Since the first isolated attosecond pulse was demonstrated through high-order harmonics generation (HHG) in 2001, researchers’ interest in the ultrashort time region has expanded. However, one realizes a limitation for related research such as attosecond spectroscopy. The bottleneck is concluded to be the lack of a high-peak-power isolated attosecond pulse source. Therefore, currently, generating an intense attosecond pulse would be one of the highest priority goals. In this paper, we review our recent work of a TW-class parallel three-channel waveform synthesizer for generating a gigawatt-scale soft-X-ray isolated attosecond pulse (IAP) using HHG. By employing several stabilization methods, we have achieved a stable 50 mJ three-channel optical-waveform synthesizer with a peak power at the multi-TW level. This optical-waveform synthesizer is capable of creating a stable intense optical field for generating an intense continuum harmonic beam thanks to the successful stabilization of all the parameters. Furthermore, the precision control of shot-to-shot reproducible synthesized waveforms is achieved. Through the HHG process employing a loose-focusing geometry, an intense shot-to-shot stable supercontinuum (50–70 eV) is generated in an argon gas cell. This continuum spectrum supports an IAP with a transform-limited duration of 170 as and a submicrojoule pulse energy, which allows the generation of a GW-scale IAP. Another supercontinuum in the soft-X-ray region with higher photon energy of approximately 100–130 eV is also generated in neon gas from the synthesizer. The transform-limited pulse duration is 106 as. Thus, the enhancement of HHG output through optimized waveform synthesis is experimentally proved.

Terahertz- (THz-) based electron manipulation has recently been shown to hold tremendous promise as a technology for manipulating and driving the next generation of compact ultrafast electron sources. Here, we demonstrate an ultrafast electron diffractometer with THz-driven pulse compression. The electron bunches from a conventional DC gun are compressed by a factor of 10 and reach a duration of ~180 fs (FWHM) with 10,000 electrons/pulse at a 1 kHz repetition rate. The resulting ultrafast electron source is used in a proof-of-principle experiment to probe the photoinduced dynamics of single-crystal silicon. The THz-compressed electron beams produce high-quality diffraction patterns and enable the observation of the ultrafast structural dynamics with improved time resolution. These results validate the maturity of THz-driven ultrafast electron sources for use in precision applications.

We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides, WS2 and MoSe2, subjected to intense linearly polarized midinfrared laser fields. The measured spectra consist of both odd- and even-order harmonics, with a high-energy cutoff extending beyond the 15th order for a laser-field strength around ~1 V/nm. In WS2, we find that the polarization direction of the odd-order harmonics smoothly follows that of the laser field irrespective of the crystal orientation, whereas the direction of the even-order harmonics is fixed by the crystal mirror planes. Furthermore, the polarization of the even-order harmonics shows a flip in the course of crystal rotation when the laser field lies between two of the crystal mirror planes. By numerically solving the semiconductor Bloch equations for a gapped-graphene model, we qualitatively reproduce these experimental features and find the polarization flipping to be associated with a significant contribution from interband polarization. In contrast, high-harmonic signals from MoSe2 exhibit deviations from the laser-field following of odd-order harmonics and crystal-mirror-plane following of even-order harmonics. We attribute these differences to the competing roles of the intraband and interband contributions, including the deflection of the electron-hole trajectories by nonparabolic crystal bands.