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Theoretical evaluation of decay mode of Th229m in solid samples

Ryotaro Masuda (益田遼太郎)1,*, Tomoya Naito (内藤智也)2,3,4,†, Masashi Kaneko (金子政志)1, Hiroyuki Kazama (風間裕行)1, So Hashiba (橋場奏)1, Kosuke Misawa (三澤宏介)1, and Yoshitaka Kasamatsu (笠松良崇)1

  • *Contact author: masudar21@chem.sci.osaka-u.ac.jp
  • †Contact author: tnaito@ribf.riken.jp

Phys. Rev. Research 7, 043217 – Published 24 November, 2025

DOI: https://doi.org/10.1103/hn1b-51yx

Abstract

The excitation energy of Th229m is extremely low at 8.4eV; thus, this isotope exhibits changes in its decay modes depending on the chemical state, specifically the outermost electronic states. However, the reported half-lives of the γ-ray transition are not consistent among the previous experiments. In this study, we investigate the chemical states of Th229m by density functional theory calculations. Based on these results, we evaluate the relationship between the experimental half-life of each sample and the electronic state of Th. The calculation results indicate that ion trap method, CaF2 model, and MgF2 one decay only via the γ-ray transition, whereas LiSrAlF6 one decays via the γ-ray transition and has a possibility of decay via internal conversion and electron bridge.

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References (41)

