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Long-lived electronic coherences in molecular wave packets probed with pulse-shape spectroscopy

2024/09/25 by Brian Kaufman, Philipp Marquetand, Tamás Rozgonyi +1 · 1 voice
Physics and Astronomy · Chemistry · #Laser-Matter Interactions and Applications #Spectroscopy and Quantum Chemical Studies #Spectroscopy and Laser Applications

paper · doi:10.1103/physreva.110.033118

openalex publication_date 2024/09/25 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

We explore long-lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that for particular pairs of states, the electronic phase remains well defined despite vibrational motion along many degrees of freedom. We explore the time dependence of the electronic coherence and show how it is modulated by the time-dependent vibrational overlap between the two wave functions. Our measurements are interpreted with electronic structure calculations and compared to analytic expressions for the electronic coherence.

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