Direct radiative forcing of anthropogenic organic aerosol

This study simulates the direct radiative forcing of organic aerosol using the GFDL AM2 GCM. The aerosol climatology is provided by the MOZART chemical transport model (CTM). The approach to calculating aerosol optical properties explicitly considers relative humidity-dependent hygroscopic growth by employing a functional group-based thermodynamic model, and makes use of the size distribution derived from AERONET measurements. The preindustrial (PI) and present-day (PD) global burdens of organic carbon are 0.17 and 1.36 Tg OC, respectively. The annual global mean total-sky and clear-sky top-of-the atmosphere (TOA) forcings (PI to PD) are estimated as -0.34 and -0.71 W m^-2, respectively. Geographically the radiative cooling largely lies over the source regions, namely part of South America, Central Africa, Europe and South and East Asia. The annual global mean total-sky and clear-sky surface forcings are -0.63 and -0.98 W m^-2, respectively. A series of sensitivity analyses shows that the treatments of hygroscopic growth and optical properties of organic aerosol are intertwined in the determination of the global organic aerosol forcing. For example, complete deprivation of water uptake by hydrophilic organic particles reduces the standard (total-sky) and clear-sky TOA forcing estimates by 18% and 20%, respectively, while the uptake by a highly soluble organic compound (malonic acid) enhances them by 18% and 32%, respectively. Treating particles as non-absorbing enhances aerosol reflection and increases the total-sky and clear-sky TOA forcing by 47% and 18%, respectively, while neglecting the scattering brought about by the water associated with particles reduces them by 24% and 7%, respectively.