Abstract

AbstractUltrafast photoexcitation of molecules prepares coherent superpositions of vibrational states, forming wave packets. We show direct experimental evidence that impulsive collisions of photo‐fragments with large energy loss generate new coherent superpositions of vibrational states, causing coherence among previously unoccupied states. We demonstrate the effect in the model system of I2 molecules in Kr solids. This coherence transfer—even in the presence of very strong dissipation—may be used for control strategies in condensed‐phase photoreactions.

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