We generated single-cycle isolated attosecond pulses around ∼36 electron volts using phase-stabilized 5-femtosecond driving pulses with a modulated polarization state. Using a complete temporal characterization technique, we demonstrated the compression of the generated pulses for as low as 130 attoseconds, corresponding to less than 1.2 optical cycles. Numerical simulations of the generation process show that the carrier-envelope phase of the attosecond pulses is stable. The availability of single-cycle isolated attosecond pulses opens the way to a new regime in ultrafast physics, in which the strong-field electron dynamics in atoms and molecules is driven by the electric field of the attosecond pulses rather than by their intensity profile.

We study numerically the generation of high-order harmonics by two-center molecules for arbitrary angles between the molecular axis and the laser polarization axis. For fixed angle, the harmonic spectrum exhibits a minimum at a frequency which is independent of the laser parameters. The amplitude of each harmonic is strongly angle dependent, and a pronounced minimum is found at the same angle where a sudden jump in the harmonic phase occurs. By calculating the spatial dependence of the harmonic amplitudes and phases, we are able to explain these effects in terms of interfering contributions from various regions within the molecule.

We study high-order harmonic generation for ${\mathrm{H}}_2^{+}$ and ${\mathrm{H}}_2$ model molecules in linearly polarized laser pulses by numerical solution of the Schrödinger equation. Maxima and minima due to intramolecular interference are found in the dependence of the harmonic intensities on the internuclear distance and on the orientation of the molecules. These extrema can be approximately predicted by regarding them as the result of interference between two radiating point sources located at the positions of the nuclei.

We experimentally investigate the process of intramolecular quantum interference in high-order harmonic generation in impulsively aligned ${\mathrm{CO}}_2$ molecules. The recombination interference effect is clearly seen through the order dependence of the harmonic yield in an aligned sample. The experimental results can be well modeled assuming that the effective de Broglie wavelength of the returning electron wave is not significantly altered by the Coulomb field of the molecular ion. We demonstrate that such interference effects can be effectively controlled by changing the ellipticity of the driving laser field.