Ultrafast laser-driven quantum dynamics in positronium chloride.

We present a computational study of the laser-driven quantum dynamics of positronium (Ps), PsH, and PsCl at the time-dependent Hartree-Fock level of theory. To eliminate finite-basis effects and to properly capture continuum dynamics, we use a spherical polar pseudospectral representation. The multicomponent theory and its implementation are described in detail. We find that relative to H- and Cl-, respectively, the presence of the positron delays electron ionization in PsH, while slightly enhancing electron ionization in PsCl. In both cases, the positronic response is faster than that of the electrons. We propose that the formation of PsCl may be directly observed through photopositron spectra in the multiphoton regime, where PsCl peaks are expected at roughly twice the energy of Ps peaks, making PsCl clearly distinguishable from Ps. In the tunneling regime, however, photopositron rescattering peaks may only be distinguishable if the amount of Ps is sufficiently low.