The lifetimes and potential change in planetary albedo owing to the oxidation of thin surfactant organic films extracted from atmospheric aerosol by hydroxyl (OH) radicals at the air–water interface of particles

Abstract. Water-insoluble organic material extracted from atmospheric aerosol samples collected in urban (Royal Holloway, University of London, UK) and remote (Halley Research Station, Antarctica) locations were shown to form stable thin surfactant films at an air–water interface. These organic films reacted quickly with gas-phase OH radicals and may impact planetary albedo. The X-ray reflectivity measurements additionally indicate that the film may be consistent with having a structure with increased electron density of film molecules towards the water, suggesting amphiphilic behaviour. Assuming the material extracted from atmospheric aerosol produces thin films on aqueous particles and cloud droplets, modelling the oxidation kinetics with a kinetic model of aerosol surface and bulk chemistry (KM-SUB) suggests half-lives of minutes to an hour and values of ksurf of ∼2×10-7 and ∼5×10-5 cm2 s−1 for urban and remote aerosol film extracts, respectively. The superfluous half-lives calculated at typical OH atmospheric ambient mixing ratios are smaller than the typical residence time of atmospheric aerosols; thus, oxidation of organic material should be considered in atmospheric modelling. Thin organic films at the air–water interface of atmospheric aerosol or cloud droplets may alter the light-scattering properties of the aerosol. X-ray reflectivity measurements of atmospheric aerosol film material at the air–water interface resulted in calculated film thickness values to be either ∼10 or ∼17 Å for remote or urban aerosol extracts, respectively, and oxidation did not remove the films completely. One-dimensional radiative transfer modelling suggests the oxidation of thin organic films on atmospheric particles by OH radicals may reduce the planetary albedo by a small, but potentially significant, amount.