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Title: Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide

Abstract

Auger electron spectra following excitation or ionization of the I 3d level in CH 3I have been recorded with horizontally or vertically plane polarized synchrotron radiation. These spectra have enabled the Auger electron angular distributions, as characterized by the β parameter, to be determined. The I 3d photoionization partial cross section of CH 3I has been calculated with the continuum multiple scattering approach, and the results show that in the photon energy range over which Auger spectra were measured, the I 3d cross section exhibits an atomic-like behavior and is dominated by transitions into the εf continuum channel. In this limit, the theoretical value of the alignment parameter (A 20) characterizing the core ionized state in an atom becomes constant, independent of photon energy. This theoretical value has been used to obtain the Auger electron intrinsic anisotropy parameters (α 2) from the β parameters extracted from our normal (non-resonant) molecular Auger spectra. The resulting anisotropy parameters for the M 45N 45N 45 transitions in CH 3I have been compared to those calculated for the corresponding transitions in xenon, and the experimental and theoretical results are in good agreement. Anisotropy parameters have also been measured for the M 45N 1N 45,more » M 45N 23N 45, and M 45N 45O 23 transitions. For the M 45N 1N 45 and M 45N 23N 45 Auger decays in CH 3I, the experimentally derived angular distributions do not exhibit the strong dependence on the final ionic state that is predicted for these transitions in xenon. Resonantly excited Auger spectra have been recorded at 620.4 and 632.0 eV, coinciding with the I 3d 5/2 → σ* and 3d 3/2 → σ* transitions, respectively. The resulting Auger electron angular distributions for the M 4N 45N 45 and M 5N 45N 45 decays were found to exhibit a higher anisotropy than those for the normal process. This is due to the larger photo-induced alignment in the neutral core excited state. For a particular Auger transition, the Auger electron kinetic energy measured in the resonantly excited spectrum is higher than that in the normal spectrum. This shift, due to the screening provided by the electron excited into the σ* orbital, has been rationalized by calculating orbital ionization energies of I 3d excited and I 3d ionized states in CH 3I.« less

