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

Abstract

Present photoionization experiments cannot measure molecular frame photoelectron angular distributions (MFPAD) from the outermost valence electrons of molecules. We show that details of the 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.

5 pages, 4 figures

References in corpus (3)

• Accurate retrieval of structural information from laser-induced photoelectron and high-harmonic spectra by few-cycle laser pulses
• Extraction of the species dependent dipole moment from high-order harmonic spectra in rare gas atoms
• Theory of high-order harmonic generation from molecules by intense laser pulses

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• Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses
• Separation of Target Structure and Medium Propagation Effects in High-Harmonic Generation
• Analysis of effects of macroscopic propagation and multiple molecular orbitals on the minimum in high-order harmonic generation of aligned CO${}_2$
• High-order harmonic spectroscopy for molecular imaging of polyatomic molecules
• General phenomenology of ionization from aligned molecular ensembles
• Orientation and Alignment Dynamics of Polar Molecule Driven by Shaped Laser Pulses
• Microscopic theory of Raman scattering for the rotational organic cation in metal halide perovskites