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| Title
| - Pump-Shaped Dump Optimal Control Reveals the NuclearReaction Pathway of Isomerization of a Photoexcited CyanineDye
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| - Using optimal control as a spectroscopic tool we decipher the details of the molecular dynamicsof the essential multidimensional excited-state photoisomerization a fundamental chemical reaction ofkey importance in biology. Two distinct nuclear motions are identified in addition to the overall bond-twistingmotion: Initially, the reaction is dominated by motion perpendicular to the torsion coordinate. At later times,a second optically active vibration drives the system along the reaction path to the bottom of the excited-state potential. The time scales of the wavepacket motion on a different part of the excited-state potentialare detailed by pump-shaped dump optimal control. This technique offers new means to control a chemicalreaction far from the Franck−Condon point of absorption and to map details of excited-state reactionpathways revealing unique insights into the underlying reaction mechanism.
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