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Experimental lifetime of the a1Δ electronically excited state of CH−

Gustav Eklund1,*, Moa K. Kristiansson1, K. C. Chartkunchand2, Emma K. Anderson3, Malcolm Simpson4, Roland Wester4, Henning T. Schmidt1,†, Henning Zettergren1, Henrik Cederquist1 et al.

Wolf D. Geppert1

  • 1Department of Physics, Stockholm University, Stockholm 10691, Sweden
  • 2Atomic, Molecular and Optical Physics Laboratory, RIKEN, Saitama 351-0198, Japan
  • 3Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark
  • 4Institut für Ionenphysik und Angewandte Physik, Universität Innsbruck, Technikerstraße 25, 6020 Innsbruck, Austria

  • *gustav.eklund@fysik.su.se
  • †schmidt@fysik.su.se

Phys. Rev. Research 4, L012016 – Published 11 February, 2022

DOI: https://doi.org/10.1103/PhysRevResearch.4.L012016

Abstract

By repeatedly probing the a1Δ excited state and the X3Σ− ground-state populations in a beam of CH− ions stored in a cryogenic ion-beam storage ring for 100 s, we extract an intrinsic lifetime of 14.9±0.5 s for this excited state. This is far longer than all earlier experimental and theoretical results, exposing large difficulties in measuring and calculating slow decays and the need for benchmark quality experiments.

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References (23)

