Time-domain measurement of Auger electron dynamics in xenon atoms after giant resonant photoionization

TL;DR

This study uses attosecond soft X-ray pulses with stabilized laser phases to observe inner-shell electron dynamics in xenon, revealing unexpected temporal shifts in Auger electron emission not explained by existing theories.

Contribution

First time-resolved inner-shell electron spectroscopy of xenon with CEP-stabilized attosecond pulses, uncovering anomalous Auger electron timing and energy features.

Findings

Observed a 1.32 fs time shift in Auger electrons from xenon

Detected a pronounced minimum in Auger electron yield at 4 fs delay

Found inconsistencies with current streaking theories and energy-based lifetimes.

Abstract

Time-resolved measurement of Auger-Meitner (AM) decay [Nature 419, 803 (2002)] marked a milestone in the development of attosecond science. To date, the time constants for the AM decay processes obtained from the time-domain experiments were found to be consistent with the values deduced from conventional energy-domain measurements. One of the main factors limiting the temporal resolution of these studies is the unlocked carrier-envelope-phase (CEP) of the laser pulses used to probe the electronic dynamics triggered by inner-shell photoabsorption. In this work, we report time-resolved inner-shell electron spectroscopy of xenon and krypton using attosecond soft X-ray (atto-SXR) pulses centered at 130 eV in combination with CEP-stabilized few-cycle Yb laser pulses. We observed that the N$_{4,5}$OO Auger electrons from xenon exhibit a clear streaking pattern, but with an unexpected time shift of $\sim$ 1.32 fs relative to the 4$d$ photoelectrons. Furthermore, the energy-integrated yield of streaked Auger electrons from xenon exhibits a pronounced minimum at a pump-probe time delay of 4 fs. Neither of these observations can be explained by current streaking theories and both are inconsistent with lifetimes inferred from energy-domain measurements. The M$_{4,5}$NN Auger electrons from krypton partly overlap in energy with the 3$d$ inner-shell photoelectrons and do not show these anomalous features. This study offers new insights into the inner-shell electron dynamics of heavy atoms in the giant dipole resonance region, laying the groundwork for attosecond soft X-ray spectroscopy of molecular systems containing iodine or bromine atoms.