Absence of recombination of neighboring H atoms in highly purified solid parahydrogen: Electron spin resonance, electron-nuclear double resonance, and electron spin echo studies

Diffusion and recombination of H atoms were studied in solid hydrogen containing ortho-H2 molecules at relative concentration Xo=0.001→0.75 using electron spin resonance (ESR), electron-nuclear double resonance (ENDOR), and electron spin echo (ESE) methods at around 4 K. When the rate-determining step for recombination is assumed to be the diffusion of H atoms, the rate constant for recombination at Xo⩾0.1 is consistent with the diffusion coefficient estimated from the analysis of ENDOR spectra and longitudinal spin relaxation behaviors. The recombination rate constant at Xo<0.1, however, is too slow to be explained using the diffusion coefficient estimated from longitudinal spin relaxation and forbidden spin-flip satellite transition studies. This result suggests that, even if one H atom finds another H in its immediate neighborhood, these H atoms do not react to form a H2 molecule at Xo≪0.1. The absence of recombination of H atoms is due to lack of the energy dispersion path required for the recombination of diatomic molecules. Since the absence of recombination becomes less significant at higher Xo, ortho-H2 molecules are found to play an important role in the energy dispersion which accompanies the recombination reaction.