Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

Dedrick, Jeramy L.; Pelayo, Christian N.; Russell, Lynn M.; Lubin, Dan; Mülmenstädt, Johannes H.; Miller, Mark

doi:10.1073/pnas.2412247122

Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

Journal Article · Mon Mar 24 00:00:00 EDT 2025 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.2412247122· OSTI ID:2536746

^[1]; Pelayo, Christian N. ^[1]; ^[1]; Lubin, Dan ^[1]; ^[2]; ^[3]

University of California, San Diego, La Jolla, CA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Rutgers University, New Brunswick, NJ (United States)

The Twomey effect brightens clouds by increasing aerosol concentrations, which activates more droplets and decreases cloud supersaturation in response to more competition for water vapor. To quantify this competition response, we used marine low cloud observations in clean and smoky conditions at Ascension Island in the tropical South Atlantic during the Layered Aerosol Smoke Interactions with Cloud (LASIC) campaign. These observations show similar increases in droplet number for increased accumulation-mode particles from surface-based and satellite cloud retrievals, demonstrating the importance of below-cloud aerosol measurements for retrieving aerosol–cloud interactions (ACI) in clean and smoky aerosol conditions. Four methods for estimating cloud supersaturation from aerosol–cloud measurements were compared, with cloud scene-based and parcel-based methods showing sufficient variability for a strong dependence on both aerosol accumulation number concentration and cloud-base updraft velocities. Decomposing aerosol-related changes in cloud albedo and optical depth shows the calculated competition response accounts for dampening the activation response by 12 to 35%, explaining the diminished Twomey effect at high aerosol concentrations observed for smoky conditions at LASIC and previously around the world. This result was consistent for independent supersaturation retrievals by cloud scene-based droplet number and cloud condensation nuclei and parcel-based multimode size-resolving Lagrangian methods. Translating aerosol effects to local radiative forcing with clean conditions as a proxy for preindustrial and smoky conditions for present-day showed that the competition response reduces cooling from the Twomey radiative forcing by 12 to 35%, providing an essential process-specific constraint for improving the representation of aerosol competition in climate model simulation of indirect aerosol forcing.

View Journal Article

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; FG02-08ER64531; SC0021045

OSTI ID:: 2536746

Alternate ID(s):: OSTI ID: 2555849

Report Number(s):: PNNL-SA--201338

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 13 Vol. 122; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (64)

