5 years ago

Observation of Structural Wavepacket Motion: The Umbrella Mode in Rydberg-Excited N-Methyl Morpholine

Observation of Structural Wavepacket Motion: The Umbrella Mode in Rydberg-Excited N-Methyl Morpholine
Yao Zhang, Sanghamitra Deb, Hannes Jónsson, Peter M. Weber
We have observed time-resolved, structural dynamics of a coherent vibrational wavepacket in Rydberg-excited N-methyl morpholine, a molecule with 48 internal degrees of freedom. The molecular structure was established by associating the time-dependent Rydberg electron binding energy, obtained from time-resolved photoionization–photoelectron spectroscopy, to the molecular structure using self-interaction corrected density functional calculations. Optical excitation at 226 nm launches an oscillatory wavepacket in the amine umbrella coordinate with a 650 fs period. Even though the Franck–Condon excitation is at an angle of 17°, the wavepacket settles into an oscillation between 4° and −10° within a fraction of a vibrational period and then dephases with a time constant of 750 fs.

Publisher URL: http://dx.doi.org/10.1021/acs.jpclett.7b01274

DOI: 10.1021/acs.jpclett.7b01274

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