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Vibronic Coupling through the Continuum in the e + CO2 System

Publication at Faculty of Mathematics and Physics |
2022

Abstract

We report two-dimensional electron energy-loss spectra of CO2. The high-resolution experiment reveals a counterintuitive fine structure at energy losses where CO2 states form a vibrational pseudocontinuum.

Guided by the symmetry of the system, we constructed a four-dimensional nonlocal model for the vibronic dynamics involving two shape resonances (forming a Renner-Teller Pi(u) doublet at the equilibrium geometry) coupled to a virtual Sigma(+)(g) state. The model elucidates the extremely non-Born-Oppenheimer dynamics of the coupled nuclear motion , explains the origin of the observed structures.

It is a prototype of the vibronic coupling of metastable states in continuum.