arXiv subjects

Yuichi Inubushi

Publications and source records attributed to Yuichi Inubushi.

At least 19 recordsLinked to original sources

arXiv2026

X-ray Coherent Attosecond Pulse Pair Spectroscopy

X-ray free electron laser (XFEL) experiments using self-amplified spontaneous emission (SASE) pulses typically achieve temporal resolutions of order several femtoseconds, as the pulse duration puts a practical limit to pump-probe or probe-probe schemes. Even with the emerging capabilities to generate pulses with attosecond durations with new single-spike SASE schemes, direct access to attosecond electron dynamics remains an experimental challenge. Here we show how X-ray coherent attosecond pulse-pair spectroscopy (X-CAPPS) provides a powerful new approach to access the ultrashort time-delay window. Coherent attosecond pulse pairs with time delays varying from ~500 as to ~5 fs are generated with Cu K$\alpha_1$ stimulated X-ray emission from a gain medium pumped by intense SASE XFEL pulses. These pulse pairs are analyzed with two subsequent Bragg crystal spectrometers, and the resulting interference spectrum is captured on two sequential 2D image detectors encoding their time separation, relative amplitudes, and phases with high precision. X-CAPPS requires no split-and-delay X-ray optics, nor XFEL pulse modifications, making it broadly implementable across existing facilities. This technique enables the investigation of attosecond processes with $\mathring{A}$ngstr\"{o}m resolution, providing a new tool for probing ultrafast dynamics across a wide range of atomic, molecular, and solid systems.

physics.optics↗

arXiv2025

Phase transitions of eutectic high entropy alloy AlCoCrFeNi2.1 under shock compression

High entropy alloys (HEAs) are a new class of metals that exhibit unique mechanical performance. Among HEAs, additively manufactured eutectic high entropy alloys (AM-EHEAs) have recently emerged as candidate materials for use in extreme conditions due to their simultaneous high strength and ductility. However, the deformation and structural evolution of AM-EHEAs under conditions of high pressure have not been well characterized, limiting their use in extreme applications. We present dynamic compression experiments and molecular dynamics simulations studying the structural evolution of AM-EHEA AlCoCrFeNi2.1 when compressed to pressures up to 400 GPa. Our in-situ X-ray diffraction measurements capture the appearance of fcc and bcc phases at different pressure conditions, with pure- and mixed-phase regions. Understanding the phase stability and structural evolution of the AM EHEA offers new insights to guide the development of high-performance complex materials for extreme conditions.

cond-mat.mtrl-sci↗

arXiv2025

Enhanced plasma heating via interaction with high-contrast laser and cone-shaped target

We investigated plasma heating enhancement using a high-intensity, high-contrast laser and a cone-attached target. Fast electron spectra and X-ray emission were measured with an electron spectrometer and a Bragg crystal spectrometer. The results were analyzed using PrismSPECT simulations with a two-component electron distribution model and empirical scaling laws. X-ray pinhole images showed that the cone effectively focused multi-spot laser light near its tip, enhancing local emission. While high-contrast laser irradiation reduced the fast electron slope temperature for flat targets, the use of a cone increased it by over threefold, corresponding to a fourfold rise in laser intensity. X-ray spectral analysis indicated an electron temperature of ~9~keV for the cone case, 17.5 times higher than that with a low-contrast laser. These findings demonstrate that combining high-contrast laser irradiation with cone-target geometry significantly improves laser energy coupling and plasma heating efficiency.

physics.plasm-ph↗

arXiv2025

X-ray free-electron laser observation of giant and anisotropic magnetostriction in $\beta$-O$_{2}$ at 110 Tesla

In strong magnetic fields beyond 100 T, the significant Zeeman energy competes with the lattice interactions, where a considerable magnetostriction is expected. However, the microscopic observation of the magnetostriction above 100 T has been hindered due to the short pulse duration of $\mu$-seconds and the coil's destruction. Here, we report the observation of the giant and anisotropic magnetostriction of $\sim 1$ % at 110 T in the spin-controlled crystal, $\beta$-O$_{2}$, by combining the single-shot diffraction of x-ray free-electron laser (XFEL) and the newly developed portable 100 T generator (PINK-02). The very soft and anisotropic response of $\beta$-O$_{2}$ should originate in the competing van der Waals force and exchange interaction, and also the frustration of spin and lattice on the triangular network. The XFEL experiment above 100 T using PINK-02 enables microscopic investigations on materials' properties at high magnetic fields, providing insights into how spins contribute to the stability of crystal structures.

