We present direct experimental evidence of laser-induced charge transfer in the dissociative single ionization of an Ar-Kr dimer: $\mathrm{Ar}\text{−}\mathrm{Kr}+n\hslash \omega \stackrel{\text{ionization}}{⟶}\mathrm{Ar}\text{−}{\mathrm{Kr}}^{+}+e^{-}+m\hslash \omega \stackrel{\text{charge transfer}}{⟶}{\mathrm{Ar}}^{+}\text{−}\mathrm{Kr}+e^{-}\stackrel{\text{dissociation}}{⟶}{\mathrm{Ar}}^{+}+\mathrm{Kr}+e^{-}$. Coincidence detection of ${\mathrm{Ar}}^{+}$ 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 ${\mathrm{Kr}}^{+}$ 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 $A_2(1/2)$ states of ${\mathrm{Ar}\text{−}\mathrm{Kr}}^{+}$. Relative-phase-controlled two-color fields enable directional control of ${\mathrm{Ar}}^{+}$ 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.

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• Atomic & molecular processes in external fields
• Chemical charge transfer
• Coherent control
• Molecular dissociation
• Multiphoton or tunneling ionization & excitation
• Strong field ionization & excitation
• Clusters
• Femtosecond laser irradiation
• Ultrafast femtosecond pump probe