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Isomer depletion as experimental evidence of nuclear excitation by electron capture

Nature volume 554, pages 216–218 (2018)Cite this article

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Matters Arising to this article was published on 02 June 2021

Abstract

The atomic nucleus and its electrons are often thought of as independent systems that are held together in the atom by their mutual attraction. Their interaction, however, leads to other important effects, such as providing an additional decay mode for excited nuclear states, whereby the nucleus releases energy by ejecting an atomic electron instead of by emitting a γ-ray. This ‘internal conversion’ has been known for about a hundred years and can be used to study nuclei and their interaction with their electrons1,2,3. In the inverse process—nuclear excitation by electron capture (NEEC)—a free electron is captured into an atomic vacancy and can excite the nucleus to a higher-energy state, provided that the kinetic energy of the free electron plus the magnitude of its binding energy once captured matches the nuclear energy difference between the two states. NEEC was predicted4 in 1976 and has not hitherto been observed5,6. Here we report evidence of NEEC in molybdenum-93 and determine the probability and cross-section for the process in a beam-based experimental scenario. Our results provide a standard for the assessment of theoretical models relevant to NEEC, which predict cross-sections that span many orders of magnitude. The greatest practical effect of the NEEC process may be on the survival of nuclei in stellar environments7, in which it could excite isomers (that is, long-lived nuclear states) to shorter-lived states. Such excitations may reduce the abundance of the isotope after its production. This is an example of ‘isomer depletion’, which has been investigated previously through other reactions8,9,10,11,12, but is used here to obtain evidence for NEEC.

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Figure 1: Relevant part of the 93Mo decay scheme.
Figure 2: Spectra demonstrating the signature of NEEC in 93Mo.
Figure 3: Spectra used to determine the NEEC probability in 93Mo.

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Acknowledgements

C.J.C. and J.J.C. thank A. D. Ayangeakaa for input on the potential contributions of Coulomb excitations to the background and M. S. Litz and N. R. Pereira for discussions. We also thank J. Rohrer for assistance in setting up the Gammasphere experiment and the ATLAS operations staff for their efforts. This work was initiated under the US Army Research Laboratory (ARL) Director’s Research Initiative, award number DRI-FY14-SE-022. Further support was provided by ARL Cooperative Agreements W911NF-12-2-0019 and W911NF-16-2-0034, the US Department of Energy (DOE), Office of Science, Office of Nuclear Physics under contract number DE-AC02-06CH11357, the National Science Foundation under grant number PHY-1203100, the Australian Research Council under grant number FT100100991, and the Polish National Science Centre under grants 2011/01/D/ST2/01286 and 2017/25/B/ST2/00901. M.P., J.R. and A.B.H. received support through Ecopulse, Inc. under ARL contract number W911QX09D0016-0004. This research used resources of Argonne National Laboratory’s ATLAS facility, which is a DOE Office of Science User Facility, and of the HIAF at ANU.

Author information

Author notes

  1. R. V. F. Janssens

    Present address: Department of Physics and Astronomy, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, 27599-3255, USA

  2. R. V. F. Janssens

    Present address: Triangle Universities Nuclear Laboratory, Duke University, Durham, North Carolina, 27708-2308, USA

  3. J. C. Marsh

    Present address: Frontier Technology, Inc., Space and Naval Warfare Systems Command, Systems Center Pacific, 49599 Lassing Road, San Diego, California, 92152, USA

  4. S. Bottoni

    Present address: Dipartimento di Fisica, Università degli Studi di Milano and INFN sez. Milano, I-20133, Milano, Italy

  5. S. A. Karamian: Deceased.

Authors and Affiliations

  1. Oak Ridge Associated Universities Fellowship Program, US Army Research Laboratory, Adelphi, 20783, Maryland, USA

    C. J. Chiara & J. C. Marsh

  2. US Army Research Laboratory, Adelphi, 20783, Maryland, USA

    J. J. Carroll

  3. Physics Division, Argonne National Laboratory, Argonne, 60439, Illinois, USA

    M. P. Carpenter, J. P. Greene, R. V. F. Janssens, D. Seweryniak, S. Zhu & S. Bottoni

  4. Department of Physics, US Naval Academy, Annapolis, 21402, Maryland, USA

    D. J. Hartley

  5. Department of Nuclear Physics, Research School of Physics and Engineering, Australian National University, Canberra, 0200, Australian Capital Territory, Australia

