Probing molecular frame photoionization via laser generated high-order harmonics from aligned molecules.

Present experiments cannot measure molecular frame photoelectron angular distributions (MFPAD) for ionization from the outermost valence orbitals of molecules. We show that the details of MFPAD can be retrieved with high-order harmonics generated by infrared lasers from aligned molecules. Using accurately calculated photoionization transition dipole moments for fixed-in-space molecules, we show that the dependence of the magnitude and phase of the high-order harmonics on the alignment angle of the molecules observed in recent experiments can be quantitatively reproduced. This result provides the needed theoretical basis for ultrafast dynamic chemical imaging using infrared laser pulses.