Long-range transport of black carbon to the Pacific Ocean and its dependence on aging timescale

Abstract

Improving the ability of global models to predict concentrations of black carbon (BC) over the Pacific Ocean is essential to evaluate the impact of BC on marine climate. In this study, we tag BC tracers from 13 source regions around the globe in a global chemical transport model MOZART-4. Numerous sensitivity simulations are carried out varying the aging timescale of BC emitted from each source region. The aging timescale for each source region is optimized by minimizing errors in vertical profiles of BC mass mixing ratios between simulations and HIAPER Pole-to-Pole Observations (HIPPO). For most HIPPO deployments, in the Northern Hemisphere, optimized aging timescales are less than half a day for BC emitted from tropical and mid-latitude source regions, and about 1 week for BC emitted from high latitude regions in all seasons except summer. We find that East Asian emissions contribute most to the BC loading over the North Pacific, while South American, African and Australian emissions dominate BC loadings over the South Pacific. Dominant source regions contributing to BC loadings in other parts of the globe are also assessed. The lifetime of BC originating from East Asia (i.e., the world's largest BC emitter) is found to be only 2.2 days, much shorter than the global average lifetime of 4.9 days, making East Asia's contribution to global burden only 36% of BC from the second largest emitter, Africa. Thus, evaluating only relative emission rates without accounting for differences in aging timescales and deposition rates is not predictive of the contribution of a given source region to climate impacts. Our simulations indicate that lifetime of BC increases nearly linearly with aging timescale for all source regions. When aging rate is fast, the lifetime of BC is largely determined by factors that control local deposition rates (e.g. precipitation). The sensitivity of lifetime to aging timescale depends strongly on the initial hygroscopicity of freshly emitted BC. Our findings suggest that the aging timescale of BC varies significantly by region and season, and can strongly influence the contribution of source regions to BC burdens around the globe. Improving parameterizations of the aging process for BC is important for enhancing the predictive skill of air quality and climate models. Future observations that investigate the evolution of hygroscopicity of BC as it ages from different source regions to the remote atmosphere are urgently needed.