Relationship between polarization-averaged molecular-frame photoelectron angular distributions and geometry

Internal inelastic scattering satellite probed by molecular-frame photoelectron angular distributions from CO2.

The molecular-frame photoelectron angular distribution (MFPAD) of the satellite accompanying the C 1s photoline of the CO2 molecule has been measured at the C 1s(2sigmag)-->4sigmau* shape resonance, using electron-ion multicoincidence momentum spectroscopy. The observed MFPAD indicates that the conjugate satellite is excited by internal inelastic scattering. In this scenario, a photoelectron is...

Imaging polyatomic molecules in three dimensions using molecular frame photoelectron angular distributions.

We demonstrate a method for determining the full three-dimensional molecular-frame photoelectron angular distribution in polyatomic molecules using methane as a prototype. Simultaneous double Auger decay and subsequent dissociation allow measurement of the initial momentum vectors of the ionic fragments and the photoelectron in coincidence, allowing full orientation by observing a three-ion dec...

Probing molecular frame photoelectron angular distributions via high-order harmonic generation from aligned molecules

We analyse the theory of single photoionization (PI) and high-order harmonic generation (HHG) by intense lasers from aligned molecules. We show that molecular-frame photoelectron angular distributions can be extracted from these measurements. We also show that, under favourable conditions, the phase of PI transition dipole matrix elements can be extracted from the HHG spectra. Furthermore, by v...

Dependence of strong-field photoelectron angular distributions on molecular orientation

We have analysed angular distributions of the photoelectron yields arising from strong-field ionization of diatomic and polyatomic linear molecules using a leading-order intense-field S-matrix theory. For molecules with active π electrons the distribution is found to strongly depend on the degree of molecular alignment, showing a nodal minimum along the laser polarization direction as a charact...

Photoelectron angular distributions for atomic chlorine.