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [6];  [7]; ORCiD logo [7];  [7];  [7];  [8];  [9]
  1. Department of Physics and Astronomy, University College London, Gower Street, London WC1E 6BT, United Kingdom; Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada
  2. European XFEL, GmbH, Holzkoppel 14, 22869 Schenefeld, Germany
  3. Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany
  4. J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, USA
  5. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, USA
  6. School of Chemistry, University of Nottingham, Nottingham NG7 2RD, United Kingdom
  7. Synchrotron SOLEIL, l’Orme des Merisiers, Saint-Aubin, BP 48, 91192 Gif-sur-Yvette, France
  8. Department of Physics and Astronomy, University College London, Gower Street, London WC1E 6BT, United Kingdom
  9. Daresbury Laboratory, Daresbury, Warrington, Cheshire WA4 4AD, United Kingdom
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; United Kingdom Science and Technology Facilities Council (STFC)
OSTI Identifier:
1477729
Alternate Identifier(s):
OSTI ID: 1468876
Grant/Contract Number:  
AC02-06CH11357; FG02-86ER1349; EP/N002148/1
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 149; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Forbes, Ruaridh, De Fanis, Alberto, Bomme, Cédric, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Nandi, Saikat, Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D., Underwood, Jonathan G., and Holland, David M. P. Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide. United States: N. p., 2018. Web. doi:10.1063/1.5045640.
Forbes, Ruaridh, De Fanis, Alberto, Bomme, Cédric, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Nandi, Saikat, Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D., Underwood, Jonathan G., & Holland, David M. P. Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide. United States. doi:10.1063/1.5045640.
Forbes, Ruaridh, De Fanis, Alberto, Bomme, Cédric, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Nandi, Saikat, Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D., Underwood, Jonathan G., and Holland, David M. P. Thu . "Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide". United States. doi:10.1063/1.5045640. https://www.osti.gov/servlets/purl/1477729.
@article{osti_1477729,
title = {Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide},
author = {Forbes, Ruaridh and De Fanis, Alberto and Bomme, Cédric and Rolles, Daniel and Pratt, Stephen T. and Powis, Ivan and Besley, Nicholas A. and Nandi, Saikat and Milosavljević, Aleksandar R. and Nicolas, Christophe and Bozek, John D. and Underwood, Jonathan G. and Holland, David M. P.},
abstractNote = {Auger electron spectra following excitation or ionization of the I 3d level in CH3I have been recorded with horizontally or vertically plane polarized synchrotron radiation. These spectra have enabled the Auger electron angular distributions, as characterized by the β parameter, to be determined. The I 3d photoionization partial cross section of CH3I has been calculated with the continuum multiple scattering approach, and the results show that in the photon energy range over which Auger spectra were measured, the I 3d cross section exhibits an atomic-like behavior and is dominated by transitions into the εf continuum channel. In this limit, the theoretical value of the alignment parameter (A20) characterizing the core ionized state in an atom becomes constant, independent of photon energy. This theoretical value has been used to obtain the Auger electron intrinsic anisotropy parameters (α2) from the β parameters extracted from our normal (non-resonant) molecular Auger spectra. The resulting anisotropy parameters for the M45N45N45 transitions in CH3I have been compared to those calculated for the corresponding transitions in xenon, and the experimental and theoretical results are in good agreement. Anisotropy parameters have also been measured for the M45N1N45, M45N23N45, and M45N45O23 transitions. For the M45N1N45 and M45N23N45 Auger decays in CH3I, the experimentally derived angular distributions do not exhibit the strong dependence on the final ionic state that is predicted for these transitions in xenon. Resonantly excited Auger spectra have been recorded at 620.4 and 632.0 eV, coinciding with the I 3d5/2 → σ* and 3d3/2 → σ* transitions, respectively. The resulting Auger electron angular distributions for the M4N45N45 and M5N45N45 decays were found to exhibit a higher anisotropy than those for the normal process. This is due to the larger photo-induced alignment in the neutral core excited state. For a particular Auger transition, the Auger electron kinetic energy measured in the resonantly excited spectrum is higher than that in the normal spectrum. This shift, due to the screening provided by the electron excited into the σ* orbital, has been rationalized by calculating orbital ionization energies of I 3d excited and I 3d ionized states in CH3I.},
doi = {10.1063/1.5045640},
journal = {Journal of Chemical Physics},
number = 9,
volume = 149,
place = {United States},
year = {2018},
month = {9}
}

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    Works referencing / citing this record:

    Effect of intermediate coupling on angular distribution of Auger electrons
    journal, February 1992


    Evolution of the anisotropy of the Auger decay of 2 p 3 / 2 1 ns resonances into anisotropy of L 3 MM Auger decay in Ar
    journal, October 1993


    Angle-resolved electron spectroscopy of the resonant Auger decay in xenon with meV energy resolution
    journal, July 2011


    Correlation effects in the M 4 , 5 N 4 , 5 O Auger spectra of Xe
    journal, August 1986


    Angular distribution in xenon M 4 , 5 N 4 , 5 N 4 , 5 Auger decay
    journal, January 1999


    The influence of the bromine atom Cooper minimum on the photoelectron angular distributions and branching ratios of the four outermost bands of bromobenzene
    journal, October 2015

    • Powis, I.; Holland, D. M. P.; Antonsson, E.
    • The Journal of Chemical Physics, Vol. 143, Issue 14
    • DOI: 10.1063/1.4931642

    A study of the photoionisation dynamics of chloromethane and iodomethane
    journal, August 2006


    Self-Consistent Field Calculations of Excited States Using the Maximum Overlap Method (MOM)
    journal, December 2008