cond-mat.str-el↗

arXiv2025

Observation of Multiplet Lines in Seeded Stimulated Mn K{\alpha}1 X-ray Emission

We report the successful resolution of the multiplet structure of the K{\alpha}1 x-ray emission in manganese (Mn) complexes through seeded stimulated X-ray emission spectroscopy (seeded S-XES). By employing a femtosecond pump pulse above the Mn K edge to generate simultaneous 1s core-holes, and a second-color tunable seed pulse to initiate the stimulated emission process, we were able to enhance individual lines within the K{\alpha}1 emission. This approach allows to resolve the fine multiplet features that are obscured by the life-time broadening in conventional Mn K{\alpha} XES. The work builds on our previous observation that S-XES from Mn(II) and Mn(VII) complexes pumped at high intensities can exhibit stimulated emission without sacrificing the chemical sensitivity to oxidation states. This technique opens the door to controlled high-resolution electronic structure spectroscopy in transition metal complexes beyond core hole life time broadening with potential applications in catalysis, inorganic chemistry, and materials science.

physics.chem-ph↗

arXiv2024

Attosecond Inner-Shell Lasing at Angstrom Wavelengths

Since the invention of the laser nonlinear effects such as filamentation, Rabi-cycling and collective emission have been explored in the optical regime leading to a wide range of scientific and industrial applications. X-ray free electron lasers (XFELs) have led to the extension of many optical techniques to X-rays for their advantages of angstrom scale spatial resolution and elemental specificity. One such example is XFEL driven population inversion of 1s core hole states resulting in inner-shell K${\alpha}$ (2p to 1s) X-ray lasing in elements ranging from neon to copper, which has been utilized for nonlinear spectroscopy and development of next generation X-ray laser sources. Here we show that strong lasing effects, similar to those observed in the optical regime, can occur at 1.5 to 2.1 angstrom wavelengths during high intensity (> ${10^{19}}$ W/cm${^{2}}$) XFEL driven inner-shell lasing and superfluorescence of copper and manganese. Depending on the temporal substructure of the XFEL pump pulses(containing ${~10^{6}}$ - ${10^{8}}$ photons) i, the resulting inner-shell X-ray laser pulses can exhibit strong spatial inhomogeneities as well as spectral splitting, inhomogeneities and broadening. Through 3D Maxwell Bloch theory we show that the observed spatial inhomogeneities result from X-ray filamentation, and that the spectral splitting and broadening is driven by Rabi cycling with sub-femtosecond periods. Our simulations indicate that these X-ray pulses can have pulse lengths of less than 100 attoseconds and coherence properties that open the door for quantum X-ray optics applications.

physics.optics↗

arXiv2024

Comment on "Comments regarding "Transonic dislocation propagation in diamond" by Katagiri, et al. (Science 382, 69-72, 2023)" by Hawreliak, et al. (arXiv:2401.04213)

In their comment (1), Hawreliak et al. claims that our observation of stacking fault formation and transonic dislocation propagation in diamond (2) is not valid as they interpret the observed features as cracks. In this response letter, we describe our rationale for interpreting the observed features as stacking faults. We also address other points raised in their comments, including the clarifications of how the results of Makarov et al. (3) are not in conflict with our study.

cond-mat.mtrl-sci↗

arXiv2024

(Sub-)picosecond surface correlations of femtosecond laser excited Al-coated multilayers observed by grazing-incidence x-ray scattering

