Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Puskar, Nicolette G.; Lin, Yen-Cheng; Gaynor, James D.; Schuchter, Maximilian C.; Chattopadhyay, Siddhartha; Marante, Carlos; Fidler, Ashley P.; Keenan, Clare L.; Argenti, Luca; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1103/physreva.107.033117

Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Journal Article · Mon Mar 27 00:00:00 EDT 2023 · Physical Review A

DOI:https://doi.org/10.1103/physreva.107.033117· OSTI ID:2228885

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Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland). Laboratory for Physical Chemistry
Univ. of Central Florida, Orlando, FL (United States)
Princeton Univ., NJ (United States)
Univ. of Chicago, IL (United States)

Attosecond noncollinear four-wave-mixing spectroscopy with one attosecond extreme ultraviolet (XUV) pulse and two few-cycle near-infrared (NIR) pulses was used to measure the autoionization decay lifetimes of inner valence electronic excitations in neon atoms. After a 43-48-eV XUV photon excites a 2s electron into the 2s2p⁶(np) Rydberg series, broadband NIR pulses couple the 2s2p⁶3p XUV-bright state to neighboring 2s2p⁶3s and 2s2p⁶3d XUV-dark states. Controllable delays of one or both NIR pulses with respect to the attosecond XUV pulse reveal the temporal evolution of either the dark or bright states, respectively. Experimental lifetimes for the 3s, 3p, and 3d states are measured to be 7±2, 48±8, and 427±40 fs, respectively, with 95% confidence. Accompanying calculations with two independent ab initio theoretical methods, newstock and astra, verify the findings. The results support the expected trend that the autoionization lifetime should be longer for states that have a smaller penetration in the radial region of the 2s core hole, which in this case is for the higher angular momentum Rydberg orbitals. In conclusion, the underlying theory thus links the lifetime results to electron correlation and provides an assessment of the direct and exchange terms in the autoionization process.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-05CH11231; SC0020311

OSTI ID:: 2228885

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 3 Vol. 107; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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