The method of variational adjoint data assimilation has been applied to assimilate chemistry observations into a comprehensive tropospheric gas phase model. The rationale of this method is to find the correct initial values for a subsequent atmospheric chemistry model run when observations scattered in time are available. The variational adjoint technique is esteemed to be a promising tool for future advanced meteorological forecasting. The stimulating experience gained with the application of four-dimensional variational data assimilation in this research area has motivated the attempt to apply the technique to air quality modeling and analysis of the chemical state of the atmosphere. The present study describes the development and application of the adjoint of the second-generation regional acid deposition model gas phase mechanism, which is used in the European air pollution dispersion model system. Performance results of the assimilation scheme using both model-generated data and real observations are presented for tropospheric conditions. In the former case it is demonstrated that time series of only few or even one measured key species convey sufficient information to improve considerably the analysis of unobserved species which are directly coupled with the observed species. In the latter case a Lagrangian approach is adopted where trajectory calculations between two comprehensively furnished measurement sites are carried out. The method allows us to analyze initial data for air pollution modeling even when only sparse observations are available. Besides remarkable improvements of the model performance by properly analyzed initial concentrations, it is shown that the adjoint algorithm offers the feasibility to estimate the sensitivity of ozone concentrations relative to its precursors.¿ 1997 American Geophysical Union