BGT) from the black-colored insulator (BI) to the golden-yellow-colored metal (GM) of samarium monosulfide (SmS), optical reflectivity, Sm $3d$ X-ray absorption spectroscopy (XAS), and X-ray diffraction (XRD) with the creation of excitons by photoexcitation (PE) are reported. In the pump-probe reflectivity measurement, following a huge reflectivity change of about 22 %, three different relaxation times with a vibration component were observed. The fast component with the relaxation time ($τ$) of less than 1 ps is due to the excitation and relaxation of electrons into the conduction band, and the slowest one with $τ> {\rm several} 100$ ps originates from the appearance of the photo-induced (PI) state. The components with $τ\sim 10$ ps and vibration originate from the appearance of the PI state and the interference between the reflection lights at the sample surface and the boundary between the BI and PI states, suggesting that the electronic structure of the PI phase is different from that of the BI state. XAS spectra indicate that the Sm mean valence is shifted from the Sm$^{2+}$ dominant to the intermediate between Sm$^{2+}$ and Sm$^{3+}$ by PE but did not change to that of the GM phase across BGT, consistent with the reflectivity data. The XRD result after PE shows that the PI state has much less lattice contraction than the GM phase. These results suggest that the BGT cannot be achieved solely by creating excitons after PE but requires other effects, such as a lattice contraction.

cond-mat.str-el↗

arXiv2023

4$f$ electron temperature driven ultrafast electron localization

Valence transitions in strongly correlated electron systems are caused by orbital hybridization and Coulomb interactions between localized and delocalized electrons. The transition can be triggered by changes in the electronic structure and is sensitive to temperature variations, applications of magnetic fields, and physical or chemical pressure. Launching the transition by photoelectric fields can directly excite the electronic states and thus provides an ideal platform to study the correlation among electrons on ultrafast timescales. The EuNi$_2$(Si$_{0.21}$Ge$_{0.79}$)$_2$ mixed-valence metal is an ideal material to investigate the valence transition of the Eu ions via the amplified orbital hybridization by the photoelectric field on sub-picosecond timescales. A direct view on the 4$f$ electron occupancy of the Eu ions is required to understand the microscopic origin of the transition. Here we probe the 4$f$ electron states of EuNi$_2$(Si$_{0.21}$Ge$_{0.79}$)$_2$ at the sub-ps timescale after photoexcitation by X-ray absorption spectroscopy across the Eu $M_5$-absorption edge. The observed spectral changes due to the excitation indicate a population change of total angular momentum multiplet states $J$ = 0, 1, 2, and 3 of Eu$^{3+}$, and the Eu$^{2+}$ $J$ = 7/2 multiplet state caused by an increase in 4$f$ electron temperature that results in a 4$f$ localization process. This electronic temperature increase combined with fluence-dependent screening accounts for the strongly non-linear effective valence change. The data allow us to extract a time-dependent determination of an effective temperature of the 4$f$ shell, which is also of great relevance in the understanding of metallic systems' properties, such as the ultrafast demagnetization of ferromagnetic rare-earth intermetallics and their all-optical magnetization switching.

cond-mat.str-el↗

arXiv2023

Photocarrier Transport of Ferroelectric Photovoltaic Thin Films Detected by the Magnetic Dynamics of Adjacent Ferromagnetic Layers

We have observed photocarrier transport behaviors in BiFeO$_3$/La$_{1-x}$Sr$_x$MnO$_3$~(BFO/LSMO) heterostructures by using time-resolved synchrotron x-ray magnetic circular dichroism in reflectivity. The magnetization of LSMO layers was used as a probe of photo-induced carrier dynamics in the photovoltaic BFO layers. During the photo-induced demagnetization process, the decay time of LSMO~($x$=0.2) magnetization strongly depends on the ferroelectric polarization direction of the BFO layer. The variation of decay time should be attributed to the different sign of accumulated photocarriers at the BFO/LSMO interface induced by the photovoltaic effect of the BFO layer. The photocarriers can reach the BFO/LSMO interface and influence the magnetization distribution in the LSMO layers within the timescale of $\sim$100~ps. Our results provide a novel strategy to investigate carrier dynamics and mechanisms of optical control of magnetization in thin film heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Spin-charge coupling and decoupling in perovskite-type iron oxides (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$