Natural aerosol–climate feedbacks suppressed by anthropogenic aerosol Spracklen, D. V.; Rap, A. Geophysical Research Letters, Vol. 40, Issue 19 https://doi.org/10.1002/2013GL057966	journal	October 2013
Twomey effect observed from collocated microphysical and remote sensing measurements over shallow cumulus Werner, F.; Ditas, F.; Siebert, H. Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 3 https://doi.org/10.1002/2013JD020131	journal	February 2014
Linear relation between convective cloud base height and updrafts and application to satellite retrievals: SATELLITE RETRIEVAL OF CLOUD UPDRAFTS Zheng, Youtong; Rosenfeld, Daniel Geophysical Research Letters, Vol. 42, Issue 15 https://doi.org/10.1002/2015GL064809	journal	August 2015
New understanding and quantification of the regime dependence of aerosol-cloud interaction for studying aerosol indirect effects: Aerosol-Cloud Interaction Regimes Chen, Jingyi; Liu, Yangang; Zhang, Minghua Geophysical Research Letters, Vol. 43, Issue 4 https://doi.org/10.1002/2016GL067683	journal	February 2016
The global aerosol‐cloud first indirect effect estimated using MODIS, MERRA, and AeroCom McCoy, D. T.; Bender, F. A. ‐M.; Mohrmann, J. K. C. Journal of Geophysical Research: Atmospheres, Vol. 122, Issue 3 https://doi.org/10.1002/2016JD026141	journal	February 2017
The Ascension Island Boundary Layer in the Remote Southeast Atlantic is Often Smoky Zuidema, Paquita; Sedlacek, Arthur J.; Flynn, Connor Geophysical Research Letters, Vol. 45, Issue 9 https://doi.org/10.1002/2017GL076926	journal	May 2018
The Radiative Forcing of Aerosol–Cloud Interactions in Liquid Clouds: Wrestling and Embracing Uncertainty Mülmenstädt, Johannes; Feingold, Graham Current Climate Change Reports, Vol. 4, Issue 1 https://doi.org/10.1007/s40641-018-0089-y	journal	February 2018
Classification of aerosol-cloud interaction regimes over Tokyo Misumi, Ryohei; Uji, Yasushi; Miura, Kazuhiko Atmospheric Research, Vol. 272 https://doi.org/10.1016/j.atmosres.2022.106150	journal	July 2022
Sensitivity of cloud microphysics to aerosol is highly associated with cloud water content: Implications for indirect radiative forcing Wang, Yuan; Jia, Hailing; Zhang, Ping Atmospheric Research, Vol. 309 https://doi.org/10.1016/j.atmosres.2024.107552	journal	October 2024
Physics and Chemistry of Clouds Lamb, Dennis; Verlinde, Johannes Cambridge University Press https://doi.org/10.1017/CBO9780511976377	book	January 2011
Aerosol dynamics in ship tracks Russell, Lynn M.; Seinfeld, John H.; Flagan, Richard C. Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D24, p. 31077-31095 https://doi.org/10.1029/1999JD900985	journal	December 1999
A parameterization of aerosol activation: 2. Multiple aerosol types Abdul-Razzak, Hayder; Ghan, Steven J. Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D5 https://doi.org/10.1029/1999JD901161	journal	March 2000
Parameterization of cloud droplet formation in global climate models Nenes, Athanasios Journal of Geophysical Research, Vol. 108, Issue D14 https://doi.org/10.1029/2002JD002911	journal	January 2003
Effects of varying aerosol regimes on low-level Arctic stratus: AEROSOL EFFECTS ON ARCTIC STRATUS Garrett, T. J.; Zhao, C.; Dong, X. Geophysical Research Letters, Vol. 31, Issue 17 https://doi.org/10.1029/2004GL019928	journal	September 2004
Evaluation of the aerosol indirect effect in marine stratocumulus clouds: Droplet number, size, liquid water path, and radiative impact Twohy, Cynthia H. Journal of Geophysical Research, Vol. 110, Issue D8 https://doi.org/10.1029/2004JD005116	journal	January 2005
Satellite-based estimate of the direct and indirect aerosol climate forcing: SATELLITE-ESTIMATE OF AEROSOL FORCINGS Quaas, Johannes; Boucher, Olivier; Bellouin, Nicolas Journal of Geophysical Research: Atmospheres, Vol. 113, Issue D5 https://doi.org/10.1029/2007JD008962	journal	March 2008
Lack of correlation between chlorophyllaand cloud droplet effective radius in shallow marine clouds Miller, Matthew A.; Yuter, Sandra E. Geophysical Research Letters, Vol. 35, Issue 13 https://doi.org/10.1029/2008GL034354	journal	July 2008
