High-order harmonic generation (HHG) from atoms and molecules offers potential application as a coherent ultrashort radiation source in the extreme ultraviolet and soft X-ray regions. In the three-step model of HHG, an electron tunnels out from the atom and may recombine with the parent ion (emitting a high-energy photon) after undergoing laser-driven motion in the continuum. Aligned molecules can be used to study quantum phenomena in HHG associated with molecular symmetries; in particular, simultaneous observations of both ion yields and harmonic signals under the same conditions serve to disentangle the contributions from the ionization and recombination processes. Here we report evidence for quantum interference of electron de Broglie waves in the recombination process of HHG from aligned CO2 molecules. The interference takes place within a single molecule and within one optical cycle. Characteristic modulation patterns of the harmonic signals measured as a function of the pump-probe delay are explained with simple formulae determined by the valence orbital of the molecules. We propose that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.

We demonstrate that molecules with a moderate permanent dipole moment can be oriented with combined electrostatic and pulsed, nonresonant laser fields. We use OCS molecules as a sample. The degree of orientation can be increased by increasing the magnitude of electrostatic field and the peak intensity of the laser field or by decreasing the rotational temperature of the molecules.

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We demonstrate laser-field-free molecular orientation with the combination of a moderate electrostatic field and an intense nonresonant rapidly turned-off laser field, which can be shaped with the plasma shutter technique. We use OCS (carbonyl sulfide) molecules as a sample. Molecular orientation is adiabatically created in the rising part of the laser pulse, and it is found to revive at around the rotational period of an OCS molecule with the same degree of orientation as that at the peak of the laser pulse in the virtually laser-field-free condition. This accomplishment means that a new class of molecular sample has become available for various applications.

We observe high-order harmonic spectra generated from a thin atomic medium, Ar, Kr, and Xe, by intense 800-nm and 1300-nm femtosecond pulses. A clear signature of a single-atom response is observed in the harmonic spectra. Especially in the case of Ar, a Cooper minimum, reflecting the electronic structure of the atom, is observed in the harmonic spectra. We successfully extract the photorecombination cross sections of the atoms in the field-free condition with the help of an accurate recolliding electron wave packet. The present protocol paves the way for exploring ultrafast imaging of molecular dynamics with attosecond resolution.

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We report clear evidence of all-optical orientation of carbonyl sulfide molecules with an intense nonresonant two-color laser field in the adiabatic regime. The technique relies on the combined effects of anisotropic hyperpolarizability interaction and anisotropic polarizability interaction and does not rely on the permanent dipole interaction with an electrostatic field. It is demonstrated that the molecular orientation can be controlled simply by changing the relative phase between the two wavelength fields. The present technique brings researchers a new steering tool of gaseous molecules and will be quite useful in various fields such as electronic stereodynamics in molecules and ultrafast molecular imaging.