High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions
Abstract
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.
- Authors:
-
- Department of Chemistry, Brown University, Providence, USA
- Publication Date:
- Research Org.:
- Brown Univ., Providence, RI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1567913
- Alternate Identifier(s):
- OSTI ID: 1594597
- Grant/Contract Number:
- SC0018679
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 10 Journal Issue: 41; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhu, Guo-Zhu, and Wang, Lai-Sheng. High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9SC03861B.
Zhu, Guo-Zhu, & Wang, Lai-Sheng. High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions. United Kingdom. https://doi.org/10.1039/C9SC03861B
Zhu, Guo-Zhu, and Wang, Lai-Sheng. Thu .
"High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions". United Kingdom. https://doi.org/10.1039/C9SC03861B.
@article{osti_1567913,
title = {High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions},
author = {Zhu, Guo-Zhu and Wang, Lai-Sheng},
abstractNote = {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.},
doi = {10.1039/C9SC03861B},
journal = {Chemical Science},
number = 41,
volume = 10,
place = {United Kingdom},
year = {Thu Oct 24 00:00:00 EDT 2019},
month = {Thu Oct 24 00:00:00 EDT 2019}
}
https://doi.org/10.1039/C9SC03861B
Web of Science
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