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

TL;DR

This paper demonstrates direct measurement of helium's doubly-excited state lifetimes in the time domain using attosecond noncollinear four-wave-mixing spectroscopy, aligning with theoretical predictions and advancing quantum dynamics understanding.

Contribution

It introduces a novel application of attosecond FWM spectroscopy to measure natural lifetimes of doubly-excited states in helium directly in the time domain.

Findings

Measured lifetimes agree with spectral and theoretical values.

FWM spectral features are Lorentzian without strong-field effects.

Strong-field effects onset at approximately 0.3 Rabi cycles.

Abstract

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, are showcase scenarios of electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly-excited $^1$P$^o$ 2s$n$p Rydberg series and the $^1$S$^e$ 2p$^2$ dark state in helium in the 60 eV to 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 are in agreement 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 such as molecules in the future.