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Title: Unambiguous observation of F-atom core-hole localization in CF 4 through body-frame photoelectron angular distributions

Abstract

A dramatic symmetry breaking in K-shell photoionization of the CF 4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. In observing the photoejected electron in coincidence with an F + atomic ion after Auger decay we see how selecting the dissociation path where the core hole was localized was almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF 3 + and F + atoms elucidates the underlying physics that derives from the Ne-like valence structure of the F(1s -1) core-excited atom.

Authors:
 [1];  [2];  [3];  [4];  [2];  [5];  [6];  [7];  [5];  [8];  [6];  [6];  [9];  [9];  [10];  [3];  [6];  [10];  [11];  [9] more »;  [6];  [2];  [2] « less
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Davis, CA (United States). Dept. of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  3. California State Univ. (CalState), Vallejo, CA (United States). Dept. of Sciences and Mathematics
  4. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Goethe Univ., Frankfurt (Germany). Inst. of Nuclear Physics
  6. Goethe Univ., Frankfurt (Germany). Inst. of Nuclear Physics
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Auburn Univ., AL (United States). Dept. of Physics
  8. Technical Univ. of Berlin (Germany). Inst. of Optics and Atomic Physics
  9. Kansas State Univ., Manhattan, KS (United States). Physics Dept.
  10. Auburn Univ., AL (United States). Dept. of Physics
  11. Univ. of Nevada, Reno, NV (United States). Dept. of Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1379684
Alternate Identifier(s):
OSTI ID: 1339764
Grant/Contract Number:  
AC02-05CH11231; SC0012198; FG02-86ER13491
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 95; Journal Issue: 1; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., Schöffler, M. S., Gatton, A., Neff, J., Stammer, P. M., Rist, J., Eckart, S., Berry, B., Severt, T., Sartor, J., Moradmand, A., Jahnke, T., Landers, A. L., Williams, J. B., Ben-Itzhak, I., Dörner, R., Belkacem, A., and Weber, Th. Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions. United States: N. p., 2017. Web. doi:10.1103/PhysRevA.95.011401.
McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., Schöffler, M. S., Gatton, A., Neff, J., Stammer, P. M., Rist, J., Eckart, S., Berry, B., Severt, T., Sartor, J., Moradmand, A., Jahnke, T., Landers, A. L., Williams, J. B., Ben-Itzhak, I., Dörner, R., Belkacem, A., & Weber, Th. Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions. United States. doi:10.1103/PhysRevA.95.011401.
McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., Schöffler, M. S., Gatton, A., Neff, J., Stammer, P. M., Rist, J., Eckart, S., Berry, B., Severt, T., Sartor, J., Moradmand, A., Jahnke, T., Landers, A. L., Williams, J. B., Ben-Itzhak, I., Dörner, R., Belkacem, A., and Weber, Th. Tue . "Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions". United States. doi:10.1103/PhysRevA.95.011401. https://www.osti.gov/servlets/purl/1379684.
@article{osti_1379684,
title = {Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions},
author = {McCurdy, C. W. and Rescigno, T. N. and Trevisan, C. S. and Lucchese, R. R. and Gaire, B. and Menssen, A. and Schöffler, M. S. and Gatton, A. and Neff, J. and Stammer, P. M. and Rist, J. and Eckart, S. and Berry, B. and Severt, T. and Sartor, J. and Moradmand, A. and Jahnke, T. and Landers, A. L. and Williams, J. B. and Ben-Itzhak, I. and Dörner, R. and Belkacem, A. and Weber, Th.},
abstractNote = {A dramatic symmetry breaking in K-shell photoionization of the CF4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. In observing the photoejected electron in coincidence with an F+ atomic ion after Auger decay we see how selecting the dissociation path where the core hole was localized was almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF3+ and F+ atoms elucidates the underlying physics that derives from the Ne-like valence structure of the F(1s-1) core-excited atom.},
doi = {10.1103/PhysRevA.95.011401},
journal = {Physical Review A},
number = 1,
volume = 95,
place = {United States},
year = {Tue Jan 17 00:00:00 EST 2017},
month = {Tue Jan 17 00:00:00 EST 2017}
}

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