Feedback Optimization Strategy for Rotational Alignment Echo Spectroscopy

The recent discovery of rotational echoes has contributed to extend the applications field‐free molecular alignment short time scales, namely a temporal region preceding first revival molecule. Most echo measurements require adjusting position over time, which in case unavoidably leads change its amplitude, unless intensity pulse sequence triggering is properly modified. Herein, it proposed avoid this drawback by using an optical shaper steered learning algorithm. It demonstrated that shaping, whose characteristics are optimized maintain constant amplitude regardless creation can be generated controlling spectral phase and laser then used open‐loop control system. As proof principle, optimization strategy applied observation short‐term dissipative dynamics laser‐aligned molecules exposed collisions measurement associated decoherence population decay constants.