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Title: 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:
ORCiD logo [1]; ORCiD logo [1]
  1. 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) (SC-22). Chemical Sciences, Geosciences & 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. doi: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. doi: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 = {2019},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1039/C9SC03861B

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Cited by: 9 works
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  • Physical Chemistry Chemical Physics, Vol. 13, Issue 38
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A velocity map imaging mass spectrometer for photofragments of fast ion beams
journal, January 2018

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Resonant photoelectron imaging of deprotonated uracil anion via vibrational levels of a dipole-bound excited state
journal, January 2017


The Capture of Negative Mesotrons in Matter
journal, September 1947


A Drude-model approach to dispersion interactions in dipole-bound anions
journal, June 2001

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Resonant Two-Photon Photoelectron Imaging and Intersystem Crossing from Excited Dipole-Bound States of Cold Anions
journal, July 2019

  • Zhu, Guo-Zhu; Cheung, Ling Fung; Liu, Yuan
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 15
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Ultrafast dynamics of low-energy electron attachment via a non-valence correlation-bound state
journal, January 2018

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