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Autoionization Dynamics of (2P1/2)ns/d States in Krypton Probed by Noncollinear Wave Mixing with Attosecond Extreme Ultraviolet and Few-Cycle Near Infrared Pulses

submitted on 10.06.2019 and posted on 11.06.2019 by Ashley Fidler, Hugo Marroux, Erika Warrick, Etienne Bloch, Wei Cao, Stephen Leone, Daniel Neumark
The autoionization dynamics of the (2P1/2)ns/d Rydberg states in krypton are investigated using wave-mixing signals generated with subfemtosecond XUV pulses and noncollinear, few-cycle NIR pulses. Despite quantum beat oscillations from the XUV-induced coherence, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states. Experimentally measured lifetimes for the wave-mixing signals emitting from the (2P1/2)6d/8s, 7d/9s, and 8d/10s resonances compare favorably with lifetimes for the (2P1/2)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways leads to reporter state-dependent decays in the wave-mixing signals. The results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.




Email Address of Submitting Author


Lawrence Berkeley National Laboratory


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflicts of interest.