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Title: Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models

Abstract

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 ( 137Cs) and xenon-133 ( 133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions ofmore » 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τ e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τ e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer ( 133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol ( 137Cs) tracer. As a result, this indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.« less

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [4];  [2]; ORCiD logo [5];  [6];  [7];  [8];  [9]; ORCiD logo [10];  [11]; ORCiD logo [12];  [9];  [9];  [9];  [9];  [13];  [14] more »;  [14];  [15]; ORCiD logo [16];  [10];  [10];  [11];  [3];  [17]; ORCiD logo [2]; ORCiD logo [8];  [6];  [15] « less
  1. NILU - Norwegian Institute for Air Research, Kjeller (Norway)
  2. Norwegian Meteorological Institute, Oslo (Norway)
  3. Dalhousie Univ., Halifax (Canada)
  4. Center for International Climate and Environmental Research - Oslo (CICERO), Oslo (Norway)
  5. The Cyprus Institute, Nicosia (Cyprus)
  6. Univ. of Mainz, Mainz (Germany)
  7. Met Office, Exeter (United Kingdom)
  8. Duke Univ., Durham, NC (United States)
  9. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  10. Columbia Univ. and NASA Goddard Institute for Space Studies, New York, NY (United States)
  11. Finnish Meteorological Institute, Kuopio (Finland)
  12. NILU - Norwegian Institute for Air Research, Kjeller (Norway); CEA-CNRS-UVSQ, Gif-sur-Yvette (France)
  13. Univ. of Wyoming, Laramie, WY (United States)
  14. Univ. of L'Aquila, L'Aquila (Italy)
  15. Chinese Meteorological Administration, Beijing (China)
  16. CEA-CNRS-UVSQ, Gif-sur-Yvette (France)
  17. Colorado State Univ., Fort Collins, CO (United States); Dalhousie Univ., Halifax (Canada)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1254571
Report Number(s):
PNNL-SA-112717
Journal ID: ISSN 1680-7324; KP1703020
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 16; Journal Issue: 5; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Kristiansen, N. I., Stohl, A., Olivie, D. J. L., Croft, B., Sovde, O. A., Klein, H., Christoudias, T., Kunkel, D., Leadbetter, S. J., Lee, Y. H., Zhang, K., Tsigaridis, K., Bergman, T., Evangeliou, N., Wang, H., Ma, P. -L., Easter, R. C., Rasch, P. J., Liu, X., Pitari, G., Di Genova, G., Zhao, S. Y., Balkanski, Y., Bauer, S. E., Faluvegi, G. S., Kokkola, H., Martin, R. V., Pierce, J. R., Schulz, M., Shindell, D., Tost, H., and Zhang, H. Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models. United States: N. p., 2016. Web. doi:10.5194/acp-16-3525-2016.
Kristiansen, N. I., Stohl, A., Olivie, D. J. L., Croft, B., Sovde, O. A., Klein, H., Christoudias, T., Kunkel, D., Leadbetter, S. J., Lee, Y. H., Zhang, K., Tsigaridis, K., Bergman, T., Evangeliou, N., Wang, H., Ma, P. -L., Easter, R. C., Rasch, P. J., Liu, X., Pitari, G., Di Genova, G., Zhao, S. Y., Balkanski, Y., Bauer, S. E., Faluvegi, G. S., Kokkola, H., Martin, R. V., Pierce, J. R., Schulz, M., Shindell, D., Tost, H., & Zhang, H. Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models. United States. doi:10.5194/acp-16-3525-2016.
Kristiansen, N. I., Stohl, A., Olivie, D. J. L., Croft, B., Sovde, O. A., Klein, H., Christoudias, T., Kunkel, D., Leadbetter, S. J., Lee, Y. H., Zhang, K., Tsigaridis, K., Bergman, T., Evangeliou, N., Wang, H., Ma, P. -L., Easter, R. C., Rasch, P. J., Liu, X., Pitari, G., Di Genova, G., Zhao, S. Y., Balkanski, Y., Bauer, S. E., Faluvegi, G. S., Kokkola, H., Martin, R. V., Pierce, J. R., Schulz, M., Shindell, D., Tost, H., and Zhang, H. Thu . "Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models". United States. doi:10.5194/acp-16-3525-2016. https://www.osti.gov/servlets/purl/1254571.
@article{osti_1254571,
title = {Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models},
author = {Kristiansen, N. I. and Stohl, A. and Olivie, D. J. L. and Croft, B. and Sovde, O. A. and Klein, H. and Christoudias, T. and Kunkel, D. and Leadbetter, S. J. and Lee, Y. H. and Zhang, K. and Tsigaridis, K. and Bergman, T. and Evangeliou, N. and Wang, H. and Ma, P. -L. and Easter, R. C. and Rasch, P. J. and Liu, X. and Pitari, G. and Di Genova, G. and Zhao, S. Y. and Balkanski, Y. and Bauer, S. E. and Faluvegi, G. S. and Kokkola, H. and Martin, R. V. and Pierce, J. R. and Schulz, M. and Shindell, D. and Tost, H. and Zhang, H.},
abstractNote = {Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. As a result, this indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.},
doi = {10.5194/acp-16-3525-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 5,
volume = 16,
place = {United States},
year = {2016},
month = {3}
}

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