Indirect effect of sulfate and carbonaceous aerosols: A mechanistic treatment

The indirect effect of anthropogenic aerosols, whereby aerosol particles change cloud optical properties, is the most uncertain component of climate forcing over the past 100 years. Here we use a mechanistic treatment of droplet nucleation and a prognostic treatment of the number of cloud droplets to study the indirect aerosol effect from changes in carbonaceous and sulfate aerosols. Cloud droplet nucleation is parameterized as a function of total aerosol number concentration, updraft velocity, and an activation parameter, which takes into account the mechanism of sulfate aerosol formation. Where previous studies focussed either on sulfate aerosols or carbonaceous aerosols only, here we estimate the combined effect. The combined indirect aerosol effect amounts to −1.1 W m−2 for an internally mixed aerosol and −1.5 W m−2 for an externally mixed aerosol compared to −1.4 W m−2, which we obtained by empirically relating sulfate mass to cloud droplet number. In the case of an internally mixed aerosol, the contribution from increasing carbonaceous and sulfate aerosols is close to being additive as the individual simulations yield an indirect effect of −0.4 W m−2 due to anthropogenic sulfate aerosols and −0.9 W m−2 due to anthropogenic carbonaceous aerosols. The contribution of anthropogenic sulfate to the indirect effect is close to zero if an externally mixed aerosol is assumed, while the contribution of carbonaceous aerosols increases to −1.3 W m−2. The effect of sulfate in the external mixture approach is much smaller than that of carbonaceous aerosols because its burden only increases by a third of that of carbonaceous aerosols and because the mode radius of sulfate is much larger than that of black and organic carbon.

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