Attosecond XUV probing of vibronic quantum superpositions in Br2+

Kobayashi, Yuki; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1103/physreva.102.051102

Title: Attosecond XUV probing of vibronic quantum superpositions in Br₂⁺

Journal Article · Fri Nov 13 00:00:00 EST 2020 · Physical Review A

DOI:https://doi.org/10.1103/physreva.102.051102· OSTI ID:1762196

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Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on a few femtosecond timescale. While recent attosecond experiments have addressed real-time observation of these primary photochemical processes, the underlying roles of simultaneous nuclear motions and how they modify and disturb the valence electronic motion remain uncertain. In this work, we investigate coherent electronic-vibrational dynamics induced among multiple vibronic levels of ionic bromine (Br₂⁺), including both spin-orbit (X²Π_3/2,g – X²Π_1/2,g) and valence (A²Π_3/2,u – ⁴Σ_3/2,u) electronic superpositions, using attosecond transient absorption spectroscopy. Decay, revival, and apparent frequency shifts of electronic coherences are measured via characteristic quantum beats on the Br-3d core-level absorption signals. Quantum-mechanical simulations attribute the observed electronic decoherence to broadened phase distributions of nuclear wave packets on anharmonic potentials. Molecular vibronic structure is further revealed to be imprinted as discrete progressions in electronic beat frequencies. These results provide a future basis to interpret complex charge-migration dynamics in polyatomic systems.

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

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF); US Army Research Office (ARO)

Grant/Contract Number:: AC02-05CH11231; CHE-1660417; CHE-1951317; W911NF-14-1-0383; W911NF-20-1-0127

OSTI ID:: 1762196

Journal Information:: Physical Review A, Vol. 102, Issue 5; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Attosecond XUV probing of vibronic quantum superpositions in Br₂⁺