Clocking Auger Electrons

Abstract

Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. As the relaxation occurs primarily via Auger emission, excited state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive at XFELs due to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here, we develop a new approach termed self-referenced attosecond streaking, based upon simultaneous measurements of streaked photo- and Auger electrons. Our technique enables sub-femtosecond resolution in spite of jitter. We exploit this method to make the first XFEL time-domain measurement of the Auger decay lifetime in atomic neon, and, by using a fully quantum-mechanical description, retrieve a lifetime of $2.2_{-0.3}^{+0.2}$ fs for the KLL decay channel. Importantly, our technique can be generalised to permit the extension of attosecond time-resolved experiments to all current and future FEL facilities.

arXiv commentMain text: 20 pages, 3 figures. Supplementary information: 17 pages, 6 figures

References in corpus (6)

• Tunable Isolated Attosecond X-ray Pulses with Gigawatt Peak Power from a Free-Electron Laser
• Double core hole production in N2: Beating the Auger clock
• Experimental Verification of the Chemical Sensitivity of Two-Site Double Core-Hole States Formed by an X-ray FEL
• Molecular double core-hole electron spectroscopy for chemical analysis
• Strong-field extreme-ultraviolet dressing of atomic double excitation
• Theoretical study of electronic damage in single particle imaging experiments at XFELs for pulse durations 0.1 - 10 fs

Cited by in corpus (6)

• Attosecond Coherent Electron Motion in Auger-Meitner Decay
• Accurate core excitation and ionization energies from a state-specific coupled-cluster singles and doubles approach
• Artificial intelligence for online characterization of ultrashort X-ray free-electron laser pulses
• Correlation Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
• Radiationless decay spectrum of O 1s double core holes in liquid water
• Streaking single-electron ionization in open-shell molecules driven by X-ray pulses