    • Gilbert, Andrew T. B.; Besley, Nicholas A.; Gill, Peter M. W.
    • The Journal of Physical Chemistry A, Vol. 112, Issue 50
    • DOI: 10.1021/jp801738f

    The High Resolution L 2,3 MM and M 4,5 NN Auger Spectra from Krypton and M 4,5 NN and N 4,5 OO Auger Spectra from Xenon
    journal, August 1972


    Resolution and signal‐to‐background enhancement in gas‐phase electron spectroscopy
    journal, August 1993

    • Baltzer, P.; Karlsson, L.; Lundqvist, M.
    • Review of Scientific Instruments, Vol. 64, Issue 8
    • DOI: 10.1063/1.1143957

    On the angular distribution of Auger electrons
    journal, October 1971


    The effect of many-electron correlations on the angular distribution and spin polarisation of Auger electrons in Kr and Xe
    journal, November 1988

    • Kabachnik, N. M.; Sazhina, I. P.; Lee, I. S.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 21, Issue 22
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    Advances in molecular quantum chemistry contained in the Q-Chem 4 program package
    journal, September 2014


    Photoionization Decay of Core Excited Molecules
    journal, January 1987


    Auger decay of the dissociating core‐excited states in the HCl and DCl molecules
    journal, March 1996

    • Kukk, E.; Aksela, H.; Sairanen, O. ‐P.
    • The Journal of Chemical Physics, Vol. 104, Issue 12
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    Auger decay parameters α 2 for krypton M 4.5 -N 2.3 N 2.3 transitions
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    • DOI: 10.1016/0368-2048(94)02197-8

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    • Kabachnik, N. M.; Ueda, K.; Muramatsu, Y.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 31, Issue 21
    • DOI: 10.1088/0953-4075/31/21/011

    Auger resonant Raman studies of atoms and molecules
    journal, March 2000


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    journal, September 1996


    Femtosecond Dissociation of Core-Excited HCl Monitored by Frequency Detuning
    journal, October 1997


    Unusual degree of angular anisotropy in the resonant Auger spectrum of Kr
    journal, April 1988


    Vibrational and Vibronic Structure in the Valence Electron Spectra of CH 3 X Molecules (X=F, Cl, Br, I, OH)
    journal, November 1977


    Angular distribution parameters in the resonant xenon 4d−16p Auger spectra
    journal, September 1993


    Electron-spectroscopy study of inner-shell photoexcitation and ionization of Xe
    journal, July 1983


    M 4 , 5 N 4 , 5 X Auger electron spectra of iodine and xenon. Many-body effects
    journal, February 1979


    Lifetime Broadening and CI-Resonances Observed in ESCA
    journal, October 1976


    The resonant Auger effect
    journal, January 2000

    • Armen, G. Bradley; Aksela, Helena; Åberg, Teijo
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 33, Issue 2
    • DOI: 10.1088/0953-4075/33/2/201

    Calibration of a monochromator/spectrometer system for the measurement of photoelectron angular distributions and branching ratios
    journal, May 1986

    • Southworth, S. H.; Parr, A. C.; Hardis, J. E.
    • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 246, Issue 1-3
    • DOI: 10.1016/0168-9002(86)90192-0

    Spin-polarised Auger-electron spectroscopy of the d atomic shell. Model calculation for noble-gas atoms
    journal, January 1988

    • Kabachnik, N. M.; Sazhina, I. P.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 21, Issue 2
    • DOI: 10.1088/0953-4075/21/2/011

    Connection between the angular distribution of Auger electrons and spectator autoionization electrons following 4d ionization/excitation in xenon
    journal, December 1990

    • Kammerling, B.; Krassig, B.; Schmidt, V.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 23, Issue 24
    • DOI: 10.1088/0953-4075/23/24/009

    An unusual π* shape resonance in the near-threshold photoionization of S1 para -difluorobenzene
    journal, June 2005

