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Observing system experiments are presented to characterise impacts of surface and vertical profile measurements on aerosol analysis and forecast skill. A three-dimensional (3D) variational data assimilation system is implemented within the Weather Research and Forecasting/Chemistry model, and the control variables consist of eight species of the Model for Simulation Aerosol Interactions and Chemistry scheme. In the experiments, the 3D profiles of aircraft speciated observations and surface concentration observations acquired during the California Research at the Nexus of Air Quality and Climate Change field campaign are assimilated. The data assimilation experiments are performed at 02:00 local time 2 June 2010, and surface observations at 02:00 and aircraft observations from 01:30 to 02:30 local time are assimilated. The results show that the assimilation of both aircraft and surface observations improves the subsequent forecasts. The improved forecast skill resulting from the assimilation of the aircraft profiles persists a time longer than the assimilation of the surface observations, which suggests the necessity of vertical profile observations for extending aerosol forecasting time. [ABSTRACT FROM AUTHOR]