High harmonic generation (HHG) using waveform-controlled, few-cycle pulses from Ti:sapphire lasers has opened emerging researches in strong-field and attosecond physics. However, the maximum photon energy of attosecond pulses via HHG remains limited to the extreme ultraviolet region. Long-wavelength light sources with carrier-envelope phase stabilization are promising to extend the photon energy of attosecond pulses into the soft X-ray region. Here we demonstrate carrier-envelope phase-dependent HHG in the water window using sub-two-cycle optical pulses at 1,600 nm. Experimental and simulated results indicate the confinement of soft X-ray emission in a single recombination event with a bandwidth of 75 eV around the carbon K edge. Control of high harmonics by the waveform of few-cycle infrared pulses is a key milestone to generate soft X-ray attosecond pulses. We measure a dependence of half-cycle bursts on the gas pressure, which indicates subcycle deformation of the waveform of the infrared drive pulses in the HHG process.

The polarization property of high harmonics from gallium selenide is investigated using linearly polarized midinfrared laser pulses. With a high electric field, the perpendicular polarization component of the odd harmonics emerges, which is not present with a low electric field and cannot be explained by the perturbative nonlinear optics. A two-dimensional single-band model is developed to show that the anisotropic curvature of an energy band of solids, which is pronounced in an outer part of the Brillouin zone, induces the generation of the perpendicular odd harmonics. This model is validated by three-dimensional quantum mechanical simulations, which reproduce the orientation dependence of the odd-order harmonics. The quantum mechanical simulations also reveal that the odd- and even-order harmonics are produced predominantly by the intraband current and interband polarization, respectively. These experimental and theoretical demonstrations clearly show a strong link between the band structure of a solid and the polarization property of the odd-order harmonics.

We report on the generation of 9.0 fs, 550 μJ, carrier-envelope phase (CEP)-stabilized optical pulses around 1.6 μm at 1 kHz. Few-cycle IR pulses are obtained from a BiB(3)O(6) optical parametric chirped-pulse amplifier. The amplification of nearly octave-spanning ultrabroad pulses without spectral broadening results in good stability in output energy (0.85% rms) and CEP (160 mrad rms). We observed high harmonics in the water window from a neon cell that corresponds to a laser intensity of 4.1×10(14) W/cm(2).

In this study, circularly polarized high harmonic generation (CP-HHG) from a chiral molecule, limonene, by a CP counter-rotating two-color laser field was found to possess circular dichroism. A high harmonic spectrum from a limonene enantiomer depends on the combination of the chirality of the enantiomer and the rotation direction of the superimposed two-color laser field in comparison with that of an achiral atom, helium. From R-enantiomer, the harmonic orders with clockwise polarization were generated more efficiently than those with counterclockwise polarization and vice versa. CP-HHG can be a sensitive probe of the chirality of biomolecules on the femtosecond and attosecond timescales.

We report 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. We associated the harmonic yield variation with the changes in the molecule's electronic state and vibrational frequencies, which are caused by isomerization. This showed us that the electronic excited state of CHD created through two-photon absorption of 3.1 eV photons relaxes almost completely within 100 fs to the electronic ground state of CHD with vibrational excitation. Subsequently, the molecule 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.

Carrier-envelope phase-stable mid-infrared pulses spanning from 5 μm to 11 μm with a pulse energy of 5 μJ were produced by difference frequency generation of two-color near-infrared pulses that were produced in a novel inline optical parametric amplifier. The mid-infrared electric waveform was characterized by electro-optic sampling using 6.5-fs pulses at 620 nm.

We describe a few-cycle intense optical parametric chirped pulse amplifier (OPCPA) in the IR that is based on bismuth triborate (BiB3O6, BIBO) crystals. Two Ti:sapphire chirped pulse amplification systems are used to generate seed and pump pulses for the OPCPA. Carrier-envelope phase (CEP)-stabilized seed pulses in the IR are produced by difference frequency mixing of white light spanning from the visible to near IR range. The seed pulses, which have a nearly one octave-spanning spectrum around 1.6 μm, are temporally stretched in an acousto-optic programmable dispersive filter and amplified up to 550 μJ in two BIBO-based parametric amplifiers without losing their bandwidth. After compression in a fused silica block, we obtained 9.2 fs optical pulses with a repetition rate of 1 kHz, which comprise less than two optical cycles at 1.6 μm. These optical pulses were used to generate extreme ultraviolet (XUV) high harmonics in krypton. We succeeded in measuring the CEP dependence of the XUV radiation near the silicon L edge around 100 eV, verifying the passive stabilization of the CEP of the sub-two cycle IR pulses. The XUV spectra consist of two half-cycle cutoffs and show a clear transition from a modulated structure to a continuum near the cutoff. The continuum-like spectra as well as their CEP dependence indicate that they originate in a single recombination burst, showing that few-cycle IR OPCPA light sources are capable of generating attosecond pulses in the XUV region.

An optical parametric chirped-pulse amplifier (OPCPA) based on bismuth triborate (BiB3O6, BIBO) crystals has been developed to deliver 1.5 mJ, 10.1 fs optical pulses around 1.6 μm with a repetition rate of 1 kHz and a stable carrier-envelope phase. The seed and pump pulses of the BIBO-based OPCPA are provided from two Ti:sapphire chirped-pulse amplification (CPA) systems. In both CPA systems, transmission gratings are used in the stretchers and compressors that result in a high throughput and robust operation without causing any thermal problem and optical damage. The seed pulses of the OPCPA are generated by intrapulse frequency mixing of a spectrally broadened continuum, temporally stretched to approximately 5 ps then, and amplified to more than 1.5 mJ. The amplified pulses are compressed in a fused silica block down to 10.1 fs. This BIBO-based OPCPA has been applied to high-flux high harmonic generation beyond the carbon K edge at 284 eV. The high-flux soft-x-ray continuum allows measuring the x-ray absorption near-edge structure of the carbon K edge within 2 min, which is shorter than a typical measurement time using synchrotron-based light sources. This laser-based table-top soft-x-ray source is a promising candidate for ultrafast soft x-ray spectroscopy with femtosecond to attosecond time resolution.