In order to make contact with prior QM/MM results, where we quantified the values of s OH that correspond to hemibonding, we compute the Mulliken charges at the "optimally-tuned" (OT)-LRC-ωPBE/6-31++G* level (as described in the Supporting Information), using 600 structures obtained from the ai MD simulations, each separated in time by 25 fs. At both simulation temperatures, the ensemble of s OH values is peaked just below 1.0, indicating nearly complete localization of the unpaired spin on the radical, but the distribution exhibits a long tail stretching to about 0.85 in electron charge units. This tail arises from spin leakage in certain configurations and indicates the presence of some hemibonding. In view of this tail, the existence of some structures with smaller values of r O * O (as compared to the canonical hydrogen-bonded value, r O * O ≈ 2.8 Å) is unsurprising; we have previously shown that the O * • • • O distance is inversely correlated with the extent of spin leakage. The s OH probability distributions obtained from periodic PBE0 + D3 simulations most closely resemble QM/MM results using LRC-ωPBE + D3. In those particular QM/ MM simulations, the small-r O * O feature in g(r O * O ) was absent, just as it is for the periodic PBE0 + D3 simulations reported here.