Analysis of transpacific transport of black carbon during HIPPO-3: implications for black carbon aging

Abstract - Long-range transport of black carbon (BC) is a growing concern as a result of the efficiency of BC in warming the climate and its adverse impact on human health. We study transpacific transport of BC during HIPPO-3 using a combination of inverse modeling and sensitivity analysis. We use the GEOS-Chem chemical transport model and its adjoint to constrain Asian BC emissions and estimate the source of BC over the North Pacific. We find that different sources of BC dominate the transport to the North Pacific during the southbound (29 March 2010) and northbound (13 April 2010) measurements in HIPPO-3. While biomass burning in Southeast Asia (SE) contributes about 60% of BC in March, more than 90% of BC comes from fossil fuel and biofuel combustion in East Asia (EA) during the April mission. GEOS-Chem simulations generally resolve the spatial and temporal variation of BC concentrations over the North Pacific, but are unable to reproduce the low and high tails of the observed BC distribution. We find that the optimized BC emissions derived from inverse modeling fail to improve model simulations significantly. This failure indicates that uncertainties in BC transport, rather than in emissions, account for the major biases in GEOS-Chem simulations of BC.

The aging process, transforming BC from hydrophobic into hydrophilic form, is one of the key factors controlling wet scavenging and remote concentrations of BC. Sensitivity tests on BC aging suggest that the aging time scale of anthropogenic BC from EA is several hours, faster than assumed in most global models, while the aging process of biomass burning BC from SE may occur much slower, with a time scale of a few days. To evaluate the effects of BC aging and wet deposition on transpacific transport of BC, we develop an idealized model of BC transport. We find that the mid-latitude air masses sampled during HIPPO-3 may have experienced a series of precipitation events, particularly near the EA and SE source region. Transpacific transport of BC is sensitive to BC aging when the aging rate is fast; this sensitivity peaks when the aging time scale is in the range of 1–1.5 d. Our findings indicate that BC aging close to the source must be simulated accurately at a process level in order to simulate better the global abundance and climate forcing of BC.

Shen, Z., J. Liu, L.W. Horowitz, D.K. Henze, S. Fan, H. Levy II, D.L. Mauzerall, J.-T. Lin, & S. Tao (2014) Analysis of transpacific transport of black carbon during HIPPO-3: implications for black carbon aging, Atmospheric Chemistry and Physics (DISCUSSION DRAFT).