J. Geophys. Res.

[1] This study with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform investigates the aerosol elemental concentrations at 9-11 km altitude in the northern hemisphere. Measurements from 31 intercontinental flights over a 2-year period between Germany and Sri Lanka/Maldives in the Indian Ocean are presented. Aerosol samples were collected with an impaction technique and were analyzed for the concentration of 18 elements using particle-induced X-ray emission (PIXE). Additional measurements of particle number concentrations, ozone and carbon monoxide concentrations, and meteorological modeling were included in the interpretation of the aerosol elemental concentrations. Particulate sulphur was found to be by far the most abundant element. Its upper tropospheric concentration increased, on average, by a factor of 2 from the tropics to midlatitudes, with another factor 2 higher concentrations in the lowermost stratosphere over midlatitudes. Correlation patterns and source profiles suggest contributions from crustal sources and biomass burning, but not from meteor ablation. Coinciding latitudinal gradients in particulate sulphur concentrations and emissions suggest that fossil fuel combustion is an important source of the aerosol in the upper troposphere and lowermost stratosphere. The measurements indicate aerosol transport along isentropic surfaces across the tropopause into the lowermost stratosphere. As a result of the prolonged residence time, ageing via oxidation of sulphur dioxide in the lowermost stratosphere was found to be a likely high-altitude, strong source that, along with downward transport of stratospheric air, could explain the vertical gradient of particulate sulphur mass concentration around the extratropical tropopause