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

Journal Article · Tue Jan 17 00:00:00 EST 2017 · Physical Review A

DOI:https://doi.org/10.1103/PhysRevA.95.011401· OSTI ID:1379684

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

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.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

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

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

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

OSTI ID:: 1379684

Alternate ID(s):: OSTI ID: 1339764

Journal Information:: Physical Review A, Vol. 95, Issue 1; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 13 works

Citation information provided by
Web of Science

References (26)

Multicoincidence studies of photo and Auger electrons from fixed-in-space molecules using the COLTRIMS technique Jahnke, T.; Weber, Th.; Osipov, T. Journal of Electron Spectroscopy and Related Phenomena, Vol. 141, Issue 2-3 https://doi.org/10.1016/j.elspec.2004.06.010	journal	December 2004
Fluorine core esca linewidths in CH3F and CF4 Goscinski, Osvaldo; Müller, Jiri; Poulain, Enrique Chemical Physics Letters, Vol. 55, Issue 3 https://doi.org/10.1016/0009-2614(78)84002-0	journal	May 1978
The double photoionization/fragmentation of CF ₄ in the threshold region (35-80 eV) Codling, K.; Frasinski, L. J.; Hatherly, P. A. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 24, Issue 5 https://doi.org/10.1088/0953-4075/24/5/018	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 ${CO}_{2}$ Liu, X. -J.; Fukuzawa, H.; Teranishi, T. Physical Review Letters, Vol. 101, Issue 8 https://doi.org/10.1103/PhysRevLett.101.083001	journal	August 2008
Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics Dörner, R.; Mergel, V.; Jagutzki, O. Physics Reports, Vol. 330, Issue 2-3 https://doi.org/10.1016/S0370-1573(99)00109-X	journal	June 2000
Asymmetry in the molecular-frame photoelectron angular distribution for oxygen 1s photoemission from CO ₂ Lucchese, R. R.; Fukuzawa, H.; Liu, X-J Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 19 https://doi.org/10.1088/0953-4075/45/19/194014	journal	September 2012
Role of symmetry restrictions on valence electron binding energies of CF ₄ Müller, Jiri; Poulain, Enrique; Goscinski, Osvaldo The Journal of Chemical Physics, Vol. 72, Issue 4 https://doi.org/10.1063/1.439456	journal	February 1980
Electron spectroscopy observation of the 1s2s22p6(2S) state in atomic fluorine by means of electron impact excitation of the hf molecule Svensson, S.; Karlsson, L.; Mårtensson, N. Journal of Electron Spectroscopy and Related Phenomena, Vol. 50, Issue 2 https://doi.org/10.1016/0368-2048(90)87078-3	journal	January 1990
Theoretical study of electron-impact excitation of $N_{2}^{+}$ Orel, A. E.; Rescigno, T. N.; Lengsfield III, B. H. Physical Review A, Vol. 42, Issue 9 https://doi.org/10.1103/PhysRevA.42.5292	journal	November 1990
Molecular frame photoelectron angular distributions for core ionization of ethane, carbon tetrafluoride and 1,1-difluoroethylene Menssen, A.; Trevisan, C. S.; Schöffler, M. S. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 49, Issue 5 https://doi.org/10.1088/0953-4075/49/5/055203	journal	February 2016
Doubly ionized states of carbon tetrafluoride Griffiths, W. J.; Svensson, S.; Naves de Brito, A. Chemical Physics, Vol. 173, Issue 1 https://doi.org/10.1016/0301-0104(93)80222-U	journal	June 1993
The fragmentation of core ionized CF ₄ probed by threshold-photoelectron-photoion-photoion coincidence (TPEPIPICO) spectroscopy Thomas, M. K.; Fisher, B. O.; Hatherly, P. A. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 32, Issue 11 https://doi.org/10.1088/0953-4075/32/11/310	journal	January 1999
Changes in molecular KLL Auger spectrum of fluorine on going from HF to LiF, NaF, and KF Sairanen, O. -P.; Aksela, H.; Aksela, S. Chemical Physics Letters, Vol. 215, Issue 4 https://doi.org/10.1016/0009-2614(93)85727-6	journal	December 1993
Conformational and nuclear dynamics effects in molecular Auger spectra: fluorine core-hole decay in CF ₄ Arion, T.; Takahashi, O.; Püttner, R. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 47, Issue 12 https://doi.org/10.1088/0953-4075/47/12/124033	journal	June 2014
The Auger spectra of CF ₄ in the light of foreign imaging Gottfried, F. O.; Cederbaum, L. S.; Tarantelli, F. The Journal of Chemical Physics, Vol. 104, Issue 24 https://doi.org/10.1063/1.471737	journal	June 1996
Vibronic coupling and symmetry breaking in core electron ionization Domcke, W.; Cederbaum, L. S. Chemical Physics, Vol. 25, Issue 2 https://doi.org/10.1016/0301-0104(77)87075-4	journal	October 1977
Interchannel coupling and ground state correlation effects in the photoionization of CO Rescigno, T. N.; Lengsfield, B. H.; Orel, A. E. The Journal of Chemical Physics, Vol. 99, Issue 7 https://doi.org/10.1063/1.466010	journal	October 1993
Vibronic coupling in the K shell excitation of ethyne Kempgens, B.; Itchkawitz, B. S.; Feldhaus, J. Chemical Physics Letters, Vol. 277, Issue 5-6 https://doi.org/10.1016/S0009-2614(97)00953-6	journal	October 1997
Theoretical study of asymmetric molecular-frame photoelectron angular distributions for $C 1 s$ photoejection from ${CO}_{2}$ Miyabe, S.; McCurdy, C. W.; Orel, A. E. Physical Review A, Vol. 79, Issue 5 https://doi.org/10.1103/PhysRevA.79.053401	journal	May 2009
Recoil-ion and electron momentum spectroscopy: reaction-microscopes Ullrich, J.; Moshammer, R.; Dorn, A. Reports on Progress in Physics, Vol. 66, Issue 9 https://doi.org/10.1088/0034-4885/66/9/203	journal	August 2003
Imaging molecular isomerization using molecular-frame photoelectron angular distributions Rescigno, T. N.; Douguet, Nicolas; Orel, A. E. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 19 https://doi.org/10.1088/0953-4075/45/19/194001	journal	September 2012
Ultrafast Probing of Core Hole Localization in N2 Schoffler, M. S.; Titze, J.; Petridis, N. Science, Vol. 320, Issue 5878 https://doi.org/10.1126/science.1154989	journal	May 2008
Imaging molecular shapes with molecular-frame photoelectron angular distributions from core hole ionization Trevisan, C. S.; McCurdy, C. W.; Rescigno, T. N. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 19 https://doi.org/10.1088/0953-4075/45/19/194002	journal	September 2012
Vibronic coupling and core-hole localization in K -shell excitations of ethylene Gadea, F. X.; Köppel, H.; Schirmer, J. Physical Review Letters, Vol. 66, Issue 7 https://doi.org/10.1103/PhysRevLett.66.883	journal	February 1991
Anisotropic Ultrafast Dissociation Probed by the Doppler Effect in Resonant Photoemission from ${C F}_{4}$ Ueda, K.; Kitajima, M.; De Fanis, A. Physical Review Letters, Vol. 90, Issue 23 https://doi.org/10.1103/PhysRevLett.90.233006	journal	June 2003
Ab initio calculation of transition rates for autoionization: the Auger spectra of HF and F− Schimmelpfennig, B.; Nestmann, B. M.; Peyerimhoff, S. D. Journal of Electron Spectroscopy and Related Phenomena, Vol. 74, Issue 3 https://doi.org/10.1016/0368-2048(95)02373-9	journal	November 1995

