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Photoelectron spectra and photoelectron angular distributions obtained in photoionization reveal important information on e.g. charge transfer or hole coherence in the parent ion. Here we show that optimal control of the underlying quantum dynamics can be used to enhance desired features in the photoelectron spectra and angular distributions. To this end, we combine Krotovs method for optimal control theory with the time-dependent configuration interaction singles formalism and a splitting approach to calculate photoelectron spectra and angular distributions. The optimization target can account for specific desired properties in the photoelectron angular distribution alone, in the photoelectron spectrum, or in both. We demonstrate the method for hydrogen and then apply it to argon under strong XUV radiation, maximizing the difference of emission into the upper and lower hemispheres, in order to realize directed electron emission in the XUV regime.
Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process. In this work, we investigate this multiplexing via computation of the observable photo
The combination of photoelectron spectroscopy and ultrafast light sources is on track to set new standards for detailed interrogation of dynamics and reactivity of molecules. A crucial prerequisite for further progress is the ability to not only dete
We show that the combination of two achiral components - atomic or molecular target plus a circularly polarized photon - can yield chirally structured photoelectron angular distributions. For photoionization of CO, the angular distribution of carbon
We present an experimental and theoretical study of core-level ionization of small hetero- and homo-nuclear molecules employing circularly polarized light and address molecular-frame photoelectron angular distributions in the lights polarization plan
Time-resolved pump-probe measurements of Xe, pumped at 133~nm and probed at 266~nm, are presented. The pump pulse prepared a long-lived hyperfine wavepacket, in the Xe $5p^5(^2P^{circ}_{1/2})6s~^2[1/2]^{circ}_1$ manifold ($E=$77185 cm$^{-1}=$9.57 eV)