An assessment of aerosol‐cloud interactions in marine stratus clouds based on surface remote sensing McComiskey, Allison; Feingold, Graham; Frisch, A. Shelby Journal of Geophysical Research, Vol. 114, Issue D9 https://doi.org/10.1029/2008JD011006	journal	January 2009
On the link between ocean biota emissions, aerosol, and maritime clouds: Airborne, ground, and satellite measurements off the coast of California: OCEAN EMISSIONS, AEROSOL, AND CLOUDS Sorooshian, Armin; Padró, Luz T.; Nenes, Athanasios Global Biogeochemical Cycles, Vol. 23, Issue 4 https://doi.org/10.1029/2009GB003464	journal	October 2009
Analysis of aerosol-cloud interaction from multi-sensor satellite observations: AEROSOL-CLOUD INTERACTION FROM SPACE Costantino, Lorenzo; Bréon, François-Marie Geophysical Research Letters, Vol. 37, Issue 11 https://doi.org/10.1029/2009GL041828	journal	June 2010
Remote Sensing of Droplet Number Concentration in Warm Clouds: A Review of the Current State of Knowledge and Perspectives Grosvenor, Daniel P.; Sourdeval, Odran; Zuidema, Paquita Reviews of Geophysics, Vol. 56, Issue 2 https://doi.org/10.1029/2017RG000593	journal	June 2018
Substantial Cloud Brightening From Shipping in Subtropical Low Clouds Diamond, Michael S.; Director, Hannah M.; Eastman, Ryan AGU Advances, Vol. 1, Issue 1 https://doi.org/10.1029/2019AV000111	journal	March 2020
Distinct Impacts of Increased Aerosols on Cloud Droplet Number Concentration of Stratus/Stratocumulus and Cumulus Jia, H.; Ma, X.; Yu, F. Geophysical Research Letters, Vol. 46, Issue 22 https://doi.org/10.1029/2019GL085081	journal	November 2019
Bounding global aerosol radiative forcing of climate change Bellouin, N.; Quaas, J.; Gryspeerdt, E. Reviews of Geophysics https://doi.org/10.1029/2019RG000660	journal	November 2019
Characterization of Aerosol Hygroscopicity Over the Northeast Pacific Ocean: Impacts on Prediction of CCN and Stratocumulus Cloud Droplet Number Concentrations Schulze, B. C.; Charan, S. M.; Kenseth, C. M. Earth and Space Science, Vol. 7, Issue 7 https://doi.org/10.1029/2020EA001098	journal	July 2020
Observed Relationships Between Cloud Droplet Effective Radius and Biogenic Gas Concentrations in Summertime Marine Stratocumulus Over the Eastern North Atlantic Miller, Mark A.; Mages, Zackary; Zheng, Qiuxuan Earth and Space Science, Vol. 9, Issue 2 https://doi.org/10.1029/2021EA001929	journal	February 2022
Phytoplankton Impact on Marine Cloud Microphysical Properties Over the Northeast Atlantic Ocean Mansour, Karam; Rinaldi, Matteo; Preißler, Jana Journal of Geophysical Research: Atmospheres, Vol. 127, Issue 10 https://doi.org/10.1029/2021JD036355	journal	May 2022
Maximum Supersaturation in the Marine Boundary Layer Clouds Over the North Atlantic Gong, Xianda; Wang, Yang; Xie, Hua AGU Advances, Vol. 4, Issue 6 https://doi.org/10.1029/2022AV000855	journal	November 2023
Aerosol‐Correlated Cloud Activation for Clean Conditions in the Tropical Atlantic Boundary Layer During LASIC Dedrick, Jeramy L.; Russell, Lynn M.; Sedlacek, Arthur J. Geophysical Research Letters, Vol. 51, Issue 3 https://doi.org/10.1029/2023GL105798	journal	February 2024
Supersaturation and Critical Size of Cloud Condensation Nuclei in Marine Stratus Clouds Svensmark, Henrik; Enghoff, Martin Bødker; Svensmark, Jacob Geophysical Research Letters, Vol. 51, Issue 9 https://doi.org/10.1029/2024GL108140	journal	April 2024
A parameterization of aerosol activation: 1. Single aerosol type Abdul-Razzak, Hayder; Ghan, Steven J.; Rivera-Carpio, Carlos Journal of Geophysical Research: Atmospheres, Vol. 103, Issue D6 https://doi.org/10.1029/97JD03735	journal	March 1998
Large contribution of natural aerosols to uncertainty in indirect forcing Carslaw, K. S.; Lee, L. A.; Reddington, C. L. Nature, Vol. 503, Issue 7474 https://doi.org/10.1038/nature12674	journal	November 2013
Observational constraint on cloud susceptibility weakened by aerosol retrieval limitations Ma, Po-Lun; Rasch, Philip J.; Chepfer, Hélène Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05028-4	journal	July 2018
