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Title: Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution

Abstract

Anthropogenic sulfur compounds play an important role in acid deposition, aerosol particle formation, and subsequent radiative forcing and human fine particulate exposure. There are substantial uncertainties in processes influencing sulfate and precursor distributions, however, that have not yet been resolved through comparisons with observations. We find here an underappreciated factor that has a large impact on model results: uncertain emission height. Global aerosol-climate model simulations indicate that the assumed effective anthropogenic emission height is very important to SO2 near-surface concentrations and vertical profile. The global range of near-surface SO2 concentration over land (ocean) due to uncertainty in industrial (international shipping) emission injection height is 81% (76%), relative to the average concentration. This sensitivity is much larger than the uncertainty of SO2 emission rates. Black carbon and primary organic matter concentration and profiles are also sensitive to emission heights (53% over land and 28% over oceans). The impact of emission height uncertainty is larger in winter for land-based emissions, but larger in summer over the Northern Hemisphere ocean for shipping emissions. The variation in aerosol optical depth related to shipping emission injection heights is 11% over oceans, revealing the potential importance of injection height on aerosol forcing and climatic effects. Themore » large impact on SO2 concentrations can confound attempts to use surface, aircraft, and satellite observations to constrain the importance of other processes that govern sulfur compound distributions in the atmosphere. In conclusion, the influence of emission height on vertical SO2 column also will impact the accuracy of satellite retrievals.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), College Park, MD (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1528914
Alternate Identifier(s):
OSTI ID: 1510106; OSTI ID: 1543308
Report Number(s):
PNNL-SA-137329
Journal ID: ISSN 2169-897X
Grant/Contract Number:  
AC05‐76RL01830; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 124; Journal Issue: 8; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; aerosol; injection height; emission; model

Citation Formats

Yang, Yang, Smith, Steven J., Wang, Hailong, Lou, Sijia, and Rasch, Philip J. Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution. United States: N. p., 2019. Web. doi:10.1029/2018JD030001.
Yang, Yang, Smith, Steven J., Wang, Hailong, Lou, Sijia, & Rasch, Philip J. Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution. United States. doi:10.1029/2018JD030001.
Yang, Yang, Smith, Steven J., Wang, Hailong, Lou, Sijia, and Rasch, Philip J. Sat . "Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution". United States. doi:10.1029/2018JD030001. https://www.osti.gov/servlets/purl/1528914.
@article{osti_1528914,
title = {Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution},
author = {Yang, Yang and Smith, Steven J. and Wang, Hailong and Lou, Sijia and Rasch, Philip J.},
abstractNote = {Anthropogenic sulfur compounds play an important role in acid deposition, aerosol particle formation, and subsequent radiative forcing and human fine particulate exposure. There are substantial uncertainties in processes influencing sulfate and precursor distributions, however, that have not yet been resolved through comparisons with observations. We find here an underappreciated factor that has a large impact on model results: uncertain emission height. Global aerosol-climate model simulations indicate that the assumed effective anthropogenic emission height is very important to SO2 near-surface concentrations and vertical profile. The global range of near-surface SO2 concentration over land (ocean) due to uncertainty in industrial (international shipping) emission injection height is 81% (76%), relative to the average concentration. This sensitivity is much larger than the uncertainty of SO2 emission rates. Black carbon and primary organic matter concentration and profiles are also sensitive to emission heights (53% over land and 28% over oceans). The impact of emission height uncertainty is larger in winter for land-based emissions, but larger in summer over the Northern Hemisphere ocean for shipping emissions. The variation in aerosol optical depth related to shipping emission injection heights is 11% over oceans, revealing the potential importance of injection height on aerosol forcing and climatic effects. The large impact on SO2 concentrations can confound attempts to use surface, aircraft, and satellite observations to constrain the importance of other processes that govern sulfur compound distributions in the atmosphere. In conclusion, the influence of emission height on vertical SO2 column also will impact the accuracy of satellite retrievals.},
doi = {10.1029/2018JD030001},
journal = {Journal of Geophysical Research: Atmospheres},
number = 8,
volume = 124,
place = {United States},
year = {2019},
month = {4}
}

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