화학공학소재연구정보센터
Journal of Physical Chemistry A, Vol.120, No.22, 3855-3860, 2016
Laser Measurements of the H Atom plus Ozone Rate Constant at Mesospheric Temperatures
The exothermic H + O-3 reaction produces OH(v) Meinel band emissions, used to derive mesospheric H concentrations and chemical heating rates. We remeasured its rate constant to reduce its uncertainty and extended the measurements to lower mesospheric temperatures using modern laser-induced fluorescence (LIF) techniques. H atoms were produced by pulsed ultraviolet laser trace photolysis of O-3, followed by reaction of O(D-1) with added H-2. A second delayed, frequency-mixed dye laser measured the reaction decay rate with the remaining ozone using LIF. We monitored either the H atom decay by two photon excitation at 205 nm and detection of red fluorescence, or the OH (v = 9) product time evolution with excitation of the B-2 Sigma(+)-X-2 Pi (0,9) band at 237 nm and emission in the blue B-2 Sigma(+)-A(2)Sigma(+) (0,7) band. By cooling the enclosed low pressure:flow cell we obtained measurements from 140 to 305 K at 20 to 200 Torr in Ar. Small kinetic modeling corrections were made for secondary regeneration of H atoms. The results are consistent with the current NASA JPL recommendation for this rate constant and establish its extrapolation down to the lower temperatures of the mesosphere.