Maximizing Hole Coherence in Ultrafast Photoionization of Argon with SPA-Optimization

Abstract: Photoionization with attosecond pulses populates hole states in the photoion. Superpositions of hole states represent ideal candidates for time-dependent spectroscopy, for example via pump-probe studies. The challenge consists in identifying pulses that create coherent superpositions of hole states while satisfying practical constraints. Here, we employ quantum optimal control to maximize the degree of coherence between these hole states. To this end, we introduce a derivative-free optimization method with Sequential PArametrization update (SPA-optimization). We demonstrate the versatility and computational efficiency of SPA-optimization for photoionization in argon by maximizing the coherence between the $3s$ and $3p_0$ hole states using shaped attosecond pulses. We show that it is possible to maximize the hole coherence while simultaneously prescribing the ratio of the final hole state populations.