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Journal Article

A molecular clock for autoionization decay


Medišauskas,  Lukas
Max Planck Institute for the Physics of Complex Systems, Max Planck Society;

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Medišauskas, L., Bello, R. Y., Palacios, A., Gonzalez-Castrillo, A., Morales, F., Plimak, L., et al. (2017). A molecular clock for autoionization decay. Journal of Physics B, 50(14): 144001. doi:10.1088/1361-6455/aa7215.

Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-C9C9-1
The ultrafast decay of highly excited electronic states is resolved with a molecular clock technique, using the vibrational motion associated to the ionic bound states as a time-reference. We demonstrate the validity of the method in the context of autoionization of the hydrogen molecule, where nearly exact full dimensional ab-initio calculations are available. The vibrationally resolved photoionization spectrum provides a time-energy mapping of the autoionization process into the bound states that is used to fully reconstruct the decay in time. A resolution of a fraction of the vibrational period is achieved. Since no assumptions are made on the underlying coupled electron-nuclear dynamics, the reconstruction procedure can be applied to describe the general problem of the decay of highly excited states in other molecular targets.