The perovskite-type iron oxide Sr$_{2/3}$La$_{1/3}$FeO$_3$ is known to show characteristic spin-charge ordering (SCO), where sixfold collinear spin ordering and threefold charge ordering are coupled with each other. Here, we report the discovery of a spin-charge decoupling and an antiferromagnetic (AFM) state competing with the SCO phase in perovskites (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$. By comprehensive measurements including neutron diffraction, M$ö$ssbauer spectroscopy, and x-ray absorption spectroscopy, we found that the isovalent Ba$^{2+}$ substitution systematically reduces the critical temperature of the SCO phase and additionally yields the spin-charge decoupling in $x$ > 0.75. Whereas the ground state remains in the SCO phase in the whole $x$ region, an unexpected G-type AFM phase with incoherent charge ordering or charge fluctuation appears as the high-temperature phase in the range of $x$ > 0.75. Reflecting the competing nature between them, the G-type AFM phase partially exists as a metastable state in the SCO phase at low temperatures. We discuss the origin of the spin-charge decoupling and the emergence of the G-type AFM phase with charge fluctuation in terms of the bandwidth reduction by the Ba substitution.

cond-mat.str-el↗

arXiv2022

Optically-induced magnetization switching in NiCo2O4 thin films using ultrafast lasers

Recently, all-optical magnetization control has been garnering considerable attention in realizing next-generation ultrafast magnetic information devices. Here, employing a magneto-optical Kerr effect (MOKE) microscope, we observed the laser-induced magnetization switching of ferrimagnetic oxide NiCo2O4 (NCO) epitaxial thin films with perpendicular magnetic anisotropy, where the sample was pumped at 1030-nm laser pulses, and magnetic domain images were acquired via the MOKE microscope with a white light emitting diode. Laser pulses irradiated an NCO thin film at various temperatures from 300 K to 400 K while altering the parameters of pulse interval, fluence, and the number of pulses with the absence of the external magnetic field. We observed accumulative all-optical switching at 380 K and above. Our observation of oxide NCO thin films facilitates the realization of chemically stable magnetization switching using ultrafast lasers, and without applying a magnetic field.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast demagnetization in NiCo2O4 thin films probed by time-resolved microscopy

Using a time-resolved magneto-optical Kerr effect (TR-MOKE) microscope, we observed ultrafast demagnetization of inverse-spinel-type NiCo2O4 (NCO) epitaxial thin films of the inverse spinel type ferrimagnet NCO with perpendicular magnetic anisotropy. This microscope uses a pump-probe method, where the sample is pumped at 1030 nm, and magnetic domain images are acquired via MOKE microscopy at 515 nm (the second harmonic). We successfully observed the dynamics of the magnetic domain of the NCO thin film via laser irradiation, and obtained a demagnetization time constant of approximately 0.4 ps. This time constant was significantly smaller than the large time constants reported for other half-metallic oxides. These results, combined with the results of our x-ray photoemission spectroscopy study, indicate that this NCO thin film is a ferrimagnetic metal whose electronic structure deviates from the theoretically predicted half-metallic one.

cond-mat.mtrl-sci↗

arXiv2021

Photo-induced Antiferromagnetic-ferromagnetic Transition and Electronic Structure Modulation in GdBaCo$_2$O$_{5.5}$ Thin Film

We investigate both the ferromagnetic (FM) and antiferromagnetic (AFM) ultrafast dynamics of a strongly correlated oxide system, GdBaCo$_2$O$_{5.5}$ 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 beyond the unpumped value and a decay of RMXD was observed. The photon-energy dependence of the transient XMCDR and reflectivity can likely be interpreted as a concomitant photo-induced spinstate transition.

cond-mat.str-el↗