1. Department of Civil & Environmental Engineering, Stanford University, Stanford, California 94305-4020, USA

Correspondence to: Correspondence and requests for information should be addressed to author (e-mail: Email: jacobson@ce.stanford.edu).

Aerosols affect the Earth's temperature and climate by altering the radiative properties of the atmosphere. A large positive component of this radiative forcing from aerosols is due to black carbon—soot—that is released from the burning of fossil fuel and biomass, and, to a lesser extent, natural fires, but the exact forcing is affected by how black carbon is mixed with other aerosol constituents. From studies of aerosol radiative forcing, it is known that black carbon can exist in one of several possible mixing states; distinct from other aerosol particles (externally mixed^{1, 2, 3, 4, 5, 6, 7}) or incorporated within them (internally mixed^{1, 3, 7}), or a black-carbon core could be surrounded by a well mixed shell⁷. But so far it has been assumed that aerosols exist predominantly as an external mixture. Here I simulate the evolution of the chemical composition of aerosols, finding that the mixing state and direct forcing of the black-carbon component approach those of an internal mixture, largely due to coagulation and growth of aerosol particles. This finding implies a higher positive forcing from black carbon than previously thought, suggesting that the warming effect from black carbon may nearly balance the net cooling effect of other anthropogenic aerosol constituents. The magnitude of the direct radiative forcing from black carbon itself exceeds that due to CH₄, suggesting that black carbon may be the second most important component of global warming after CO₂ in terms of direct forcing.