Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping

Abstract

We report two schemes to generate perfect anisotropy in the photoelectron angular distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full control over the anisotropy of photoelectron emission, we exploit interferences between single-photon pathways and a manifold of resonantly-enhanced two-photon pathways. These are shown to outperform nonsequential (ω, 2ω) bichromatic phase control for the example of CHFClBr molecules. We are able to optimize pulses that yield anisotropic photoelectron emission thanks to a very efficient calculation of photoelectron momentum distributions. This is accomplished by combining elements of quantum chemistry, variational scattering theory, and time-dependent perturbation theory.

Disentangling enantiosensitivity from dichroism using bichromatic fields

“…Type (iii) signals are well known in atoms subject to light fields whose Lissajous figure is not symmetric under spatial inversion [30]. They have also been recently calculated for the case of randomly oriented chiral molecules [31] for parallel polarizations of ω and 2ω. Here, type (iii) signals are due to the asymmetry of the field (2) along the z direction (see Fig.…”

Disentangling enantiosensitivity from dichroism using bichromatic fields

“…Type (iii) signals are well known in atoms subject to light fields whose Lissajous figure is not symmetric under spatial inversion. 33 They have also been recently calculated for the case of randomly oriented chiral molecules 34 for parallel polarizations of ω and 2 ω . Here, type (iii) signals are due to the asymmetry of the field (2) along the z direction (see Fig.…”

Multi-photon above threshold ionization of multi-electron atoms and molecules using the R-matrix approach

“…Multi-photon ionization (MPI) and its variant resonance-enhanced multi-photon ionization (REMPI) in atoms and molecules have a range of important applications ranging from laser-induced plasma generation [1,2], chemical diagnostics [3][4][5], chiral recognition [6][7][8][9][10] to laser-filamentation [11][12][13][14][15], harmonic [16][17][18] and high-harmonic [19] generation and photoelectron spectroscopy [20]. Given its practical importance accurate data on MPI are surprisingly scarce and striking discrepancies in the MPI cross sections remain in the literature despite recent advances in the experimental technology [1].…”