New evidence is presented for the observation of a muoniated radical in the Mu + Br2 system, from μSR longitudinal field (LF) repolarisation studies in the gas phase, at Br2 concentrations of 0.1 bar in a Br2/N2 mixture at 300 K and at 10 bar total pressure. The LF repolarisation curve, up to a field of 4.5 kG, reveals two paramagnetic components, one for the Mu atom, formed promptly during the slowing-down process of the positive muon, with a known Mu hyperfine coupling constant (hfcc) of 4463 MHz, and one for a muoniated radical formed by fast Mu addition. From model fits to the Br2/N2 data, the radical component is found to have an unusually high muon hfcc, assessed to be ∼3300 MHz with an overall error due to systematics expected to exceed 10%. This high muon hfcc is taken as evidence for the observation of either the Br–Mu–Br radical, and hence of vibrational bonding in this –– system, or of a Mu⋯Br2 van der Waals complex formed in the entrance channel. Preliminary ab initio electronic structure calculations suggest the latter is more likely but fully rigorous calculations of the effect of dynamics on the hfcc for either system have yet to be carried out.
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