Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO2
Abstract
We report the results of ab initio calculations of cross sections and molecular-frame photoelectron angular distributions for C 1s ionization of CO2, and propose a mechanism for the recently observed asymmetry of those angular distributions with respect to the CO^+and O^+ions produced by subsequent Auger decay. The fixed-nuclei, photoionization amplitudes were constructed using variationally obtained electron-molecular ion scattering wave functions. We have also carried out electronic structure calculations which identify a dissociative state of the CO2^++ dication that is likely populated following Auger decay and which leads to O^+ + CO^+ fragment ions. We show that a proper accounting of vibrational motion in the computation of the photoelectron angular distributions, along with reasonable assumptions about the nuclear dissociation dynamics, gives results in good agreement with recent experimental observations. We also demonstrate that destructive interference between different partial waves accounts for sudden changes with photon energy in the observed angular distributions.
- Authors:
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- Chemical Sciences Division
- OSTI Identifier:
- 978867
- Report Number(s):
- LBNL-2822E
Journal ID: ISSN 1050-2947; PLRAAN; TRN: US1003042
- DOE Contract Number:
- DE-AC02-05CH11231
- Resource Type:
- Journal Article
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 79; Related Information: Journal Publication Date: 2009; Journal ID: ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74; AMPLITUDES; ANGULAR DISTRIBUTION; ASYMMETRY; CROSS SECTIONS; DECAY; DISSOCIATION; ELECTRONIC STRUCTURE; IONIZATION; PARTIAL WAVES; PHOTOIONIZATION; PHOTONS; SCATTERING; WAVE FUNCTIONS; CO2 Photoionization
Citation Formats
Rescigno, Thomas N, Miyabe, S, McCurdy, C W, and Orel, A E. Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO2. United States: N. p., 2009.
Web.
Rescigno, Thomas N, Miyabe, S, McCurdy, C W, & Orel, A E. Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO2. United States.
Rescigno, Thomas N, Miyabe, S, McCurdy, C W, and Orel, A E. 2009.
"Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO2". United States. https://www.osti.gov/servlets/purl/978867.
@article{osti_978867,
title = {Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1s photoejection from CO2},
author = {Rescigno, Thomas N and Miyabe, S and McCurdy, C W and Orel, A E},
abstractNote = {We report the results of ab initio calculations of cross sections and molecular-frame photoelectron angular distributions for C 1s ionization of CO2, and propose a mechanism for the recently observed asymmetry of those angular distributions with respect to the CO^+and O^+ions produced by subsequent Auger decay. The fixed-nuclei, photoionization amplitudes were constructed using variationally obtained electron-molecular ion scattering wave functions. We have also carried out electronic structure calculations which identify a dissociative state of the CO2^++ dication that is likely populated following Auger decay and which leads to O^+ + CO^+ fragment ions. We show that a proper accounting of vibrational motion in the computation of the photoelectron angular distributions, along with reasonable assumptions about the nuclear dissociation dynamics, gives results in good agreement with recent experimental observations. We also demonstrate that destructive interference between different partial waves accounts for sudden changes with photon energy in the observed angular distributions.},
doi = {},
url = {https://www.osti.gov/biblio/978867},
journal = {Physical Review A},
issn = {1050-2947},
number = ,
volume = 79,
place = {United States},
year = {Wed Feb 18 00:00:00 EST 2009},
month = {Wed Feb 18 00:00:00 EST 2009}
}