Cited By (2)

Resonance signatures in the body-frame valence photoionization of CF ₄ Larsen, K. A.; Trevisan, C. S.; Lucchese, R. R. Physical Chemistry Chemical Physics, Vol. 20, Issue 32 https://doi.org/10.1039/c8cp03637c	journal	January 2018
Dynamics of tunneling ionization using Bohmian mechanics Douguet, Nicolas; Bartschat, Klaus Physical Review A, Vol. 97, Issue 1 https://doi.org/10.1103/physreva.97.013402	journal	January 2018

Similar Records

Observing pre-edge

K

-shell resonances in Kr, Xe, and

{XeF}_{2}

Journal Article · Fri Aug 09 00:00:00 EDT 2019 · Physical Review A · OSTI ID:1379684

Southworth, S. H.; Dunford, R. W.; Ray, D.; +11 more

Auger decay of

1 σ_{g}

and

1 σ_{u}

hole states of the

N_{2}

molecule: Disentangling decay routes from coincidence measurements

Journal Article · Thu Apr 29 00:00:00 EDT 2010 · Physical Review A - Atomic, Molecular, and Optical Physics · OSTI ID:1379684

Semenov, S. K.; Schöffler, M. S.; Titze, J.; +17 more

Photoelectron and Auger electron asymmetries: Alignment of

{Xe}^{+ 2} D_{\frac{5}{2}}

by photoionization

Journal Article · Thu Oct 01 00:00:00 EDT 1981 · Physical Review, A (General Physics) · OSTI ID:1379684

Southworth, S. H.; Kobrin, P. H.; Truesdale, C. M.; +3 more

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS

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

Citation Formats

References (26)

Cited By (2)

Similar Records

Related Subjects

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