  1. F. Ponce, E. Swanberg, J. Burke, R. Henderson, and S. Friedrich, Accurate measurement of the first excited nuclear state in U235, Phys. Rev. C 97, 054310 (2018).
  2. M. N. de Mevergnies, Perturbation of the U235m decay rate by implantation in transition metals, Phys. Rev. Lett. 29, 1188 (1972).
  3. M. N. de Mevergnies and P. Del Marmol, Effect of the oxidation state on the half-life of 235Um, Phys. Lett. B 49, 428 (1974).
  4. S. Kraemer, Observation of the radiative decay of the Th229 nuclear clock isomer, Nature (London) 617, 706 (2023).
  5. A. Yamaguchi, Y. Shigekawa, H. Haba, H. Kikunaga, K. Shirasaki, M. Wada, and H. Katori, Laser spectroscopy of triply charged Th229 isomer for a nuclear clock, Nature (London) 629, 62 (2024).
  6. J. Tiedau, M. V. Okhapkin, K. Zhang, J. Thielking, G. Zitzer, E. Peik, F. Schaden, T. Pronebner, I. Morawetz, L. T. De Col, F. Schneider, A. Leitner, M. Pressler, G. A. Kazakov, K. Beeks, T. Sikorsky, and T. Schumm, Laser excitation of the Th-229 nucleus, Phys. Rev. Lett. 132, 182501 (2024).
  7. R. Elwell, C. Schneider, J. Jeet, J. E. S. Terhune, H. W. T. Morgan, A. N. Alexandrova, H. B. Tran Tan, A. Derevianko, and E. R. Hudson, Laser excitation of the Th229 nuclear isomeric transition in a solid-state host, Phys. Rev. Lett. 133, 013201 (2024).
  8. T. Hiraki et al., Controlling Th229 isomeric state population in a VUV transparent crystal, Nat. Commun. 15, 5536 (2024).
  9. V. F. Strizhov and E. V. Tkalya, Decay channel of low-lying isomer state of the Th229 nucleus. Possibilities of experimental investigation, Zh. Eksp. Teor. Fiz. 99, 697 (1991) [Sov. Phys. JETP 72, 387 (1991)].
  10. V. A. Dzuba and V. V. Flambaum, Resonance nuclear excitation of the Th229 nucleus via electronic bridge process in Th II, Phys. Rev. A 111, L041103 (2025).
  11. F. E. Karpeshin and M. B. Trzhaskovskaya, Impact of the ionization of the atomic shell on the lifetime of the Th229 isomer, Nucl. Phys. A 969, 173 (2018).
  12. L. von der Wense and B. Seiferle, The Th229 isomer: Prospects for a nuclear optical clock, Eur. Phys. J. A 56, 277 (2020).
  13. L. von der Wense, B. Seiferle, M. Laatiaoui, J. B. Neumayr, H.-J. Maier, H.-J. Maier, H.-F. Wirth, C. Mokry, J. Runke, K. Eberhardt, C. E. Düllmann, N. G. Trautmann, and P. G. Thirolf, Direct detection of the Th229 nuclear clock transition, Nature (London) 553, 47 (2016).
  14. B. Seiferle, L. von der Wense, and P. G. Thirolf, Lifetime measurement of the Th229 nuclear isomer, Phys. Rev. Lett. 118, 042501 (2017).
  15. E. Peik and C. Tamm, Nuclear laser spectroscopy of the 3.5 eV transition in Th-229, Europhys. Lett. 61, 181 (2003).
  16. V. A. Dzuba and V. V. Flambaum, Using the Th III ion for a nuclear clock and searches for new physics, Phys. Rev. A 111, 053109 (2025).
  17. E. Peik, T. Schumm, M. S. Safronova, A. Pálffy, J. Weitenberg, and P. G. Thirolf, Nuclear clocks for testing fundamental physics, Quantum Sci. Technol. 6, 034002 (2021).
  18. V. V. Flambaum, Enhanced effect of temporal variation of the fine structure constant and the strong interaction in Th229, Phys. Rev. Lett. 97, 092502 (2006).
  19. E. V. Tkalya, Spontaneous emission probability for M1 transition in a dielectric medium: Th229 (3/2+, 3.5±1.0eV) decay, Jetp Lett. 71, 311 (2000).
  20. R. A. Müller, A. V. Volotka, S. Fritzsche, and A. Surzhykov, Theoretical analysis of the electron bridge process in 229Th3+, Nucl. Instrum. Methods Phys. Res., Sect. B 408, 84 (2017).
  21. S. G. Porsev, C. Cheung, and M. S. Safronova, Low-lying energy levels of 229Th35+ and the electronic bridge process, Quantum Sci. Technol. 6, 034014 (2021).
  22. S. G. Porsev, V. V. Flambaum, E. Peik, and C. Tamm, Excitation of the isomeric Th229m nuclear state via an electronic bridge process in Th229+, Phys. Rev. Lett. 105, 182501 (2010).
  23. H. W. T. Morgan, H. B. Tran Tan, R. Elwell, A. N. Alexandrova, E. R. Hudson, and A. Derevianko, Theory of internal conversion of the Th229 nuclear isomer in solid-state hosts, Phys. Rev. Lett. 134, 253801 (2025).
  24. K. Persson, Materials data on CaF2 (SG:225) by materials project (2014), https://doi.org/10.17188/1201632.
  25. K. Persson, Materials data on MgF2 (SG:205) by materials project (2014), https://doi.org/10.17188/1192516.
  26. K. Persson, Materials data on SrLiAlF6 (SG:163) by materials project (2014), https://doi.org/10.17188/1281377.
  27. P. Hohenberg and W. Kohn, Inhomogeneous electron gas, Phys. Rev. 136, B864 (1964).
  28. W. Kohn and L. J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
  29. W. Kohn, Nobel lecture: Electronic structure of matter—wave functions and density functionals, Rev. Mod. Phys. 71, 1253 (1999).
  30. P. Giannozzi et al., quantum espresso: A modular and open-source software project for quantum simulations of materials, J. Phys.: Condens. Matter 21, 395502 (2009).
  31. J. P. Perdew, K. Burke, and Y. Wang, Generalized gradient approximation for the exchange-correlation hole of a many-electron system, Phys. Rev. B 54, 16533 (1996).
  32. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  33. M. Torrent, N. A. W. Holzwarth, F. Jollet, D. Harris, N. Lepley, and X. Xu, Electronic structure packages: Two implementations of the projector augmented wave (PAW) formalism, Comput. Phys. Commun. 181, 1862 (2010).
  34. A. Dal Corso, Pseudopotentials periodic table: From H to Pu, Comput. Mater. Sci. 95, 337 (2014).
  35. G. te Velde, F. M. Bickelhaupt, E. J. Baerends, C. Fonseca Guerra, S. J. A. van Gisbergen, J. G. Snijders, and T. Ziegler, Chemistry with ADF, J. Comput. Chem. 22, 931 (2001).
  36. E. Van Lenthe and E. J. Baerends, Optimized slater-type basis sets for the elements 1–118, J. Comput. Chem. 24, 1142 (2003).
  37. A. D. Becke, Density-functional thermochemistry. III. The role of exact exchange, J. Chem. Phys. 98, 5648 (1993).
  38. E. van Lenthe, E. J. Baerends, and J. G. Snijders, Relativistic regular two-component hamiltonians, J. Chem. Phys. 99, 4597 (1993).
  39. J. I. Rodríguez, R. F. Bader, P. W. Ayers, C. Michel, A. W. Götz, and C. Bo, A high performance grid-based algorithm for computing QTAIM properties, Chem. Phys. Lett. 472, 149 (2009).
  40. P. Dessovic, P. Mohn, R. A. Jackson, G. Winkler, M. Schreitl, G. Kazakov, and T. Schumm, 229Thorium-doped calcium fluoride for nuclear laser spectroscopy, J. Phys.: Condens. Matter 26, 105402 (2014).
  41. K. Momma and F. Izumi, VESTA3 for three-dimensional visualization of crystal, volumetric and morphology data, J. Appl. Cryst. 44, 1272 (2011).

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