ESR study of atomic hydrogen and tritium in solid T2 and T2:H2 matrices below 1 K

• Published in: Physical chemistry chemical physics : PCCP 2017, Vol.19 (4), p.2834-2842
• Main Authors: Sheludiakov, S, Ahokas, J, Järvinen, J, Lehtonen, L, Vainio, O, Vasiliev, S, Lee, D M, Khmelenko, V V
• Format: Article
• Language: English
• Subjects: Atomic properties; Chemical reactions; Diffusion; Exchange; Hydrogen; Migration; Tritium; Tunneling
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/c6cp06933a

We report on the first ESR study of atomic hydrogen and tritium stabilized in solid T2 and T2:H2 matrices down to 70 mK. The concentrations of T atoms in pure T2 approached 2 × 1020 cm-3 (0.60%) and record-high concentrations of H atoms ∼1 × 1020 cm-3 (0.33%) were reached in T2:H2 solid mixtures where a fraction of T atoms became converted into H due to the isotopic exchange reaction T + H2 → TH + H. The maximum concentrations of unpaired T and H atoms were limited by their recombination which becomes enhanced by efficient atomic diffusion due to the presence of a large number of vacancies and phonons generated in the matrices by β-particles. Recombination also appeared in an explosive manner, both being stimulated and spontaneously in thick films where sample cooling was insufficient. We suggest that the main mechanism for H and T migration is physical diffusion related to tunneling or hopping to vacant sites in contrast to tunneling chemical exchange reactions which govern diffusion of H and D atoms created in H2 and D2 matrices by other methods.