    G. J. Lane

  6. Defense Threat Reduction Agency, Fort Belvoir, 22060, Virginia, USA

    D. A. Matters

  7. Faculty of Chemistry, Nicolaus Copernicus University in Toruń, Toruń, 87-100, Poland

    M. Polasik

  8. National Centre for Nuclear Research, Otwock, 05-400, Poland

    J. Rzadkiewicz

  9. Institute of Optics, University of Rochester, Rochester, 14627, New York, USA

    A. B. Hayes

  10. Flerov Laboratory of Nuclear Reactions, Joint Institute for Nuclear Research, Dubna, 141980, Russia

    S. A. Karamian

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  1. C. J. Chiara
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Contributions

C.J.C. led the experimental effort. The experiment was conceptualized by S.A.K. and J.J.C., with the final design provided by C.J.C. and J.J.C. with input from D.J.H. and G.J.L. The targets were prepared by J.P.G. All authors, except S.B., A.B.H. and S.A.K., participated in the experiment. C.J.C. analysed the data, with substantial input from J.J.C. Guidance on the atomic conditions for NEEC was provided by M.P. and J.R. The calculations of inelastic-scattering cross-sections with FRESCO were performed by S.B. and those of Coulomb excitation with GOSIA by A.B.H. We wish to call attention to the role of our late colleague S.A.K., who provided the initial impetus for this work but sadly did not see these results.

Corresponding author

Correspondence to C. J. Chiara.

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The authors declare no competing financial interests.

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Reviewer Information Nature thanks O. Kocharovskaya and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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Extended data figures and tables

Extended Data Figure 1 Configuration of the target used in the experiment.

a, Schematic of the target construction showing the layers in which 93Mo production occurs (Li), NEEC can occur (C) and the backing that stops all recoils (208Pb), in addition to the important gap of about 3 mm that is needed to accommodate the effective half-life for the decay of the 4,900-keV level. Relative dimensions are not to scale. The beam is incident on the Li surface. b, Photograph of the target positioned inside the Gammasphere target chamber. The beam enters from the lower right side and is parallel to the double rods shown in the upper left part of the photograph.

Extended Data Figure 2 Spectra showing the line shape of the 2,475-keV transition in 93Mo.

a, b, The spectra are from the detectors in ring 9 of Gammasphere at 90° (a) and ring 7 at 79° (b). The spectra in red were recorded while using a Li target backed with 208Pb and with no gap in between. The blue spectra were obtained with a modified target configuration with a gap of about 3 mm. The 2,361-keV peak corresponds to a transition in 92Mo that lies below a level with a half-life of t1/2 = 35 ps. The similar line shapes of these two transitions support the estimate of a delay of tens of picoseconds in the 2,475-keV emission and therefore the rationale for the final target construction.

Extended Data Figure 3 Spectra used to determine background contributions.

Component spectra for the double gate on the Doppler-shifted 2,475-keV γ-ray (1) and the unshifted 1,478-keV γ-ray (2), where gates on the peak and background regions are denoted as ‘g’ and ‘b’, respectively (see text). a, g1g2. b, g1b2. c, b1g2. d, b1b2. Only those γ-rays in 93Mo relevant to the discussion are labelled, with the dashed lines marking their energies. We note that the 770-keV peak in a is a multiplet with the 773- and 777-keV transitions in 92Mo and 97Ru, respectively; only the last two peaks appear in b and d.

Extended Data Figure 4 Calculations of possible competing processes.

The inelastic-scattering cross-sections for exciting 93mMo to the intermediate state, calculated with the code FRESCO, are plotted versus the energy of recoiling 93Mo ions traversing the 7Li (blue) and 12C (red) target layers. The initial energy is the average recoil energy corresponding to 93Mo production at the centre of the Li target.

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Chiara, C., Carroll, J., Carpenter, M. et al. Isomer depletion as experimental evidence of nuclear excitation by electron capture. Nature 554, 216–218 (2018). https://doi.org/10.1038/nature25483

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