Direct and indirect methods for studying the energetics and dynamics of the Auger Doppler effect in femtosecond ultra-fast dissociation

Molecules may fragment within a few femtoseconds after core-excitation, a phenomenon known as ultra-fast dissociation. With the aim of providing an understanding of the fundamental phenomenology of the Auger Doppler effect, two methods are presented to study the energetics and dynamics, i.e., the kinetic energy release and the fragment velocities in such processes. The first, direct, method is based on the shifts in kinetic energy of the Auger electrons due to the velocity acquired by the fragment in the ultra-fast dissociation process, i.e., the Auger Doppler effect. The second, indirect, method is based on total-energy arguments in a Born–Haber cycle for excitation, dissociation, and ionization. A combination of the two methods is shown to be able to reproduce experimental spectra well. Based on this, predictions are made for other, yet unstudied, molecular systems. It is also shown that the Auger Doppler effect is not static, but will exhibit dynamic photon energy dependence. The complete energetics of...

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