State-selective probing of CO2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Fidler, Ashley P.; Lin, Yen-Cheng; Gaynor, James D.; McCurdy, C. William; Leone, Stephen R.; Lucchese, Robert R.; Neumark, Daniel M.

doi:10.1103/physreva.106.063525

Title: State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Journal Article · Fri Dec 30 00:00:00 EST 2022 · Physical Review A

DOI:https://doi.org/10.1103/physreva.106.063525· OSTI ID:1974754

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^[2]; Gaynor, James D. ^[2]; McCurdy, C. William ^[3];

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^[4]; Neumark, Daniel M. ^[2]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States); Princeton Univ., NJ (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Davis, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO₂. This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ_g Rydberg series that converges to the ionic $$\widetilde{B}$$ ²Σ$$^{+}_{u}$$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ_g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ_g Rydberg series and emission from the sharp ndσ_g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

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

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

Grant/Contract Number:: AC02-05CH11231; BES-ERCAP0020143; DEAC02-05CH11231

OSTI ID:: 1974754

Alternate ID(s):: OSTI ID: 1907191

Journal Information:: Physical Review A, Vol. 106, Issue 6; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
autoionization & auger processes
electronic excitation & ionization
light-matter interaction
nonlinear optics
optical transient phenomena
single- and few-photon ionization & excitation
ultrafast phenomena
molecules
Rydberg atoms & molecules
attosecond laser spectrometry
configuration interaction
four-wave mixing
high-harmonic generation
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Title: State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

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