DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Photoelectron angular distributions from rotationally resolved autoionizing states of N2

Abstract

The single-photon, photoelectron-photoion coincidence spectrum of N2 has been recorded at high (~1.5 cm-1) resolution in the region between the N2+ X 2Σg+, v+ = 0 and 1 ionization thresholds by using a double imaging spectrometer and intense vacuum-ultraviolet light from the Synchrotron SOLEIL. This approach provides the relative photoionization cross section, the photoelectron energy distribution, and the photoelectron angular distribution as a function of photon energy. The region of interest contains autoionizing valence states, vibrationally autoionizing Rydberg states converging to vibrationally excited levels of the N2+ X 2Σg+ ground state, and electronically autoionizing states converging to the N2+ A 2Π and B 2Σu+ states. The wavelength resolution is sufficient to resolve rotational structure in the autoionizing states, but the electron energy resolution is insufficient to resolve rotational structure in the photoion spectrum. Here, a simplified approach based on multichannel quantum defect theory is used to predict the photoelectron angular distribution parameters, β, and the results are in reasonably good agreement with experiment.

Authors:
 [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5];  [6]; ORCiD logo [7];  [7];  [8]
  1. Bryn Mawr College, Bryn Mawr, PA (United States)
  2. Bryn Mawr College, Bryn Mawr, PA (United States); Bowdoin College , Brunswick, ME (United States)
  3. ETH Zurich, Zurich (Switzerland)
  4. Daresbury Lab., Cheshire (United Kingdom)
  5. Univ. Paris-Sud, Univ. Paris-Saclay, Orsay (France)
  6. Synchrotron Soleil, Gif-sur-Yvette (France); Chinese Academy of Sciences, Anhui (China)
  7. Synchrotron Soleil, Gif-sur-Yvette (France)
  8. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1422406
Alternate Identifier(s):
OSTI ID: 1411991
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; Photoionization; Photoelectron Spectroscopy; Photoelectron Angular Distributions

Citation Formats

Chartrand, A. M., McCormack, E. F., Jacovella, U., Holland, D. M. P., Gans, Berenger, Tang, Xiaofeng, Garcia, G. A., Nahon, L., and Pratt, S. T. Photoelectron angular distributions from rotationally resolved autoionizing states of N2. United States: N. p., 2017. Web. doi:10.1063/1.5004538.
Chartrand, A. M., McCormack, E. F., Jacovella, U., Holland, D. M. P., Gans, Berenger, Tang, Xiaofeng, Garcia, G. A., Nahon, L., & Pratt, S. T. Photoelectron angular distributions from rotationally resolved autoionizing states of N2. United States. https://doi.org/10.1063/1.5004538
Chartrand, A. M., McCormack, E. F., Jacovella, U., Holland, D. M. P., Gans, Berenger, Tang, Xiaofeng, Garcia, G. A., Nahon, L., and Pratt, S. T. Fri . "Photoelectron angular distributions from rotationally resolved autoionizing states of N2". United States. https://doi.org/10.1063/1.5004538. https://www.osti.gov/servlets/purl/1422406.
@article{osti_1422406,
title = {Photoelectron angular distributions from rotationally resolved autoionizing states of N2},
author = {Chartrand, A. M. and McCormack, E. F. and Jacovella, U. and Holland, D. M. P. and Gans, Berenger and Tang, Xiaofeng and Garcia, G. A. and Nahon, L. and Pratt, S. T.},
abstractNote = {The single-photon, photoelectron-photoion coincidence spectrum of N2 has been recorded at high (~1.5 cm-1) resolution in the region between the N2+ X 2Σg+, v+ = 0 and 1 ionization thresholds by using a double imaging spectrometer and intense vacuum-ultraviolet light from the Synchrotron SOLEIL. This approach provides the relative photoionization cross section, the photoelectron energy distribution, and the photoelectron angular distribution as a function of photon energy. The region of interest contains autoionizing valence states, vibrationally autoionizing Rydberg states converging to vibrationally excited levels of the N2+ X 2Σg+ ground state, and electronically autoionizing states converging to the N2+ A 2Π and B 2Σu+ states. The wavelength resolution is sufficient to resolve rotational structure in the autoionizing states, but the electron energy resolution is insufficient to resolve rotational structure in the photoion spectrum. Here, a simplified approach based on multichannel quantum defect theory is used to predict the photoelectron angular distribution parameters, β, and the results are in reasonably good agreement with experiment.},
doi = {10.1063/1.5004538},
journal = {Journal of Chemical Physics},
number = 22,
volume = 147,
place = {United States},
year = {Fri Dec 08 00:00:00 EST 2017},
month = {Fri Dec 08 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Uncovering multiple orbitals influence in high harmonic generation from aligned N 2
journal, October 2009

