Role of the intramolecular phase in high-harmonic generation

Phys Rev Lett. 2002 May 6;88(18):183903. doi: 10.1103/PhysRevLett.88.183903. Epub 2002 Apr 23.


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.