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Coherence among rotational ion channels during photoionization is exploitedto control the anisotropy of the resulting photoelectron angular distributionsat specific photoelectron energies. The strategy refers to a robust and singleparameter control using two ultra-short light pulses delayed in time. The firstpulse prepares a superposition of a few ion rotational states, whereas thesecond pulse serves as a probe that gives access to a control of the molecularasymmetry parameter $\beta$ for individual rotational channels. This isachieved by tuning the time delay between the pulses leading to channelinterferences that can be turned from constructive to destructive. Theillustrative example is the ionization of the $E(1\Sigma_{g}^{+})$ state ofLi$_{2}$. Quantum wave packet evolutions are conducted including bothelectronic and nuclear degrees of freedom to reach angle-resolved photoelectronspectra. A simple interference model based on coherent phase accumulationduring the field-free dynamics between the two pulses is precisely exploited tocontrol the photoelectron angular distributions from almost isotropic, tomarked anisotropic.

Anisotropy Control in Photoelectron Spectra: A Coherent Two-Pulse Interference Strategy