Femtosecond high-intensity laser pulses at intensities surpassing $10^{14} \,\text{W}/\text{cm}^2$ can generate a diverse range of functional surface nanostructures. Achieving precise control over the production of these functional structures necessitates a thorough understanding of the surface morphology dynamics with nanometer-scale spatial resolution and picosecond-scale temporal resolution. In this study, we show that individual XFEL pulses can elucidate structural changes on surfaces induced by laser-generated plasmas, employing grazing-incidence small-angle x-ray scattering (GISAXS). Using aluminum-coated multilayer samples we can differentiate between ultrafast surface morphology dynamics and subsequent subsurface density dynamics, achieving nanometer-depth sensitivity and subpicosecond temporal resolution. The observed subsurface density dynamics serve to validate advanced simulation models depicting matter under extreme conditions. Our findings promise to unveil novel avenues for laser material nanoprocessing and high-energy-density science.

physics.plasm-ph↗

arXiv2024

Sub-photon accuracy noise reduction of single shot coherent diffraction pattern with atomic model trained autoencoder

Single-shot imaging with femtosecond X-ray lasers is a powerful measurement technique that can achieve both high spatial and temporal resolution. However, its accuracy has been severely limited by the difficulty of applying conventional noise-reduction processing. This study uses deep learning to validate noise reduction techniques, with autoencoders serving as the learning model. Focusing on the diffraction patterns of nanoparticles, we simulated a large dataset treating the nanoparticles as composed of many independent atoms. Three neural network architectures are investigated: neural network, convolutional neural network and U-net, with U-net showing superior performance in noise reduction and subphoton reproduction. We also extended our models to apply to diffraction patterns of particle shapes different from those in the simulated data. We then applied the U-net model to a coherent diffractive imaging study, wherein a nanoparticle in a microfluidic device is exposed to a single X-ray free-electron laser pulse. After noise reduction, the reconstructed nanoparticle image improved significantly even though the nanoparticle shape was different from the training data, highlighting the importance of transfer learning.

physics.optics↗

arXiv2023

Transonic Dislocation Propagation in Diamond

The motion of line defects (dislocations) has been studied for over 60 years but the maximum speed at which they can move is unresolved. Recent models and atomistic simulations predict the existence of a limiting velocity of dislocation motions between the transonic and subsonic ranges at which the self-energy of dislocation diverges, though they do not deny the possibility of the transonic dislocations. We use femtosecond x-ray radiography to track ultrafast dislocation motion in shock-compressed single-crystal diamond. By visualizing stacking faults extending faster than the slowest sound wave speed of diamond, we show the evidence of partial dislocations at their leading edge moving transonically. Understanding the upper limit of dislocation mobility in crystals is essential to accurately model, predict, and control the mechanical properties of materials under extreme conditions.

cond-mat.mtrl-sci↗

arXiv2023

Interplay of thermal and non-thermal effects in x-ray-induced ultrafast melting

X-ray laser-induced structural changes in silicon undergoing femtosecond melting have been investigated by using an x-ray pump-x-ray probe technique. The experimental results for different initial sample temperatures reveal that the onset time and the speed of the atomic disordering are independent of the initial temperature, suggesting that equilibrium atomic motion in the initial state does not play a pivotal role in the x-ray-induced ultrafast melting. By comparing the observed time-dependence of the atomic disordering and the dedicated theoretical simulations, we interpret that the energy transfer from the excited electrons to ions via electron-ion coupling (thermal effect) as well as a strong modification of the interatomic potential due to electron excitations (non-thermal effect) trigger the ultrafast atomic disordering. Our finding of the interplay of thermal and non-thermal effects in the x-ray-induced melting demonstrates that accurate modeling of intense x-ray interactions with matter is essential to ensure a correct interpretation of experiments using intense x-ray laser pulses.

physics.app-ph↗

arXiv2023

Femtosecond reduction of atomic scattering factors triggered by intense x-ray pulse

X-ray diffraction of silicon irradiated with tightly focused femtosecond x-ray pulses (photon energy: 11.5 keV, pulse duration: 6 fs) was measured at various x-ray intensities up to $4.6\times10^{19}$ W/cm$^2$. The measurement reveals that the diffraction intensity is highly suppressed when the x-ray intensity reaches of the order of $10^{19}$ W/cm$^2$. With a dedicated simulation, we confirm the observed reduction of the diffraction intensity is attributed to the femtosecond change in individual atomic scattering factors due to the ultrafast creation of highly ionized atoms through photoionization, Auger decay, and subsequent collisional ionization. We anticipate that this ultrafast reduction of atomic scattering factor will be a basis for new x-ray nonlinear techniques, such as pulse shortening and contrast variation x-ray scattering.

