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.