Photoionization of the I 4d and valence orbitals of methyl iodide
Abstract
Here, the photoabsorption and photoionization dynamics of the I 4d and valence orbitals in methyl iodide have been studied both experimentally and theoretically. Synchrotron radiation has been employed to measure the total ion yield in the vicinity of the I 4d ionization thresholds. The observed structure, due to excitations into Rydberg or valence states, has been assigned using transition energies and relative intensities computed with time-dependent density functional theory within the Tamm–Dancoff approximation. Photoelectron spectra, recorded with plane polarized radiation in two polarization geometries, have allowed the effect of autoionization on the valence electron angular distributions to be investigated. The spectra obtained at photon energies of 50.62 and 52.34 eV, coinciding respectively with the I 4d5/2 → σ* and 4d3/2 → σ* transitions, reveal, in addition to valence shell photoelectron bands, features not associated with simple photoionization of the parent molecule. High resolution photoelectron spectra of the I 4d main-lines display structure resulting from spin–orbit coupling and molecular field splitting. The binding energies of the five states contributing to the (I 4d)-1 ionization have been determined. The iodine (in CH3I) N45VV Auger spectrum has been measured and the observed structure has been assigned using the core hole binding energies derivedmore »
- Authors:
-
- Univ. of College London (United Kingdom); Univ. of Ottawa, ON (Canada); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- European XFEL, Schenefeld (Germany)
- Kansas State Univ., Manhattan, KS (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Nottingham (United Kingdom)
- Synchrotron SOLEIL, Gif-sur-Yvette (France)
- Daresbury Lab., Cheshire (United Kingdom)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Engineering and Physical Sciences Research Council (EPSRC); Science and Technology Facilities Council (STFC)
- OSTI Identifier:
- 1646792
- Alternate Identifier(s):
- OSTI ID: 1660713
- Grant/Contract Number:
- AC02-76SF00515; AC02-06CH11357; FG02-86ER13491; EP/N002148/1
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Journal of Physics. B, Atomic, Molecular and Optical Physics
- Additional Journal Information:
- Journal Volume: 53; Journal Issue: 15; Journal ID: ISSN 0953-4075
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; photoionization; spin-orbit coupling; Auger electron; Rydberg and valence states
Citation Formats
Forbes, Ruaridh, De Fanis, Alberto, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D, and Holland, David M. P. Photoionization of the I 4d and valence orbitals of methyl iodide. United States: N. p., 2020.
Web. doi:10.1088/1361-6455/ab8c5a.
Forbes, Ruaridh, De Fanis, Alberto, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D, & Holland, David M. P. Photoionization of the I 4d and valence orbitals of methyl iodide. United States. https://doi.org/10.1088/1361-6455/ab8c5a
Forbes, Ruaridh, De Fanis, Alberto, Rolles, Daniel, Pratt, Stephen T., Powis, Ivan, Besley, Nicholas A., Milosavljević, Aleksandar R., Nicolas, Christophe, Bozek, John D, and Holland, David M. P. 2020.
"Photoionization of the I 4d and valence orbitals of methyl iodide". United States. https://doi.org/10.1088/1361-6455/ab8c5a. https://www.osti.gov/servlets/purl/1646792.
@article{osti_1646792,
title = {Photoionization of the I 4d and valence orbitals of methyl iodide},
author = {Forbes, Ruaridh and De Fanis, Alberto and Rolles, Daniel and Pratt, Stephen T. and Powis, Ivan and Besley, Nicholas A. and Milosavljević, Aleksandar R. and Nicolas, Christophe and Bozek, John D and Holland, David M. P.},
abstractNote = {Here, the photoabsorption and photoionization dynamics of the I 4d and valence orbitals in methyl iodide have been studied both experimentally and theoretically. Synchrotron radiation has been employed to measure the total ion yield in the vicinity of the I 4d ionization thresholds. The observed structure, due to excitations into Rydberg or valence states, has been assigned using transition energies and relative intensities computed with time-dependent density functional theory within the Tamm–Dancoff approximation. Photoelectron spectra, recorded with plane polarized radiation in two polarization geometries, have allowed the effect of autoionization on the valence electron angular distributions to be investigated. The spectra obtained at photon energies of 50.62 and 52.34 eV, coinciding respectively with the I 4d5/2 → σ* and 4d3/2 → σ* transitions, reveal, in addition to valence shell photoelectron bands, features not associated with simple photoionization of the parent molecule. High resolution photoelectron spectra of the I 4d main-lines display structure resulting from spin–orbit coupling and molecular field splitting. The binding energies of the five states contributing to the (I 4d)-1 ionization have been determined. The iodine (in CH3I) N45VV Auger spectrum has been measured and the observed structure has been assigned using the core hole binding energies derived in the present work together with established ionization energies of the doubly charged ion. The experimentally determined Auger electron angular distributions have been discussed in relation to the theoretical angular distribution parameter characterizing the spatial alignment of molecular axes in the (I 4d)-1 state.},
doi = {10.1088/1361-6455/ab8c5a},
url = {https://www.osti.gov/biblio/1646792},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
issn = {0953-4075},
number = 15,
volume = 53,
place = {United States},
year = {Thu Jun 25 00:00:00 EDT 2020},
month = {Thu Jun 25 00:00:00 EDT 2020}
}
Web of Science
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