Analysis of polarimetric satellite measurements suggests stronger cooling due to aerosol-cloud interactions Hasekamp, Otto P.; Gryspeerdt, Edward; Quaas, Johannes Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13372-2	journal	November 2019
Large uncertainty in future warming due to aerosol forcing Watson-Parris, Duncan; Smith, Christopher J. Nature Climate Change, Vol. 12, Issue 12 https://doi.org/10.1038/s41558-022-01516-0	journal	November 2022
Substantial cooling effect from aerosol-induced increase in tropical marine cloud cover Chen, Ying; Haywood, Jim; Wang, Yu Nature Geoscience, Vol. 17, Issue 5 https://doi.org/10.1038/s41561-024-01427-z	journal	April 2024
Weak average liquid-cloud-water response to anthropogenic aerosols Toll, Velle; Christensen, Matthew; Quaas, Johannes Nature, Vol. 572, Issue 7767 https://doi.org/10.1038/s41586-019-1423-9	journal	July 2019
Increased aerosols can reverse Twomey effect in water clouds through radiative pathway Khatri, Pradeep; Hayasaka, Tadahiro; Holben, Brent N. Scientific Reports, Vol. 12, Issue 1 https://doi.org/10.1038/s41598-022-25241-y	journal	November 2022
Occurrence of pristine aerosol environments on a polluted planet Hamilton, Douglas S.; Lee, Lindsay A.; Pringle, Kirsty J. Proceedings of the National Academy of Sciences, Vol. 111, Issue 52 https://doi.org/10.1073/pnas.1415440111	journal	December 2014
On the relationship between aerosol model uncertainty and radiative forcing uncertainty Lee, Lindsay A.; Reddington, Carly L.; Carslaw, Kenneth S. Proceedings of the National Academy of Sciences, Vol. 113, Issue 21 https://doi.org/10.1073/pnas.1507050113	journal	February 2016
Constraining the instantaneous aerosol influence on cloud albedo Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine Proceedings of the National Academy of Sciences, Vol. 114, Issue 19 https://doi.org/10.1073/pnas.1617765114	journal	April 2017
The hemispheric contrast in cloud microphysical properties constrains aerosol forcing McCoy, Isabel L.; McCoy, Daniel T.; Wood, Robert Proceedings of the National Academy of Sciences, Vol. 117, Issue 32 https://doi.org/10.1073/pnas.1922502117	journal	July 2020
A critical examination of the residual cloud contamination and diurnal sampling effects on MODIS estimates of aerosol over ocean Kaufman, Y. J.; Remer, L. A.; Tanre, D. IEEE Transactions on Geoscience and Remote Sensing, Vol. 43, Issue 12 https://doi.org/10.1109/TGRS.2005.858430	journal	December 2005
Cloud droplet nucleation and cloud scavenging of aerosol sulphate in polluted atmospheres Leaitch, W. R.; Strapp, J. W.; Isaac, G. A. Tellus B, Vol. 38B, Issue 5 https://doi.org/10.1111/j.1600-0889.1986.tb00258.x	journal	November 1986
From aerosol-limited to invigoration of warm convective clouds Koren, I.; Dagan, G.; Altaratz, O. Science, Vol. 344, Issue 6188 https://doi.org/10.1126/science.1252595	journal	June 2014
Aerosol-driven droplet concentrations dominate coverage and water of oceanic low-level clouds Rosenfeld, Daniel; Zhu, Yannian; Wang, Minghuai Science, Vol. 363, Issue 6427 https://doi.org/10.1126/science.aav0566	journal	January 2019
The Effect of Cloud Type on Earth's Energy Balance: Global Analysis Hartmann, Dennis L.; Ockert-Bell, Maureen E.; Michelsen, Marc L. Journal of Climate, Vol. 5, Issue 11 https://doi.org/10.1175/1520-0442(1992)005<1281:TEOCTO>2.0.CO;2	journal	November 1992
The Influence of Pollution on the Shortwave Albedo of Clouds Twomey, S. Journal of the Atmospheric Sciences, Vol. 34, Issue 7 https://doi.org/10.1175/1520-0469(1977)034<1149:TIOPOT>2.0.CO;2	journal	July 1977
Variability of the Supersaturation in Cumulus Clouds Politovich, Marcia K.; Cooper, William A. Journal of the Atmospheric Sciences, Vol. 45, Issue 11 https://doi.org/10.1175/1520-0469(1988)045<1651:VOTSIC>2.0.CO;2	journal	June 1988
The Measurement and Parameterization of Effective Radius of Droplets in Warm Stratocumulus Clouds Martin, G. M.; Johnson, D. W.; Spice, A. Journal of the Atmospheric Sciences, Vol. 51, Issue 13 https://doi.org/10.1175/1520-0469(1994)051<1823:TMAPOE>2.0.CO;2	journal	July 1994
