An evaluation of global organic aerosol schemes using airborne observations
Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different...
| Main Authors: | , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
Copernicus GmbH
2020
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| Online Access: | https://hdl.handle.net/1721.1/125765 |
| _version_ | 1826203212967837696 |
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| author | Pai, Sidhant J. Heald, Colette L. Pierce, Jeffrey R. Farina, Salvatore C. Marais, Eloise A. Jimenez, Jose L. Campuzano-Jost, Pedro Nault, Benjamin A. Middlebrook, Ann M. Coe, Hugh Shilling, John E. Bahreini, Roya Dingle, Justin H. Vu, Kennedy |
| author2 | Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences |
| author_facet | Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Pai, Sidhant J. Heald, Colette L. Pierce, Jeffrey R. Farina, Salvatore C. Marais, Eloise A. Jimenez, Jose L. Campuzano-Jost, Pedro Nault, Benjamin A. Middlebrook, Ann M. Coe, Hugh Shilling, John E. Bahreini, Roya Dingle, Justin H. Vu, Kennedy |
| author_sort | Pai, Sidhant J. |
| collection | MIT |
| description | Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally distributed airborne campaigns from 2008 to 2017, primarily in the spring and summer seasons. These include the ATom, KORUS-AQ, GoAmazon, FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric composition regimes - anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA - a "simple scheme" that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation and a "complex scheme" that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44, respectively). The simple scheme displays greater skill in minimizing the overall model bias (with a normalized mean bias of 0.04 compared to 0.30 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within the GEOS-Chem model. However, there are significant differences in model performance across different chemical source regimes, classified here into seven categories. Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. Our analysis suggests that a semi-volatile treatment of POA is superior to a non-volatile treatment. It is also likely that the complex scheme parameterization overestimates biogenic SOA at the global scale. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias, such as emissions, transport and deposition, that are exogenous to the OA chemical scheme. |
| first_indexed | 2024-09-23T12:33:26Z |
| format | Article |
| id | mit-1721.1/125765 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T12:33:26Z |
| publishDate | 2020 |
| publisher | Copernicus GmbH |
| record_format | dspace |
| spelling | mit-1721.1/1257652022-10-01T09:45:54Z An evaluation of global organic aerosol schemes using airborne observations Pai, Sidhant J. Heald, Colette L. Pierce, Jeffrey R. Farina, Salvatore C. Marais, Eloise A. Jimenez, Jose L. Campuzano-Jost, Pedro Nault, Benjamin A. Middlebrook, Ann M. Coe, Hugh Shilling, John E. Bahreini, Roya Dingle, Justin H. Vu, Kennedy Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Massachusetts Institute of Technology. Department of Civil and Environmental Engineering Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally distributed airborne campaigns from 2008 to 2017, primarily in the spring and summer seasons. These include the ATom, KORUS-AQ, GoAmazon, FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric composition regimes - anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA - a "simple scheme" that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation and a "complex scheme" that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44, respectively). The simple scheme displays greater skill in minimizing the overall model bias (with a normalized mean bias of 0.04 compared to 0.30 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within the GEOS-Chem model. However, there are significant differences in model performance across different chemical source regimes, classified here into seven categories. Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. Our analysis suggests that a semi-volatile treatment of POA is superior to a non-volatile treatment. It is also likely that the complex scheme parameterization overestimates biogenic SOA at the global scale. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias, such as emissions, transport and deposition, that are exogenous to the OA chemical scheme. National Science Foundation (AGS-1564495) 2020-06-11T16:24:29Z 2020-06-11T16:24:29Z 2020-03 2019-12 2020-05-27T17:53:37Z Article http://purl.org/eprint/type/JournalArticle 1680-7324 https://hdl.handle.net/1721.1/125765 Pai, Sidhant J. et al. "An evaluation of global organic aerosol schemes using airborne observations." Atmospheric Chemistry and Physics 20, 5 (March 2020): 2637–2665 © 2020 BMJ Publishing Group en http://dx.doi.org/10.5194/acp-20-2637-2020 Atmospheric Chemistry and Physics Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf Copernicus GmbH Copernicus Publications |
| spellingShingle | Pai, Sidhant J. Heald, Colette L. Pierce, Jeffrey R. Farina, Salvatore C. Marais, Eloise A. Jimenez, Jose L. Campuzano-Jost, Pedro Nault, Benjamin A. Middlebrook, Ann M. Coe, Hugh Shilling, John E. Bahreini, Roya Dingle, Justin H. Vu, Kennedy An evaluation of global organic aerosol schemes using airborne observations |
| title | An evaluation of global organic aerosol schemes using airborne observations |
| title_full | An evaluation of global organic aerosol schemes using airborne observations |
| title_fullStr | An evaluation of global organic aerosol schemes using airborne observations |
| title_full_unstemmed | An evaluation of global organic aerosol schemes using airborne observations |
| title_short | An evaluation of global organic aerosol schemes using airborne observations |
| title_sort | evaluation of global organic aerosol schemes using airborne observations |
| url | https://hdl.handle.net/1721.1/125765 |
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