We report the experimental implementation of femtosecond polarization pulse shaping within an adaptive learning loop. This technique makes it possible to optimally and automatically generate light fields in which intensity, momentary frequency, and light polarization (i.e., ellipticity and orientation) change as a function of time within a single femtosecond laser pulse. By use of second-harmonic generation as a feedback signal in an evolutionary algorithm, specific phase- and polarization-modulated laser pulses are generated. Material dispersion and time-dependent modulations of the polarization state can be compensated. These experiments demonstrate the feasibility of adaptive quantum control experiments with polarization-shaped femtosecond laser pulses.
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