  1. T. J. Millar, C. Walsh, and T. A. Field, Negative ions in space, Chem. Rev. 117, 1765 (2017).
  2. N. Sakai, T. Sakai, Y. Osamura, and S. Yamamoto, Detection of C6H− toward the low-mass protostar IRAS 04368+2557 in L1527, Astrophys. J. 667, L65 (2007).
  3. V. Vuitton, P. Lavvas, R. Yelle, M. Galand, A. Wellbrock, G. Lewis, A. Coates, and J.-E. Wahlund, Negative ion chemistry in Titan's upper atmosphere, Planet. Space Sci. 57, 1558 (2009).
  4. E. Yurtsever, M. Satta, R. Wester, and F. A. Gianturco, On the formation of interstellar CH− anions: Exploring mechanism and rates for CH2 reacting with H−, J. Phys. Chem. A 124, 5098 (2020).
  5. D. Feldmann, Photoablösung von Elektronen bei einigen stabilen negativen Ionen, Z. Naturforsch. A 25, 621 (1970).
  6. A. Kasdan, E. Herbst, and W. Lineberger, Laser photoelectron spectrometry of CH−, Chem. Phys. Lett. 31, 78 (1975).
  7. D. J. Goebbert, Photoelectron imaging of CH−, Chem. Phys. Lett. 551, 19 (2012).
  8. D. Feller, Application of a convergent, composite coupled cluster approach to bound state, adiabatic electron affinities in atoms and small molecules, J. Chem. Phys. 144, 014105 (2016).
  9. M. Okumura, L. I. Yeh, D. Normand, and Y. T. Lee, The lifetimes for spontaneous emission from the X3Σ−(v=1) and a1Δ states of CH−, J. Chem. Phys. 85, 1971 (1986).
  10. B. H. Lengsfield, J. O. Jensen, and D. R. Yarkony, On the evaluation of lifetimes for spin-forbidden radiative transitions originating in coupling to states embedded in a continuum. application to CH−, J. Chem. Phys. 88, 3853 (1988).
  11. S. Srivastava and N. Sathyamurthy, Radiative lifetimes of spin forbidden and spin allowed - transitions and complete basis set extrapolated ab initio potential energy curves for the ground and excited states of CH−, J. Chem. Phys. 137, 214314 (2012).
  12. R. D. Thomas, H. T. Schmidt, G. Andler, M. Björkhage, M. Blom, L. Brännholm, E. Bäckström, H. Danared, S. Das, N. Haag, P. Halldén, F. Hellberg, A. I. S. Holm, H. A. B. Johansson, A. Källberg, G. Källersjö, M. Larsson, S. Leontein, L. Liljeby, P. Löfgren et al., The double electrostatic ion ring experiment: A unique cryogenic electrostatic storage ring for merged ion-beams studies, Rev. Sci. Instrum. 82, 065112 (2011).
  13. H. T. Schmidt, R. D. Thomas, M. Gatchell, S. Rosén, P. Reinhed, P. Löfgren, L. Brännholm, M. Blom, M. Björkhage, E. Bäckström, J. D. Alexander, S. Leontein, D. Hanstorp, H. Zettergren, L. Liljeby, A. Källberg, A. Simonsson, F. Hellberg, S. Mannervik, M. Larsson et al., First storage of ion beams in the double electrostatic ion-ring experiment: DESIREE, Rev. Sci. Instrum. 84, 055115 (2013).
  14. H. T. Schmidt, G. Eklund, K. C. Chartkunchand, E. K. Anderson, M. Kamińska, N. de Ruette, R. D. Thomas, M. K. Kristiansson, M. Gatchell, P. Reinhed, S. Rosén, A. Simonsson, A. Källberg, P. Löfgren, S. Mannervik, H. Zettergren, and H. Cederquist, Rotationally Cold OH− Ions in the Cryogenic Electrostatic Ion-Beam Storage Ring DESIREE, Phys. Rev. Lett. 119, 073001 (2017).
  15. E. Bäckström, D. Hanstorp, O. M. Hole, M. Kaminska, R. F. Nascimento, M. Blom, M. Björkhage, A. Källberg, P. Löfgren, P. Reinhed, S. Rosén, A. Simonsson, R. D. Thomas, S. Mannervik, H. T. Schmidt, and H. Cederquist, Storing keV Negative Ions for an Hour: The Lifetime of the Metastable P21/2o Level in S32−, Phys. Rev. Lett. 114, 143003 (2015).
  16. K. C. Chartkunchand, M. Kamińska, E. K. Anderson, M. K. Kristiansson, G. Eklund, O. M. Hole, R. F. Nascimento, M. Blom, M. Björkhage, A. Källberg, P. Löfgren, P. Reinhed, S. Rosén, A. Simonsson, R. D. Thomas, S. Mannervik, V. T. Davis, P. A. Neill, J. S. Thompson, D. Hanstorp et al., Radiative lifetimes of the bound excited states of Pt−, Phys. Rev. A 94, 032501 (2016).
  17. M. K. Kristiansson, S. Schiffmann, J. Grumer, J. Karls, N. de Ruette, G. Eklund, V. Ideböhn, N. D. Gibson, T. Brage, H. Zettergren, D. Hanstorp, and H. T. Schmidt, Experimental and theoretical studies of excited states in Ir−, Phys. Rev. A 103, 062806 (2021).
  18. S. Rosén, H. T. Schmidt, P. Reinhed, D. Fischer, R. D. Thomas, H. Cederquist, L. Liljeby, L. Bagge, S. Leontein, and M. Blom, Operating a triple stack microchannel plate-phosphor assembly for single particle counting in the 12-300 K temperature range, Rev. Sci. Instrum. 78, 113301 (2007).
  19. U. Mänz, A. Zilch, P. Rosmus, and H.-J. Werner, MCSCF-CI calculations of infrared transition probabilities in the CH− and NH− ions, J. Chem. Phys. 84, 5037 (1986).
  20. J. Fedor, K. Hansen, J. U. Andersen, and P. Hvelplund, Nonthermal Power Law Decay of Metal Dimer Anions, Phys. Rev. Lett. 94, 113201 (2005).
  21. E. K. Anderson, A. F. Schmidt-May, P. K. Najeeb, G. Eklund, K. C. Chartkunchand, S. Rosén, A. Larson, K. Hansen, H. Cederquist, H. Zettergren, and H. T. Schmidt, Spontaneous Electron Emission from Hot Silver Dimer Anions: Breakdown of the Born-Oppenheimer Approximation, Phys. Rev. Lett. 124, 173001 (2020).
  22. J. E. Sansonetti and W. C. Martin, Handbook of basic atomic spectroscopic data, J. Phys. Chem. Ref. Data 34, 1559 (2005).
  23. T. Carette and M. R. Godefroid, Theoretical study of the C−S3/2o4 and D3/2,5/2o2 bound states and C ground configuration: Fine and hyperfine structures, isotope shifts, and transition probabilities, Phys. Rev. A 83, 062505 (2011).

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