  • Le, Anh-Thu; Lucchese, R. R.; Lin, C. D.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 42, Issue 21
  • DOI: 10.1088/0953-4075/42/21/211001

Ab initio approach to the multichannel quantum defect calculation of the electronic autoionisation in the Hopfield series of N 2
journal, December 1983

  • Raoult, M.; Rouzo, H. Le; Raseev, G.
  • Journal of Physics B: Atomic and Molecular Physics, Vol. 16, Issue 24
  • DOI: 10.1088/0022-3700/16/24/016

Partial-Wave Decomposition of the Ionization Continuum Accessed by Vibrational Autoionization of the NO 14 s ( ν = 1 , N = 20 , N R + = 20 ) Level
journal, April 2000


On the rotational structure of a prominent band in the vacuum-ultraviolet spectrum of molecular nitrogen
journal, March 2006


Analysis of the 8 f , 9 f , and 10 f , v =1 Rydberg states of N 2
journal, September 1991


Rydberg-state-resolved zero-kinetic-energy photoelectron spectroscopy
journal, October 2001


The f Rydberg series in the absorption spectrum of N 2
journal, June 1994

  • Huber, K. P.; Jungen, Ch.; Yoshino, K.
  • The Journal of Chemical Physics, Vol. 100, Issue 11
  • DOI: 10.1063/1.466841

Near-threshold photoionisation studies of N 2
journal, November 1988

  • Zubek, M.; King, G. C.; Rutter, P. M.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 21, Issue 21
  • DOI: 10.1088/0953-4075/21/21/014

Angular Distributions of Photoelectrons from H 2 : Effects of Rotational Autoionization
journal, July 1972


DESIRS: a state-of-the-art VUV beamline featuring high resolution and variable polarization for spectroscopy and dichroism at SOLEIL
journal, May 2012

  • Nahon, Laurent; de Oliveira, Nelson; Garcia, Gustavo A.
  • Journal of Synchrotron Radiation, Vol. 19, Issue 4
  • DOI: 10.1107/s0909049512010588

Angular Momentum Transfer in the Theory of Angular Distributions
journal, July 1972


The effect of autoionization on the N 2 + X 2 Σ g + state vibrationally resolved photoelectron anisotropy parameters and branching ratios
journal, April 2013

  • Holland, D. M. P.; Seddon, E. A.; Daly, S.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 9
  • DOI: 10.1088/0953-4075/46/9/095102

Assignment in the near-threshold absorption spectrum of N2
journal, April 2005

  • Lefebvre-Brion, Hélène
  • The Journal of Chemical Physics, Vol. 122, Issue 14
  • DOI: 10.1063/1.1876232

High-resolution laser absorption spectroscopy in the extreme ultraviolet
journal, September 2002

  • Sommavilla, M.; Hollenstein, U.; Greetham, G. M.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 35, Issue 18
  • DOI: 10.1088/0953-4075/35/18/309

High‐resolution jet absorption study of nitrogen near 800 Å
journal, January 1990

  • Huber, K. P.; Jungen, Ch.
  • The Journal of Chemical Physics, Vol. 92, Issue 2
  • DOI: 10.1063/1.458589

Double-resonance spectroscopy of a complex resonance in molecular nitrogen
journal, April 1992


Double-resonance spectroscopy of autoionizing states of N 2 near the ionization threshold
journal, November 1990


Two-dimensional charged particle image inversion using a polar basis function expansion
journal, November 2004

