Sensitivity of sulfate direct climate forcing to the hysteresis of particle phase transitions

The effects of solid-aqueous phase transitions on sulfate direct climate forcing (SDCF) are investigated by using both a column model and a global chemical transport model. Aqueous particles have a larger mass extinction efficiency but a smaller backscattered fraction than their solid counterparts. The column model shows that the hysteresis of the phase transition can result in an uncertainty in the SDCF of 20%. The global chemical transport model explicitly accounts for the relative humidity processing of particles and the associated hysteresis. The model also treats the extent of sulfate neutralization by ammonia. For the anthropogenic sulfate, the base case simulation finds that solid particles contribute 41% of the global burden, 26% of the clear-sky optical thickness, 31% of the clear-sky SDCF, and 37% of the full-sky SDCF, a trend that reflects the correlation of solid particles with clear skies. A perturbation to the model, omitting hysteresis by assuming that all particles are aqueous, results in an overestimate of the SDCF by +8% compared to the base case. A converse assumption that crystallization occurs at the deliquescence relative humidity underestimates the SDCF by -8%. A case that assumes that aqueous particles occur whenever the ambient relative humidity exceeds the crystallization relative humidity biases the SDCF by +5%. A case that includes hysteresis but omits the difference in the fraction of radiation backscattered to space by aqueous compared to solid particles changes the SDCF by +15%. Seasonal and regional differences can be much larger. We recommend that the ratio of the sulfate aerosol optical thickness calculated with versus without consideration of particle hygroscopicity be reported as a standard output of SDCF models to facilitate meaningful intercomparisons among different models.