Carbonaceous material in aerosol particles in the lower stratosphere and tropopause region

Abstract

The Particle Analysis by Laser Mass Spectrometry (PALMS) instrument has measured the composition of single particles in the lower stratosphere. The average fraction of carbonaceous material in the stratospheric particles decreased rapidly above the tropopause. The decrease in the average carbon content was mostly associated with a sharp increase in the bottom 2 km of the stratosphere in the frequency of fairly pure sulfate particles both with or without meteoric metals. The low potassium content of the fairly pure sulfate particles is used to show that they were formed in the stratosphere and were not tropospheric particles that had lost organics because of oxidation. Of the tropospheric carbonaceous‐sulfate particles found in the stratosphere, the mass spectra had similar patterns from the upper troposphere to the maximum altitude sampled, about 19 km. A reduction in the carbon to sulfate ratio in tropospheric particles was only apparent above about 440 K potential temperature. This implies that carbon compounds can remain for months in particles larger than about 300 nm. Despite the slow rate, these data do not exclude rapid heterogeneous reactions of organics in the particles with OH or other radicals. There was no evidence of significant transfer of semivolatile organics between particles in the stratosphere. However, particles that originated in the stratosphere acquired small amounts of carbon when they were transported to the tropopause.