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Optical oscillators present a powerful optimization mechanism. The inherentcompetition for the gain resources between possible modes of oscillationentails the prevalence of the most efficient single mode. We harness this'ultrafast' coherent feedback to optimize an optical field \emph{in time}, andshow that when an optical oscillator based on a molecular gain medium issynchronously-pumped by ultrashort pulses, a temporally coherent multi modefield can develop that optimally dumps a general, dynamically-evolvingvibrational wave-packet, into a \emph{single vibrational target state}.Measuring the emitted field opens a new window to visualization and control offast molecular dynamics. The realization of such a coherent oscillator with hotalkali dimers appears within experimental reach.

Coherent Amplification of Ultrafast Molecular Dynamics in an Optical Oscillator