Time-and-energy-resolved measurement of Auger cascades following Kr 3d excitation by attosecond pulses

Physics

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Scientific paper

We show that attosecond metrology has evolved from proof-of-principle experiments to a level where complex processes can be resolved in time that cannot be accessed using any other existing technique. The cascaded Auger decay following ionization and excitation of the 3d-subshell in Kr with subfemtosecond 94 eV soft x-ray pulses has been energy- and time-resolved in an x-ray pump-infrared probe experiment. This Auger cascade reveals rich multi-electron dynamics, which despite the fact that there are many experimental and theoretical data available, is not yet fully understood. We present time-resolved data showing the sequence of the temporal dynamics in the cascaded Auger decay. The decay time of several groups of lines has been measured, including the lines at the low-energy part of the spectrum, which are predominantly produced by the second-step Auger transitions. Our experimental data reveal long lifetimes (up to 70 fs) of the subvalence excited ionic (intermediate) states in the cascaded resonant Auger decay. Extensive theoretical calculations within the multiconfiguration Dirac-Fock (MCDF) approach show that the observed long lifetime may be attributed to the second-step Auger decay of the resonantly excited 3d-1np states with n = 6,7. Furthermore, our experimental data show that the electrons with a kinetic energy around 25 eV (generally assigned as M4,5N1N1 1S0 normal Auger lines) have a component corresponding to the second-step Auger decay of the ion after resonant Auger transition 3d-1np → 4s2 4p3 4dnp → 4s2 4p4 with a lifetime of 26 ± 4 fs.

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