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

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

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

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. 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.

Original languageEnglish (US)
Article number033117
JournalPhysical Review A
Volume107
Issue number3
DOIs
StatePublished - Mar 2023

Funding

This work was performed by personnel and equipment supported by the Office of Science, Office of Basic Energy Sciences through the Atomic, Molecular, and Optical Sciences Program of the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy (DOE) at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231. Y-C.L. acknowledges financial support from the Taiwan Ministry of Education. J.G. acknowledges the Arnold and Mabel Beckman Foundation for support as an Arnold O. Beckman Postdoctoral Fellow. L.A., S.C., and C.M. acknowledge financial support from NSF theoretical AMO Grant No. PHY-1912507 and from DOE CAREER Grant No. DE-SC0020311. C.K. acknowledges support through the National Science Foundation Research Experiences for Undergraduates Grants No. EEC-1461231 and No. EEC-1852537.

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Fingerprint

Dive into the research topics of 'Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy'. Together they form a unique fingerprint.

Cite this