Keisuke Kaneshima

VO ₂ is a prototypical strongly correlated material that undergoes photoinduced phase transitions on the femtosecond scale. To explore its potential for ultrafast all-optical phase modulation, we constructed a femtosecond time-resolved interferometer to directly probe the optical phase response, revealing the change in the real part of the refractive index during the phase transition. The observed optical phase dynamics exhibit faster and slower components, reflecting different stages of the phase transition process. The overall magnitude of the phase shift is largely determined by the ultrafast response, demonstrating the feasibility of femtosecond all-optical phase modulation in VO ₂ thin films.

Tapered undulators are designed to generate broadband, chirped radiation for advanced synchrotron light sources. However, the complete electric-field waveform of the radiation has never been directly measured. Here, we report the first, to the best of our knowledge, direct characterization of a chirped wavepacket generated from a tapered undulator using spectral phase interferometry for direct electric-field reconstruction (SPIDER). The retrieved spectral phase reveals a distinct linear chirp, and its magnitude shows essential agreement with theoretical predictions. This work provides the first experimental validation of the chirped waveform generated from an undulator, enabling advanced temporal control of next-generation light sources.

This study introduces a compact, portable femtosecond fibre laser system designed for synchronization with SPring-8 synchrotron X-ray pulses in a uniform filling mode. Unlike traditional titanium–sapphire mode-locked lasers, which are fixed installations, our system utilizes fibre laser technology to provide a practical alternative for time-resolved spectroscopy, striking a balance between usability, portability and cost-efficiency. Comprehensive evaluations, including pulse characterization, timing jitter and frequency stability tests revealed a centre wavelength of 1600 nm, a pulse energy of 4.5 nJ, a pulse duration of 35 fs with a timing jitter of less than 9 ps, confirming the suitability of the system for time-resolved spectroscopic studies. This development enhances the feasibility of experiments that combine synchrotron X-rays and laser pulses, offering significant scientific contributions by enabling more flexible and diverse research applications.

Abstract Observing ultrafast pulse-to-pulse dynamics of highly photoexcited materials could foster a comprehensive understanding of the initial stage of irreversible photoinduced events, such as phase change, structural deformation, and laser ablation. In this study, using high-repetition-rate single-shot spectroscopy and a laser microscope, the pulse-to-pulse ultrafast dynamics of energy relaxation in Ge₂Sb₂Te₅ thin films are revealed under high-density photoexcitation that induces sequential events involving the crystalline-to-amorphous phase transition, melt and quench processes, and formation of laser-induced periodic surface structures (LIPSSs). Above the threshold excitation density for LIPSS formation, the first excitation pulse induces the transient transmittance change of the crystalline phase in a picosecond timescale, and subsequent pulses provoke the amorphous phase energy relaxation with a long decay time of hundreds of picoseconds. We observed that the subsequent pulses gradually reduce the amplitude and decay time of the transient transmittance, leading to efficient energy relaxation and LIPSS formation in the photoinduced amorphous phase.

Objective lenses are frequently employed in state-of-the-art ultrafast time-resolved microscopy techniques. While it enables tight spatial focusing, its dispersion causes a longer optical pulse duration. Since an objective lens is a combination of different lens materials, finding its correct dispersion can be challenging. In this paper, we propose a dispersion measurement method for an objective lens using white light interferometry. Our proposed method enables the experimental determination of the lens dispersion and improves the temporal resolution of ultrafast time-resolved microscopy techniques.

The formation of nitrous acid (HONO) through photolysis of o-nitrophenol was captured in real time by time-resolved photoelectron spectroscopy using single-order high harmonic probe pulses. HONO is released 250 fs after photoexcitation.

We report, to the best of our knowledge, the first time-resolved high-harmonic spectroscopy (TR-HHS) study of a chemical bond rearrangement. We investigate the transient change of the high-harmonic signal from 1,3-cyclohexadiene (CHD), which undergoes ring-opening and isomerizes to 1,3,5-hexatriene (HT) upon photoexcitation. By associating the variation in the harmonic yield to the changes in the electronic state and vibrational frequencies of the molecule due to isomerization, we find that the CHD excited via two-photon absorption of 3.1 eV photons isomerizes to HT, i.e., ring-opening occurs, around 400 fs after the excitation. The present results demonstrate that TR-HHS, which can track both electronic and nuclear dynamics, is a powerful tool for studying ultrafast photochemical reactions.

<p>Recent progress of optical parametric amplification has realized the generation of intense ultrashort pulses in the mid-infrared (MIR) range. Tight focusing of micro-joule-class MIR pulses can produce strong electric fields exceeding 100 MV/cm. The photon energies in the MIR range are far less than the bandgap energies of typical solids, avoiding the optical damage initiated by multiphoton ionization. Using such advantages, strong-field and attosecond physics can be extended from the gas phase to solids, which is a promising sub-field of extreme nonlinear optics. In this report, we will show a novel method to produce intense MIR pulses with a stable carrier-envelope phase, electro-optical sampling of MIR fields with visible 6.5-fs pulses, and their application to high harmonic generation in crystalline solids and photoemission from nanotips.</p>