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arXiv · 1606.02663

Imaging the Breakdown of Molecular-Frame Dynamics through Rotational Uncoupling

Lucas J. Zipp·Adi Natan·Philip H. Bucksbaum
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Abstract

We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through photoelectron imaging of a coherent molecular Rydberg wave packet in $\textrm{N}_2$. The photoelectron angular distribution shows a radically different time evolution than that of a typical molecular-frame-fixed electron orbital, revealing the uncoupled motion of the electron as it precesses around the $averaged$ anisotropic potential of the rotating ion-core.

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Lucas J. Zipp, Adi Natan, Philip H. Bucksbaum. 2017-07-04. Imaging the Breakdown of Molecular-Frame Dynamics through Rotational Uncoupling. https://doi.org/10.1103/physreva.95.061403

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