Excitation of the primary tropospheric chemical mode in a global three-dimensional model
Published Web Locationhttps://doi.org/10.1029/2000JD900399
Coupling of local chemical processes over the globe by atmospheric transport leads to the existence of chemical modes that are a fundamental characterization of global atmospheric chemistry and provide a true description of the atmospheric response to small changes in trace-gas emissions. Such coupled chemistry-transport modes in global tropospheric chemistry are an inherent feature of three-dimensional chemical transport models (CTMs). In CTMs these modes cannot be solved for explicitly, as they have been for the case of low-order, fully linearized systems, but they are investigated here through a series of perturbation experiments. When using meteorological fields that recycle every year, the long-lived modes are readily seen as seasonal decay patterns that e-fold each year. An important application of chemical modes is the study of how emissions of CO and NO excite perturbations to the CH4-like mode, the longest-lived (primary) mode found in tropospheric chemistry (i.e., with fixed stratospheric composition). Perturbation experiments are conducted with the University of California, Irvine, three-dimensional tropospheric CTM to identify this primary tropospheric mode and to determine its five-dimensional structure. The previous demonstrations of a long-lived chemical mode with 1.5 times the lifetime of CH4are corroborated. The ability of emissions of CO and NO to excite this mode is then demonstrated, and a quantitative evaluation of the indirect effect of CO emissions on the greenhouse gases CH4 and tropospheric O3 is made, showing that 100 kg of CO is equivalent to 5–6 kg of CH4 emissions.