Charge Transfer in the Dissociative Single Ionization of an Ar-Kr Dimer

We present direct experimental evidence of laser-induced charge transfer in the dissociative single ionization of an Ar-Kr dimer: Ar-Kr+nℏω⟶ionizationAr-Kr++e−+mℏω⟶charge transferAr+-Kr+e−⟶dissociationAr++Kr+e−. Coincidence detection of Ar+ fragments and photoelectrons generated by a 400 nm femtosecond pulse shows that ionization initially occurs at the Kr site, followed by charge transfer from Ar to Kr+ prior to dissociation. Time-resolved kinetic energy release spectra, obtained with a delayed 800 nm probe, exhibit vibrational revivals that map nuclear wave packet motion on the X(1/2) and A2(1/2) states of Ar-Kr+. Relative-phase-controlled two-color fields enable directional control of Ar+ emission, with phase-dependent asymmetries reproduced by time-dependent Schrödinger equation simulations, revealing the governing role of wave packet interference in the charge transfer dynamics.