Abstract

We theoretically investigate the decaying dynamics in model molecules by using attosecond wave-mixing spectroscopy. We find that transient wave-mixing signal in molecular systems can be used to measure the lifetimes of vibrational states with attosecond time resolution. Typically, there are many vibrational states in the molecular system, and the molecular wave-mixing signal with a specific energy at a specific emitting angle is contributed by many possible wave-mixing pathways. In addition, the vibrational revival phenomenon in the previous ion detection experiments has also been observed in this all-optical approach. This work provides a new, to the best of our knowledge, route for the decaying dynamics detection and wave packet control of molecular systems.

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