We show that the proportion of double Auger decay following creation of single 1s core holes in molecules containing C, N and O atoms is greater than usually assumed, amounting to about 10% of single Auger decay in many cases. It varies from molecule to molecule, where the size of the molecule has a positive correlation to the amount of double Auger decay. In neon, examined as a related benchmark, the proportion of double Auger decay is similar to that in methane, and is in the order of 5%.
Three-electron Auger decay is an exotic and elusive process, in which two outer-shell electrons simultaneously refill an inner-shell double vacancy with emission of a single Auger electron. Such transitions are forbidden by the many-electron selection rules, normally making their decay lifetimes orders of magnitude longer than the few-femtosecond lifetimes of normal (two-electron) Auger decay. Here we present theoretical predictions and direct experimental evidence for a few-femtosecond three-electron Auger decay of a double inner-valence-hole state in CH_{3}F. Our analysis shows that in contrast to double core holes, double inner-valence vacancies in molecules can decay exclusively by this ultrafast three-electron Auger process, and we predict that this phenomenon occurs widely.
Using a new multi-electron multi-ion coincidence apparatus and soft x-ray synchrotron radiation we have determined branching ratios to final Xen+ states with 2 < n < 9 from the 4d−1, 4p−1, 4s−1, 3d−1 and 3p−1 Xe+ hole states. The coincident electron spectra give information on the Auger cascade pathways. We show that by judicious choice of coincident electrons, almost pure single charge states of the final ions can be selected.
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