Ultrafine particles (UFP) in the atmosphere may have significant impacts on the regional water and radiation budgets through secondary effects on cloud microphysics. Yet, as these particles are invisible for current remote sensing techniques, knowledge about their three-dimensional distribution, source strengths and budgets is limited. Building on a 40-yr-old Australia-wide airborne survey which provides a reference case study of aerosol sources and budgets, this study presents results from a new airborne survey over Eastern Australia, northern New South Wales and Queensland. Observations identified apparent changes in the number and distribution of major anthropogenic aerosol sources since the early 1970s, which might relate to the simultaneously observed changes in rainfall patterns over eastern Queensland. Coal-fired power stations in the inland areas between Brisbane and Rockhampton were clearly identified as the major sources for ultrafine particulate matter. Sugar mills, smelters and shipping along the coast close to the Ports of Townsville and Rockhampton were comparable minor sources. Airborne Lagrangian plume studies were a ... mehrpplied to investigate source strength and ageing properties within power station plumes. Significant changes observed, compared to the measurements in the 1970s, included a significant increase in the number concentration of UFP related to coal-fired power station emissions in the sparsely populated Queensland hinterland coincident with the area with the most pronounced reduction in rainfall.