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Odd hydrogen chemistry

Our ability to predict future concentrations of significant greenhouse gases such as methane and O depends on our ability to correctly predict tropospheric odd hydrogen chemistry. Prediction of CHCCl concentrations have provided one test of our understanding and theoretical ability to predict global OH concentrations, but the test depends on accurate calibration of the measured CHCCl and on accurate estimates of emissions. Measurements of negative ocean saturation anomalies for CHCCl (Butler et al., 1992) have pointed to a previously unaccounted for ocean sink that would require small (10%) downward corrections to model-predicted OH concentrations in order to maintain good agreement with ambient CHCCl data. On the other hand, new rate data for the reaction between CHCCl and OH are lower than previously recommended rates by between 5 and 15% depending on temperature (Finlayson-Pitt et al., 1992). This finding implies that previously predicted OH concentrations would still be consistent with the measured abundance of CHCCl even accounting for the ocean sink. However, in contrast to model calibration studies with CHCCl (Taylor et al., 1991; Spivakovsky et al., 1990), studies which use 14CO for calibration indicate that model concentrations of global OH are too low by about 45% (Mak et al., 1992).

An alternate method for testing our theoretical understanding of odd hydrogen chemistry and our ability to predict OH is to compare local photochemical model predictions of OH and peroxy radicals with measurements in well-characterized field experiments. In contrast to studies with CHCCl and 14CO, however, these studies indicate that predicted OH may be too high. For example, Liu et al. (1992) used observed and computed ratios of HNO to NO and observed and computed CHO and CHOOH concentrations at Mauna Loa to argue that model predicted OH is significantly overestimated, although other factors such as measurement inaccuracy may also explain the discrepancies between theory and observation. Studies in more polluted areas by Cantrell et al. (1993) have shown that in some cases model predicted peroxy radical concentrations agree with data, while in others they do not. Significant progress has been made in developing instrumentation to measure the concentrations of OH and HO along with their organic analogues (Eisele and Tanner, 1991; Mount, 1992; Hard et al., 1992; Cantrell et al., 1993). In the future, comparison of models with measurements along with more accurate understanding of kinetic mechanisms should enable the tropospheric chemistry community to derive a more accurate understanding of odd hydrogen chemistry.



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Next: Heterogenous chemical interactions Up: Tropospheric chemistry research in Previous: Ozone



U.S. National Report to IUGG, 1991-1994
Rev. Geophys. Vol. 33 Suppl., © 1995 American Geophysical Union