Abstract
We demonstrate that the vibrational nuclear motion of singly ionized argon dimers can be controlled with two ultrashort laser pulses of different wavelengths. In particular, we observe a striking "gap" in the pump-probe-delay-dependent kinetic-energy release spectrum only if the probe-pulse wavelength exceeds the pump-pulse wavelength. This "frustrated dissociation effect" is reproduced by our two-state quantum mechanical model, validating its interpretation as a pump-pulse-initiated population transfer between dipole-coupled Born-Oppenheimer electronic states of the dissociating Ar(2)(+) molecular ion. Our numerical results also reproduce the measured collapse and fractional revival of the oscillating Ar(2)(+) nuclear wave packet, and, for single-pulse dissociation, the decrease of the kinetic-energy release with increasing laser wavelength.
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