  • Garcia, Gustavo A.; Nahon, Laurent; Powis, Ivan
  • Review of Scientific Instruments, Vol. 75, Issue 11
  • DOI: 10.1063/1.1807578

Studies of differential and total photoionization cross sections of molecular nitrogen
journal, May 1982

  • Lucchese, Robert R.; Raseev, Georges; McKoy, Vincent
  • Physical Review A, Vol. 25, Issue 5
  • DOI: 10.1103/physreva.25.2572

Rotational Branching Ratios in N 2 + : Observation of Photon Energy Dependence by Photoelectron Spectroscopy
journal, July 1998


DELICIOUS III: A multipurpose double imaging particle coincidence spectrometer for gas phase vacuum ultraviolet photodynamics studies
journal, May 2013

  • Garcia, G. A.; Cunha de Miranda, B. K.; Tia, M.
  • Review of Scientific Instruments, Vol. 84, Issue 5
  • DOI: 10.1063/1.4807751

Photoelectron study of electronic autoionization in rotationally cooled N 2 : the n=6 member of the Hopfield series
journal, September 1993

  • Ueda, K.; West, J. B.; Hayes, M. A.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 26, Issue 18
  • DOI: 10.1088/0953-4075/26/18/005

The ‘cathedral’ in the near-threshold absorption spectrum of N2
journal, June 2005


Complete dipole oscillator strength distribution and its moments for N 2
journal, February 1985

  • Kosman, Warren M.; Wallace, Scott
  • The Journal of Chemical Physics, Vol. 82, Issue 3
  • DOI: 10.1063/1.448461

Vacuum upgrade and enhanced performances of the double imaging electron/ion coincidence end-station at the vacuum ultraviolet beamline DESIRS
journal, December 2015

  • Tang, Xiaofeng; Garcia, Gustavo A.; Gil, Jean-François
  • Review of Scientific Instruments, Vol. 86, Issue 12
  • DOI: 10.1063/1.4937624

Channel coupling and shape resonance effects in the photoelectron angular distributions of the 3 σ g 1 and 2 σ u 1 channels of N 2
journal, February 1986


Vibrationally resolved photoionization of N 2 near threshold
journal, March 2012

  • O’Keeffe, P.; Bolognesi, P.; Moise, A.
  • The Journal of Chemical Physics, Vol. 136, Issue 10
  • DOI: 10.1063/1.3692687

Photoionization of N 2 X1 Σ + g , v ″=0 and 1 near threshold. Preionization of the Worley–Jenkins Rydberg series
journal, February 1984

  • Dehmer, P. M.; Miller, P. J.; Chupka, W. A.
  • The Journal of Chemical Physics, Vol. 80, Issue 3
  • DOI: 10.1063/1.446829

Tomographic imaging of molecular orbitals
journal, December 2004


The effect of autoionising Rydberg states on the formation of low energy electrons
journal, April 2011

  • Holland, D. M. P.; Shaw, D. A.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 184, Issue 3-6
  • DOI: 10.1016/j.elspec.2010.12.006

P HOTOELECTRON A NGULAR D ISTRIBUTIONS
journal, October 2003


Isotope effects and spectroscopic assignments in the non-dissociative photoionization spectrum of N 2
journal, May 2014

  • Randazzo, John B.; Croteau, Philip; Kostko, Oleg
  • The Journal of Chemical Physics, Vol. 140, Issue 19
  • DOI: 10.1063/1.4873717

Autoionization of nonpenetrating Rydberg states in diatomic molecules
journal, October 1986


The near-threshold absorption spectrum of N2
journal, March 2003

  • Jungen, Ch.; Huber, K. P.; Jungen, M.
  • The Journal of Chemical Physics, Vol. 118, Issue 10
  • DOI: 10.1063/1.1542877

A high resolution angle resolved photoelectron spectroscopy study of N 2
journal, April 1990


Works referencing / citing this record:

Photoionization studies of reactive intermediates using synchrotron radiation
journal, January 2019

  • Dyke, John M.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 18
  • DOI: 10.1039/c9cp00623k

Double-resonance studies of electronically autoionizing states of molecular nitrogen
journal, January 2019