physics.atom-ph↗

arXiv2022

Pushing the limits of flow strength in diamond

Extreme pressures and temperatures create conditions that allow even hard and brittle materials to deform plastically. Despite extensive research, the upper limits of flow strength, the resistance to plastic flow, remain uncertain, and the mechanisms driving deformation at the relevant stresses are a subject of debate. Using femtosecond in situ X-ray diffraction experiments and large-scale molecular dynamics simulations, we demonstrate that stacking fault-mediated strengthening enables shock-compressed nano-polycrystalline diamond to achieve a peak flow strength of 107+-5 GPa at a stress of 227+-8 GPa. Our findings show that extreme conditions can unlock unusual strength via mechanisms that can be used as design tools in targeted applications.

cond-mat.mtrl-sci↗

arXiv2022

Delayed onset and directionality of x-ray-induced atomic displacements observed on subatomic length scales

Transient structural changes of Al$_2$O$_3$ on subatomic length scales following irradiation with an intense x-ray laser pulse (photon energy: 8.70 keV; pulse duration: 6 fs; fluence: 8$\times$10$^2$ J/cm$^{2}$) have been investigated by using an x-ray pump x-ray probe technique. The measurement reveals that aluminum and oxygen atoms remain in their original positions by $\sim$20 fs after the intensity maximum of the pump pulse, followed by directional atomic displacements at the fixed unit cell parameters. By comparing the experimental results and theoretical simulations, we interpret that electron excitation and relaxation triggered by the pump pulse modifies the potential energy surface and drives the directional atomic displacements. Our results indicate that high-resolution x-ray structural analysis with the accuracy of 0.01 Åis feasible even with intense x-ray pulses by making the pulse duration shorter than the timescale needed to complete electron excitation and relaxation processes, which usually take up to a few tens of femtoseconds.

physics.optics↗

arXiv2021

Generation of Intense Phase-Stable Femtosecond Hard X-ray Pulse Pairs

Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length and time scale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more thank 3 x 10e7 photons at 5.9 keV (2.1 Angstrom) with about 1 fs duration and 2-5 fs separation. The highly directional pulse pairs are manifested by interference fringes in the superfluorescent and seeded stimulated manganese K-alpha emission induced by an X-ray free-electron laser. The fringes constitute the time-frequency X-ray analogue of the Young double-slit interference allowing for frequency-domain X-ray measurements with attosecond time resolution.

physics.atom-ph↗

arXiv2021

Nanoscale subsurface dynamics of solids upon high-intensity laser irradiation observed by femtosecond grazing-incidence x-ray scattering

Observing ultrafast laser-induced structural changes in nanoscale systems is essential for understanding the dynamics of intense light-matter interactions. For laser intensities on the order of $10^{14} \, \rm W/cm^2$, highly-collisional plasmas are generated at and below the surface. Subsequent transport processes such as heat conduction, electron-ion thermalization, surface ablation and resolidification occur at picosecond and nanosecond time scales. Imaging methods, e.g. using x-ray free-electron lasers (XFEL), were hitherto unable to measure the depth-resolved subsurface dynamics of laser-solid interactions with appropriate temporal and spatial resolution. Here we demonstrate picosecond grazing-incidence small-angle x-ray scattering (GISAXS) from laser-produced plasmas using XFEL pulses. Using multi-layer (ML) samples, both the surface ablation and subsurface density dynamics are measured with nanometer depth resolution. Our experimental data challenges the state-of-the-art modeling of matter under extreme conditions and opens new perspectives for laser material processing and high-energy-density science.

physics.plasm-ph↗

arXiv2021

Shortening X-ray Pulse Duration via Saturable Absorption

To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000 keV, duration: 6-7 fs, fluence: 2.0-3.5$\times$10$^5$ J/cm$^2$) by $\sim$35%. This finding that core-hole atoms are applicable to nonlinear x-ray optics is an essential stepping stone for extending nonlinear technologies commonplace at optical wavelengths to the hard x-ray region.

physics.optics↗

arXiv2020

Nonlinear resonant X-ray Raman scattering

We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes.

physics.atom-ph↗