References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-14-6315-2014

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

Shen

¹ ⁷ Liu

¹ Horowitz

L. W.

² Henze

D. K.

³ Fan

² H.

Levy II

² Mauzerall

D. L.

⁴ ⁵ Lin

J.-T.

⁶ Tao

College of Urban and Environmental Sciences, Peking University, Beijing, China

NOAA Geophysical Fluid Dynamics Laboratory, Princeton, NJ, USA

Department of Mechanical Engineering, University of Colorado, Boulder, CO, USA

Woodrow Wilson School of Public and International Affairs, Princeton University, Princeton, NJ, USA

Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ, USA

Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100871, China

now at: Program in Atmospheric and Oceanic Sciences, Princeton University, Princeton, NJ, USA

25 06 2014

14 12 6315 6327

2014

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://acp.copernicus.org/articles/14/6315/2014/acp-14-6315-2014.html

The full text article is available as a PDF file from https://acp.copernicus.org/articles/14/6315/2014/acp-14-6315-2014.pdf

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 removal as well as transport, rather than in emissions, account for the major biases in GEOS-Chem simulations of BC over the North Pacific. 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 (ignoring uncertainties of other factors controlling BC long range transport) suggest that in order to fit HIPPO-3 observations, the aging timescale of anthropogenic BC from EA may be 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 timescale 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 timescale 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.

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