Preprints
https://doi.org/10.5194/egusphere-2023-886
https://doi.org/10.5194/egusphere-2023-886
12 Jun 2023
 | 12 Jun 2023

Biomass-burning smoke properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns

Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Nicole Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg McFarquhar, Jens Redemann, Arther J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema

Abstract. A large part of the uncertainty in climate projections comes from poorly understood or constrained aerosol properties (e.g., particle size, composition, mixing state, aging processes) and aerosol-cloud interactions, as well as the difficulty in remotely sensing them. This is an issue especially in remote regions such as the southeast Atlantic, which exhibits large model spread due to the seasonal coexistence of extensive cloud cover and regional biomass burning smoke. Here we address these gaps by comparing the WRF-CAM5 model to multi-campaign observations (ORACLES, CLARIFY, and LASIC) of the southeastern Atlantic region in August 2017 to evaluate a broad swath of the model’s aerosol properties, processes, and transport, and the degree to which aerosol interactions with clouds are captured. Building on earlier work showing strong performance in model advection and mixing, we find that biomass-burning smoke aerosol size and composition are generally well-captured in the marine free troposphere, except for a likely overprediction of dust in the accumulation mode (7–17 % modeled dust fraction which is not present in the observations). Evaluating smoke aging trends, the model shows a steady increase in aerosol mean diameter and an unchanging composition as smoke ages, deviating from the observed trends that show a rise and subsequent fall in mean diameter over 4–12 days and a decreasing OA : BC ratio beyond 3 days. Both results are likely due to missing processes in the model that remove OA from the particle phase such as photolysis and heterogeneous aerosol chemistry. The observed composition change from the free-troposphere to the marine boundary layer (MBL) is not fully captured in the model, especially the observed enhancement of sulfate from 11 % to 37 % by mean mass fraction in ORACLES, and from 11 % to 26 % in CLARIFY. This points to the importance of properly representing sulfate formation from marine dimethyl sulfide (DMS) emissions and in smoke-free parcels. Additionally, the model does not capture the occurrence of an Aitken mode during clean and medium-smoke conditions in the boundary layer, likely pointing to misrepresentation of new particle formation. The model shows a persistent overprediction of aerosols in the MBL, especially for clean conditions, that multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes the model not representing observed shifts in the aerosol size distribution towards smaller sizes, the model not capturing the relative concentrations of carbon monoxide compared to black carbon, model underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. Average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (~0.65), while it decreases substantially in observations from ORACLES (~0.78) to CLARIFY (~0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD=400–500 cm-3 observed in both ORACLES and CLARIFY and also overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10 and having a bimodal—rather than the observed unimodal—probability distribution of updraft turbulent kinetic energy. We expect these results to motivate similar evaluations of other modeling systems and promote model development in these critical areas to reduce uncertainties in climate simulations.

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Journal article(s) based on this preprint

08 Nov 2023
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023,https://doi.org/10.5194/acp-23-13911-2023, 2023
Short summary
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Nicole Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg McFarquhar, Jens Redemann, Arther J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-886', Anonymous Referee #1, 04 Jul 2023
  • RC2: 'Comment on egusphere-2023-886', Anonymous Referee #2, 04 Jul 2023
  • RC3: 'Comment on egusphere-2023-886', Anonymous Referee #3, 01 Aug 2023
  • AC1: 'Response to referee comments on egusphere-2023-886', Calvin Howes, 12 Sep 2023

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-886', Anonymous Referee #1, 04 Jul 2023
  • RC2: 'Comment on egusphere-2023-886', Anonymous Referee #2, 04 Jul 2023
  • RC3: 'Comment on egusphere-2023-886', Anonymous Referee #3, 01 Aug 2023
  • AC1: 'Response to referee comments on egusphere-2023-886', Calvin Howes, 12 Sep 2023

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by Calvin Howes on behalf of the Authors (13 Sep 2023)  Author's response   Author's tracked changes   Manuscript 
ED: Publish as is (19 Sep 2023) by Annele Virtanen
AR by Calvin Howes on behalf of the Authors (25 Sep 2023)

Journal article(s) based on this preprint

08 Nov 2023
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023,https://doi.org/10.5194/acp-23-13911-2023, 2023
Short summary
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Nicole Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg McFarquhar, Jens Redemann, Arther J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Nicole Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg McFarquhar, Jens Redemann, Arther J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema

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Short summary
To better understand smoke properties and its interactions with clouds, we compare WRF-CAM5 with observations from ORACLES, CLARIFY, and LASIC field campaigns in the Southeastern Atlantic in August 2017. The model transports and mixes smoke well but is not fully capturing some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, new particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.