Effects of Autoionizing Resonances on Wave-Packet Dynamics Studied by Time-Resolved Photoelectron Spectroscopy

Zhang, Pengju; Hoang, Van-Hung; Wang, Chuncheng; Luu, Tran Trung; Svoboda, Vít; Le, Anh-Thu; Wörner, Hans Jakob

doi:10.1103/physrevlett.130.153201

Effects of Autoionizing Resonances on Wave-Packet Dynamics Studied by Time-Resolved Photoelectron Spectroscopy

Journal Article · Wed Apr 12 00:00:00 EDT 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.130.153201· OSTI ID:2422210

Zhang, Pengju ^[1]; ^[2]; Wang, Chuncheng ^[3]; Luu, Tran Trung ^[4]; Svoboda, Vít ^[5]; Le, Anh-Thu ^[6]; ^[7]

Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); OSTI
Missouri Univ. of Science and Technology, Rolla, MO (United States); Kansas State Univ., Manhattan, KS (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Jilin Univ., Changchun (China)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Univ. of Hong Kong, Pokfulam (Hong Kong)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Univ. of Colorado, Boulder, CO (United States); National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
Missouri Univ. of Science and Technology, Rolla, MO (United States); Univ. of Connecticut, Storrs, CT (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)

Here, we report a combined experimental and theoretical study on the effect of autoionizing resonances in time-resolved photoelectron spectroscopy. The coherent excitation of N₂ by ~14.15 eV extreme-ultraviolet photons prepares a superposition of three dominant adjacent vibrational levels (v'=14–16) in the valence b' ¹$$Σ^+_u$$ state, which are probed by the absorption of two or three near-infrared photons (800 nm). The superposition manifests itself as coherent oscillations in the measured photoelectron spectra. A quantum-mechanical simulation confirms that two autoionizing Rydberg states converging to the excited A ²Π_u and B ²$$Σ^+_u$$ $$N^+_2$$ cores are accessed by the resonant absorption of near-infrared photons. We show that these resonances apply different filters to the observation of the vibrational wave packet, which results in different phases and amplitudes of the oscillating photoelectron signal depending on the nature of the autoionizing resonance. This work clarifies the importance of resonances in time-resolved photoelectron spectroscopy and particularly reveals the phase of vibrational quantum beats as a powerful observable for characterizing the properties of such resonances.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Connecticut, Storrs, CT (United States)

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

Grant/Contract Number:: SC0023192

OSTI ID:: 2422210

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 15 Vol. 130; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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