Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

Rupprecht, Patrick; Puskar, Nicolette G.; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1103/PhysRevResearch.6.043100

Title: Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

Journal Article · 04 November 2024 · Physical Review Research

DOI: https://doi.org/10.1103/PhysRevResearch.6.043100 · OSTI ID:2476265

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The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited $^{1} P^{o} 2 s n p$ Rydberg series and the $^{1} S^{e} 2 p^{2}$ dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2476265

Journal Information:: Physical Review Research, Journal Name: Physical Review Research Journal Issue: 4 Vol. 6; ISSN PPRHAI; ISSN 2643-1564

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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