Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions

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.

doi:10.1103/PhysRevA.95.011401

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 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.

Authors:

McCurdy, C. W. ^[1]; Rescigno, T. N. ^[2]; Trevisan, C. S. ^[3]; Lucchese, R. R. ^[4]; Gaire, B. ^[2]; Menssen, A. ^[5]; Schöffler, M. S. ^[6]; Gatton, A. ^[7]; Neff, J. ^[5]; Stammer, P. M. ^[8]; Rist, J. ^[6]; Eckart, S. ^[6]; Berry, B. ^[9]; Severt, T. ^[9]; Sartor, J. ^[10]; Moradmand, A. ^[3]; Jahnke, T. ^[6]; Landers, A. L. ^[10]; Williams, J. B. ^[11]; Ben-Itzhak, I. ^[9] more »

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Davis, CA (United States). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
California State Univ. (CalState), Vallejo, CA (United States). Dept. of Sciences and Mathematics
Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Goethe Univ., Frankfurt (Germany). Inst. of Nuclear Physics
Goethe Univ., Frankfurt (Germany). Inst. of Nuclear Physics
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Auburn Univ., AL (United States). Dept. of Physics
Technical Univ. of Berlin (Germany). Inst. of Optics and Atomic Physics
Kansas State Univ., Manhattan, KS (United States). Physics Dept.
Auburn Univ., AL (United States). Dept. of Physics
Univ. of Nevada, Reno, NV (United States). Dept. of Physics

Publication Date:: Tue Jan 17 00:00:00 EST 2017

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1379684

Alternate Identifier(s):: OSTI ID: 1339764

Grant/Contract Number:: AC02-05CH11231; SC0012198; FG02-86ER13491

Resource Type:: 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.

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                    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.  https://doi.org/10.1103/PhysRevA.95.011401

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                    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.  https://doi.org/10.1103/PhysRevA.95.011401.  https://www.osti.gov/servlets/purl/1379684.

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@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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Works referencing / citing this record:

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

Abstract

Citation Formats

Multicoincidence studies of photo and Auger electrons from fixed-in-space molecules using the COLTRIMS technique journal, December 2004

Fluorine core esca linewidths in CH3F and CF4 journal, May 1978

The double photoionization/fragmentation of CF 4 in the threshold region (35-80 eV) journal, March 1991

Breakdown of the Two-Step Model in K -Shell Photoemission and Subsequent Decay Probed by the Molecular-Frame Photoelectron Angular Distributions of CO 2 journal, August 2008

Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics journal, June 2000

Asymmetry in the molecular-frame photoelectron angular distribution for oxygen 1s photoemission from CO 2 journal, September 2012

Role of symmetry restrictions on valence electron binding energies of CF 4 journal, February 1980

Electron spectroscopy observation of the 1s2s22p6(2S) state in atomic fluorine by means of electron impact excitation of the hf molecule journal, January 1990

Theoretical study of electron-impact excitation of N 2 + journal, November 1990

Molecular frame photoelectron angular distributions for core ionization of ethane, carbon tetrafluoride and 1,1-difluoroethylene journal, February 2016

Doubly ionized states of carbon tetrafluoride journal, June 1993

The fragmentation of core ionized CF 4 probed by threshold-photoelectron-photoion-photoion coincidence (TPEPIPICO) spectroscopy journal, January 1999

Changes in molecular KLL Auger spectrum of fluorine on going from HF to LiF, NaF, and KF journal, December 1993

Conformational and nuclear dynamics effects in molecular Auger spectra: fluorine core-hole decay in CF 4 journal, June 2014

The Auger spectra of CF 4 in the light of foreign imaging journal, June 1996

Vibronic coupling and symmetry breaking in core electron ionization journal, October 1977

Interchannel coupling and ground state correlation effects in the photoionization of CO journal, October 1993

Vibronic coupling in the K shell excitation of ethyne journal, October 1997

Theoretical study of asymmetric molecular-frame photoelectron angular distributions for C 1 s photoejection from CO 2 journal, May 2009

Recoil-ion and electron momentum spectroscopy: reaction-microscopes journal, August 2003

Imaging molecular isomerization using molecular-frame photoelectron angular distributions journal, September 2012

Ultrafast Probing of Core Hole Localization in N2 journal, May 2008

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Vibronic coupling and core-hole localization in K -shell excitations of ethylene journal, February 1991

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Ab initio calculation of transition rates for autoionization: the Auger spectra of HF and F− journal, November 1995

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

Multicoincidence studies of photo and Auger electrons from fixed-in-space molecules using the COLTRIMS technique
journal, December 2004

Fluorine core esca linewidths in CH3F and CF4
journal, May 1978

The double photoionization/fragmentation of CF ₄ in the threshold region (35-80 eV)
journal, March 1991

Breakdown of the Two-Step Model in $K$ -Shell Photoemission and Subsequent Decay Probed by the Molecular-Frame Photoelectron Angular Distributions of ${CO}_{2}$
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Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics
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Asymmetry in the molecular-frame photoelectron angular distribution for oxygen 1s photoemission from CO ₂
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Role of symmetry restrictions on valence electron binding energies of CF ₄
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Electron spectroscopy observation of the 1s2s22p6(2S) state in atomic fluorine by means of electron impact excitation of the hf molecule
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Theoretical study of electron-impact excitation of $N_{2}^{+}$
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Molecular frame photoelectron angular distributions for core ionization of ethane, carbon tetrafluoride and 1,1-difluoroethylene
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Doubly ionized states of carbon tetrafluoride
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The fragmentation of core ionized CF ₄ probed by threshold-photoelectron-photoion-photoion coincidence (TPEPIPICO) spectroscopy
journal, January 1999

Changes in molecular KLL Auger spectrum of fluorine on going from HF to LiF, NaF, and KF
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Interchannel coupling and ground state correlation effects in the photoionization of CO
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