A New Moist Turbulence Parameterization in the Community Atmosphere Model Bretherton, Christopher S.; Park, Sungsu Journal of Climate, Vol. 22, Issue 12 https://doi.org/10.1175/2008JCLI2556.1	journal	June 2009
CCN and Vertical Velocity Influences on Droplet Concentrations and Supersaturations in Clean and Polluted Stratus Clouds Hudson, James G.; Noble, Stephen Journal of the Atmospheric Sciences, Vol. 71, Issue 1 https://doi.org/10.1175/JAS-D-13-086.1	journal	January 2014
Impact of Cloud-Base Turbulence on CCN Activation: CCN Distribution Grabowski, Wojciech W.; Thomas, Lois; Kumar, Bipin Journal of the Atmospheric Sciences, Vol. 79, Issue 11 https://doi.org/10.1175/JAS-D-22-0075.1	journal	November 2022
The value of remote marine aerosol measurements for constraining radiative forcing uncertainty Regayre, Leighton A.; Schmale, Julia; Johnson, Jill S. Atmospheric Chemistry and Physics, Vol. 20, Issue 16 https://doi.org/10.5194/acp-20-10063-2020	journal	January 2020
Constraining the Twomey effect from satellite observations: issues and perspectives Quaas, Johannes; Arola, Antti; Cairns, Brian Atmospheric Chemistry and Physics, Vol. 20, Issue 23 https://doi.org/10.5194/acp-20-15079-2020	journal	January 2020
On the relationship between cloud water composition and cloud droplet number concentration MacDonald, Alexander B.; Hossein Mardi, Ali; Dadashazar, Hossein Atmospheric Chemistry and Physics, Vol. 20, Issue 13 https://doi.org/10.5194/acp-20-7645-2020	journal	January 2020
Environmental effects on aerosol–cloud interaction in non-precipitating marine boundary layer (MBL) clouds over the eastern North Atlantic Zheng, Xiaojian; Xi, Baike; Dong, Xiquan Atmospheric Chemistry and Physics, Vol. 22, Issue 1 https://doi.org/10.5194/acp-22-335-2022	journal	January 2022
Opportunistic experiments to constrain aerosol effective radiative forcing Christensen, Matthew W.; Gettelman, Andrew; Cermak, Jan Atmospheric Chemistry and Physics, Vol. 22, Issue 1 https://doi.org/10.5194/acp-22-641-2022	journal	January 2022
Seasonal updraft speeds change cloud droplet number concentrations in low-level clouds over the western North Atlantic Kirschler, Simon; Voigt, Christiane; Anderson, Bruce Atmospheric Chemistry and Physics, Vol. 22, Issue 12 https://doi.org/10.5194/acp-22-8299-2022	journal	June 2022
Evaluation of liquid cloud albedo susceptibility in E3SM using coupled eastern North Atlantic surface and satellite retrievals Varble, Adam C.; Ma, Po-Lun; Christensen, Matthew W. Atmospheric Chemistry and Physics, Vol. 23, Issue 20 https://doi.org/10.5194/acp-23-13523-2023	journal	October 2023
Uncertainty in aerosol–cloud radiative forcing is driven by clean conditions Gryspeerdt, Edward; Povey, Adam C.; Grainger, Roy G. Atmospheric Chemistry and Physics, Vol. 23, Issue 7 https://doi.org/10.5194/acp-23-4115-2023	journal	April 2023
Aerosol first indirect effect of African smoke at the cloud base of marine cumulus clouds over Ascension Island, southern Atlantic Ocean de Graaf, Martin; Sarna, Karolina; Brown, Jessica Atmospheric Chemistry and Physics, Vol. 23, Issue 9 https://doi.org/10.5194/acp-23-5373-2023	journal	May 2023
Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN) Reutter, P.; Su, H.; Trentmann, J. Atmospheric Chemistry and Physics, Vol. 9, Issue 18 https://doi.org/10.5194/acp-9-7067-2009	journal	January 2009
Better calibration of cloud parameterizations and subgrid effects increases the fidelity of the E3SM Atmosphere Model version 1 Ma, Po-Lun; Harrop, Bryce E.; Larson, Vincent E. Geoscientific Model Development, Vol. 15, Issue 7 https://doi.org/10.5194/gmd-15-2881-2022	journal	January 2022

Similar Records

Related Subjects

54 ENVIRONMENTAL SCIENCES
Aerosol
Climate
Clouds
Earth, Atmospheric, and Planetary Sciences
Physical Sciences
Supersaturation
Twomey

Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

Citation Formats

References (64)

Similar Records

Related Subjects