title: Potential climatic impact of organic haze on early Earth.
abstract: We have explored the direct and indirect radiative effects on climate of organic particles likely to have been present on early Earth by measuring their hygroscopicity and cloud nucleating ability. The early Earth analog aerosol particles were generated via ultraviolet photolysis of an early Earth analog gas mixture, which was designed to mimic possible atmospheric conditions before the rise of oxygen. An analog aerosol for the present-day atmosphere of Saturn's moon Titan was tested for comparison. We exposed the early Earth aerosol to a range of relative humidities (RHs). Water uptake onto the aerosol was observed to occur over the entire RH range tested (RH=80-87%). To translate our measurements of hygroscopicity over a specific range of RHs into their water uptake ability at any RH < 100% and into their ability to act as cloud condensation nuclei (CCN) at RH > 100%, we relied on the hygroscopicity parameter κ, developed by Petters and Kreidenweis. We retrieved κ=0.22 ±0.12 for the early Earth aerosol, which indicates that the humidified aerosol (RH < 100 %) could have contributed to a larger antigreenhouse effect on the early Earth atmosphere than previously modeled with dry aerosol. Such effects would have been of significance in regions where the humidity was larger than 50%, because such high humidities are needed for significant amounts of water to be on the aerosol. Additionally, Earth organic aerosol particles could have activated into CCN at reasonable-and even low-water-vapor supersaturations (RH > 100%). In regions where the haze was dominant, it is expected that low particle concentrations, once activated into cloud droplets, would have created short-lived, optically thin clouds. Such clouds, if predominant on early Earth, would have had a lower albedo than clouds today, thereby warming the planet relative to current-day clouds.
authors.affiliation: Department of Atmospheric and Oceanic Sciences, University of Colorado, Boulder, Colorado 80309, USA. Christa.Hasenkopf@colorado.edu
authors.forename: Christa A
authors.initials: CA
authors.lastname: Hasenkopf
authors.forename: Miriam A
authors.initials: MA
authors.lastname: Freedman
authors.forename: Melinda R
authors.initials: MR
authors.lastname: Beaver
authors.forename: Owen B
authors.initials: OB
authors.lastname: Toon
authors.forename: Margaret A
authors.initials: MA
authors.lastname: Tolbert
mesh_terms: D000336:Aerosols / Q000737:chemistry; D001272:Atmosphere / Q000737:chemistry*; D002980:Climate; D003198:Computer Simulation; D004391:Dust; D018534:Earth, Planet; D006813:Humidity; D010316:Particle Size; D052638:Particulate Matter / Q000737:chemistry
chemical_list: D000336:Aerosols; D004391:Dust; D052638:Particulate Matter