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We have studied the reaction of reduced nitric-oxide synthase (NOS) with molecular oxygen at -30 o C. In the first reaction cycle (from l-Arg to hydroxy-l-Arg), an oxygen adduct complex formed rapidly. Experiments in the absence of the reductase domain demonstrated that this complex was then further reduced by one electron stemming from the cofactor tetrahydrobiopterin (BH4). Spectral evidence...