State-to-state rotational energy transfer (RET) rate coefficients for NO (A(2)Sigma(+); v'=0, J=5.5, 11.5, 17.5) were measured for N-2 and O-2 at room temperature using a pump-probe method. The NO A(2)Sigma(+) state is prepared by 226 nm light and the RET is monitored by fluorescence from the D(2)Sigma(+) v'=0 state, following excitation by a time-delayed laser at similar to1.1 mum. Additionally, total collisional removal and final state distributions were measured exciting in the Q(1)+P-21 band head, to simulate an NO laser-induced fluorescence atmospheric monitoring scheme. Time-resolved modeling is used to understand relaxation mechanisms and predict relaxation times in ambient air. H2O at atmospherically relevant concentrations does not affect the degree of RET in ambient air. (C) 2004 American Institute of Physics.