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.

We demonstrate an optical parametric chirped-pulse amplifier producing infrared 20 fs (3-optical-cycle) pulses with a stable carrier-envelope phase. The amplifier is seeded with self-phase-stabilized pulses obtained by optical rectification of the output of an ultrabroadband Ti:sapphire oscillator. Energies of -80 microJ with a well-suppressed background of parametric superfluorescence and up to 400 microJ with a superfluorescence background are obtained from a two-stage parametric amplifier based on periodically poled LiNbO3 and LiTaO3 crystals. The parametric amplifier is pumped by an optically synchronized 1 kHz, 30 ps, 1053 nm Nd:YLF amplifier seeded by the same Ti:sapphire oscillator.

We produce carrier-envelope-phase-stable 15.7-fs (2-cycle) 740-microJ pulses at the 2.1-microm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 49-ps 11-mJ Nd:YLF laser. A novel seed pulse spectral shaping method is used to ascertain the true amplified seed energy and the parametric superfluorescence levels.

We propose a method for achieving molecular orientation by two-step excitation with intense femtosecond laser and terahertz (THz) pulses. First, the femtosecond laser pulse induces off-resonant impulsive Raman excitation to create rotational wave packets. Next, a delayed intense THz pulse effectively induces resonant dipole transition between neighboring rotational states. By controlling the intensities of both the pulses and the time delay, we can create rotational wave packets consisting of states with different parities in order to achieve a high degree of molecular orientation under a field-free condition. We numerically demonstrate that the highest degree of orientation of cos θ > 0.8 in HBr molecules is feasible under experimentally available conditions.

Using light to manipulate materials into desired states is one of the goals in condensed matter physics, since light control can provide ultrafast and environmentally friendly photonics devices. However, it is generally difficult to realise a photo-induced phase which is not merely a higher entropy phase corresponding to a high-temperature phase at equilibrium. Here, we report realisation of photo-induced insulator-to-metal transitions in Ta2Ni(Se1−xSx)5 including the excitonic insulator phase using time- and angle-resolved photoemission spectroscopy. From the dynamic properties of the system, we determine that screening of excitonic correlations plays a key role in the timescale of the transition to the metallic phase, which supports the existence of an excitonic insulator phase at equilibrium. The non-equilibrium metallic state observed unexpectedly in the direct-gap excitonic insulator opens up a new avenue to optical band engineering in electron–hole coupled systems.

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.

Real-time impulsive resonant Raman scattering induced by a 4-fs ultrashort laser pulse was spectrally resolved with a multichannel lock-in amplifier. An optical and vibrational two-dimensional spectrum was introduced to separate the effects of electronic and vibrational broadening in the power spectrum of the vibrations. Spectrally resolved real-time oscillations can identify the wave packet motion associated with the stretching vibrational mode of the carbon-carbon double and triple bonds of the polymer polydiacetylene. Calculated nonlinear polarizations which take into account the ground-state wave packets reproduced the observed dynamics fairly well. It is confirmed that the ground-state vibrations play a significant role in the dynamics of the wave packet even far below the absorption edge, as well as the excited-state vibrations.

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).