Experimental results are presented that support the surface-catalyzed production of nitric oxide from the recombination of oxygen and nitrogen atoms on quartz. The experiments employ two-photon laser-induced fluorescence detection of atomic oxygen and atomic nitrogen to characterize changes in gas-phase atom concentrations as the ratio of O to N atoms is varied at the opening of a diffusion-tube side-arm reactor. The measurements verify a correlation between decreased O-atom loss and enhanced N-atom loss in N 2 =N=O mixtures. Computational simulations of the side-arm reactor with a multispecies reaction-diffusion model strengthen the case for NO surface formation, reproducing observed changes in O-and N-atom concentration profiles with varying O/N ratios at the side-arm entrance when surface-catalyzed NO production is included in the boundary conditions. Nomenclature c = concentration or molar density, mol m 3 D = diffusion coefficient, m 2 s 1 F = volumetric flow rate, sccm f s;r = branching fraction of reactant s into product r j = diffusive mass flux, kg m 2 s 1 k B = Boltzmann's constant 1:381 10 23 J K 1 L = side-arm length, m M = molar mass, kg mol 1 N Avro = Avogadro's number, 6:022 10 23 mol 1 P = pressure, Pa R = side-arm radius, m R = universal gas constant, 8:314 J mol 1 K 1 r = radial side-arm coordinate, m T = temperature, K v = bulk flow speed, m s 1 v = average thermal speed, m s 1 w = gas-phase production rate, kg m 3 s 1 w w = surface production rate, kg m 2 s 1 x = mole fraction z = axial side-arm coordinate, m = loss probability 1;1 rs = collision integral, m 2 = viscosity, Pa s = mass density, kg m 3 = diffusion velocity, m s 1 ! s = weighting factor, Eq. (4) Subscripts O, O 2 , N, N 2 , NO = species s = species index r = species index or radial direction w = wall z = axial direction