    • Bellm, Susan M.; Davies, Julia A.; Whiteside, Paul T.
    • The Journal of Chemical Physics, Vol. 122, Issue 22
    • DOI: 10.1063/1.1927523

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    journal, June 1990


    Photoelectron and Auger electron asymmetries: Alignment of Xe + 2 D 5 2 by photoionization
    journal, October 1981


    Analysis of the angular distribution of Auger electrons in a Xe atom
    journal, October 2003

    • Elizarov, A. Yu.; Tupitsyn, I. I.
    • Journal of Experimental and Theoretical Physics, Vol. 97, Issue 4
    • DOI: 10.1134/1.1625056

    Self-consistent-field calculations of core excited states
    journal, March 2009

    • Besley, Nicholas A.; Gilbert, Andrew T. B.; Gill, Peter M. W.
    • The Journal of Chemical Physics, Vol. 130, Issue 12
    • DOI: 10.1063/1.3092928

    High-resolution inner-shell spectroscopies of free atoms and molecules using soft-x-ray beamlines at the third-generation synchrotron radiation sources
    journal, February 2003


    The plane grating and elliptical mirror: A new optical configuration for monochromators
    journal, February 1982


    Ultrafast dissociation: An unexpected tool for probing molecular dynamics
    journal, September 2012


    Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields
    journal, November 1994

    • Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.
    • The Journal of Physical Chemistry, Vol. 98, Issue 45, p. 11623-11627
    • DOI: 10.1021/j100096a001

    High resolution measurement for the resonant Auger emission of Xe following 3d 5/2 →6p excitation
    journal, May 2001

    • Fanis, A. De; Saito, N.; Kitajima, M.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 34, Issue 11
    • DOI: 10.1088/0953-4075/34/11/103

    An investigation of dissociative resonant photoionization in HCl and DCl using two-dimensional photoelectron spectroscopy
    journal, May 2005

    • Sokell, E.; Wills, A. A.; Wiedenhoeft, M.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 38, Issue 10
    • DOI: 10.1088/0953-4075/38/10/011

    Theoretical study of inner-shell alignment of atoms in electron impact ionisation: angular distribution and polarisation of X-rays and Auger electrons
    journal, August 1977

    • Berezhko, E. G.; Kabachnik, N. M.
    • Journal of Physics B: Atomic and Molecular Physics, Vol. 10, Issue 12
    • DOI: 10.1088/0022-3700/10/12/025

    Spin–orbit effects, electronic decay and breakdown phenomena in the photoelectron spectra of iodomethane
    journal, October 2012


    Angular distribution of ejected electrons in resonant Auger processes of Ar, Kr, and Xe
    journal, February 1989

    • Carlson, Thomas A.; Mullins, David R.; Beall, Charles E.
    • Physical Review A, Vol. 39, Issue 3
    • DOI: 10.1103/physreva.39.1170

    Angular distribution in resonant Auger decay
    journal, November 1991

    • Hergenhahn, U.; Kabachnik, N. M.; Lohmann, B.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 24, Issue 22
    • DOI: 10.1088/0953-4075/24/22/013

    Angular Distribution of Auger Electrons Following Photoionization
    journal, July 1972


    Soft x-ray photoionization of atoms and molecules
    journal, April 2005


    Angular distribution in resonant Auger spectra of xenon excited below the 3 d 5 / 2 ionization threshold
    journal, February 2001


    Atomic Autoionization Following Very Fast Dissociation of Core-Excited HBr
    journal, May 1986


    Auger electron angular distributions following excitation or ionization of the I 3d level in methyl iodide
    text, January 2018

    • Forbes, Ruaridh; De Fanis, Alberto; Bomme, Cedric
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-00089

    Angular Distribution of Molecular K -Shell Auger Electrons: Spectroscopy of Photoabsorption Anisotropy
    journal, October 1980


    Angular distribution of electronic decay following molecular and Rydberg excitations at the Cl 2 p edge of HCl
    journal, April 1998