Molecular Imaging Using High-Order Harmonic Generation and Above-Threshold Ionization

Accurate molecular imaging via high-order harmonic generation relies on comparing harmonic emission from a laser-irradiated molecule and an adequate reference system. However, an ideal reference atom with the same ionization properties as the molecule is not always available. We show that for suitably designed, very short laser pulses, a one-to-one mapping from high-order harmonic frequencies to electron momenta in above-threshold ionization exists. Comparing molecular and atomic momentum distributions then provides the electron recollision amplitude in the molecule for enhanced molecular imaging. The method retrieves the molecular recombination transition moments highly accurately, even with suboptimal reference atoms.