Tropospheric ozone changes at unpolluted and semipolluted regions induced by stratospheric ozone changes

摘要

Model studies show that changes in photodissociation rates resulting from changes in ozone column densities induce changes in lower tropospheric ozone, which vary significantly with location and time of the year. The validity of the model results is tested against daily total ozone and ground level ozone at three selected stations (Samoa, Mauna Loa, and Hohenpeissenberg). Observational data for a period of more than 1 decade have been analyzed. Comparisons are made of model-simulated distribution of ozone and its precursors (NO x and CO) at the three stations. Further comparisons are made of observed and model-calculated sensitivity in surface ozone to reduction in ozone column densities. Calculations performed with a global-scale chemical transport model (CTM) with extensive ozone chemistry reproduce well the observed levels and seasonal distribution of NO x , CO, and ozone at remote background stations (Samoa and Mauna Loa) and at stations in more polluted regions (Hohenpeissenberg). A chemical box model is used to demonstrate the chemical link between surface ozone changes and changes in total ozone for different NO x levels. Model studies and analysis of the observational data show that ground level ozone at the remote, low-NO x stations of Mauna Loa and Samoa is correlated positively with total ozone, with an exception at Mauna Loa during winter months. A reduction in ozone column densities, which leads to enhanced photochemical activity, reduces ozone levels at ground level. The sensitivity of surface ozone to changes in total ozone is particularly large in the low-NO x regime at Samoa. An anticorrelation between ground level ozone and total ozone is found at the Hohenpeissenberg station both in the observational data and in the model results during wintertime with high NO x levels. Enhanced photochemical activity leads to enhanced ozone production. There is, however, a disagreement between the observed and CTM-modeled sensitivity in surface ozone to ozone column density during the summer months at Hohenpeissenberg. The strong anticorrelation found in the observations, giving increases in surface ozone at low ozone column densities, is not present in the CTM model studies. It is suggested that a correlation between low ozone column densities and stagnant high-pressure systems is an important cause for the observed anticorrelation.