High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions

Zhu, Guo-Zhu; Wang, Lai-Sheng

doi:10.1039/C9SC03861B

Title: High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions

Journal Article · Thu Oct 24 00:00:00 EDT 2019 · Chemical Science

DOI:https://doi.org/10.1039/C9SC03861B· OSTI ID:1567913

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Department of Chemistry, Brown University, Providence, USA

Valence-bound anions with polar neutral cores (μ > ~2.5 D) can support dipole-bound excited states below the detachment threshold. These dipole-bound states (DBSs) are highly diffuse and the weakly bound electron in the DBS can be readily autodetached via vibronic coupling. Excited DBSs can be observed in photodetachment spectroscopy using a tunable laser. Tuning the detachment laser to above-threshold vibrational resonances yields vibrationally enhanced resonant photoelectron spectra, which are highly non-Franck–Condon with much richer vibrational information. This perspective describes recent advances in the studies of excited DBSs of cryogenically cooled anions using high-resolution photoelectron imaging (PEI) and resonant photoelectron spectroscopy (rPES). The basic features of dipole-bound excited states and highly non-Franck–Condon resonant photoelectron spectra will be discussed. The power of rPES to yield rich vibrational information beyond conventional PES will be highlighted, especially for low-frequency and Franck–Condon-inactive vibrational modes, which are otherwise not accessible from non-resonant conventional PES. Mode-selectivity and intra-molecular rescattering have been observed during the vibrationally induced autodetachment. Conformer-specific rPES is possible due to the different dipole-bound excited states of molecular conformers with polar neutral cores. For molecules with μ $$\ll$$ 2.5 D or without dipole moments, but large quadrupole moments, excited quadrupole-bound states can exist, which can also be used to conduct rPES.

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Research Organization:: Brown Univ., Providence, RI (United States)

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

Grant/Contract Number:: SC0018679

OSTI ID:: 1567913

Alternate ID(s):: OSTI ID: 1594597

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 10 Journal Issue: 41; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 39 works

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Zhu, Guo-Zhu; Qian, Chen-Hui; Wang, Lai-Sheng

Observation of a dipole-bound excited state in 4-ethynylphenoxide and comparison with the quadrupole-bound excited state in the isoelectronic 4-cyanophenoxide

Journal Article · Thu Sep 23 00:00:00 EDT 2021 · Journal of Chemical Physics · OSTI ID:1567913

Zhang, Yue-Rou; Yuan, Dao-Fu; Qian, Chen-Hui; +1 more

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions

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