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Weak average liquid-cloud-water response to anthropogenic aerosols
Open accessAbstract
The cooling of the Earth's climate through the effects of anthropogenic aerosols on clouds offsets an unknown fraction of greenhouse gas warming. An increase in the amount of water inside liquid-phase clouds induced by aerosols, through the suppression of rain formation, has been postulated to lead to substantial cooling, which would imply that the Earth's surface temperature is highly sensitive to anthropogenic forcing. Here we provide direct observational evidence that, instead of a strong increase, aerosols cause a relatively weak average decrease in the amount of water in liquid-phase clouds compared with unpolluted clouds. Measurements of polluted clouds downwind of various anthropogenic sources-such as oil refineries, smelters, coal-fired power plants, cities, wildfires and ships-reveal that aerosol-induced cloud-water increases, caused by suppressed rain formation, and decreases, caused by enhanced evaporation of cloud water, partially cancel each other out. We estimate that the observed decrease in cloud water offsets 23% of the global climate-cooling effect caused by aerosol-induced increases in the concentration of cloud droplets. These findings invalidate the hypothesis that increases in cloud water cause a substantial climate cooling effect and translate into reduced uncertainty in projections of future climate.
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“More recent studies show that aerosols can also change LWP and total cloud fraction (CF), which also greatly affect the amount of solar radiation reflected by clouds2,13–16.”
From Abrupt reduction in shipping emission as an inadvertent geoengineering termination shock produces substantial radiative warming (2024) · cites this paper as [16]
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BackgroundMethodResultInfluentialSurprising similarities in model and observational aerosol radiative forcing estimates
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BackgroundSelf-citationZhang, J., Zhou, X., Goren, T., & Feingold, G. (2022) · Atmospheric chemistry and physics · doi:10.5194/acp-22-861-2022 · Cited by 80
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“We refer to these clouds as “overcast clouds”.”
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“This is not surprising, as AOD and AI are directly related. sensitivity estimates that use log s as an aerosol proxy correlations amongst the other CCF sensitivity patterns are lower (on average 0.92– sensitivities are not strongly correlated 10 SW 10 − − 2 − 1 ) 10 − − 2 − 1 − − 2 − 1 Similar to the recent study by W…”
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“…used using more conventional measurements ( 17 , 27 – 29 ), including surface sulfate aerosols ( 18 ), aerosol optical depth (AOD) ( 16 , 17 , 30 , 31 ), and aerosol extinction ( 32 , 33 ) from which attempts were made to retrieve the CCN ( 34 , 35 ), but their effectiveness in a wide range of…”
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“This large uncertainty is often dominated by uncertainty in changes in cloud water amount or liquid water path (LWP) caused by anthropogenic aerosol perturbation (Ackerman et al., 2004; Malavelle et al., 2017; Rosenfeld et al., 2019; Toll et al., 2019; Wang et al., 2012).”
BackgroundXiao, D., Wang, N., Chen, S., Wu, L., Müller, D., Veselovskii, I. A., Li, C., Landulfo, E., Sivakumar, V., Li, J., et al. (2023) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2023.162091 · Cited by 27
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“These observations sample a wider geographical area compared to large‐scale cloud perturbations in Moscow area, Russia, and Kazakhstan studied by Toll et al. (2019).”
BackgroundMethodResultInfluentialSelf-citationThe Evolving Role of External Forcing in North Atlantic SST Variability over the Last Millennium
Klavans, J. M., Clement, A., Cane, M. A., & Murphy, L. N. (2022) · Journal of Climate · doi:10.1175/jcli-d-21-0338.1 · Cited by 25
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Exploring Impacts of Size‐Dependent Evaporation and Entrainment in a Global Model
Karset, I. H. H., Gettelman, A., Storelvmo, T., Alterskjær, K., & Berntsen, T. K. (2020) · Journal of Geophysical Research Atmospheres · doi:10.1029/2019jd031817 · Cited by 24
Veals, P. G., Varble, A. C., Russell, J. O. H., Hardin, J. C., & Zipser, E. J. (2021) · Journal of the Atmospheric Sciences · doi:10.1175/jas-d-21-0119.1 · Cited by 24
“This has been shown to decrease the efficiency of collision–coalescence in warm clouds, suppressing rainfall (e.g., Rosenfeld 1999; Braga et al. 2017; Toll et al. 2019).”
BackgroundGupta, S., McFarquhar, G. M., O'Brien, J. R., Poellot, M. R., Delene, D. J., Miller, R. M., & Griswold, J. D. S. (2022) · Atmospheric chemistry and physics · doi:10.5194/acp-22-2769-2022 · Cited by 24
“Due to aerosol-induced changes in entrainment and boundary layer stability, the aerosol impact on H and ZT can have the strongest influence on LWP adjustments associated with ACIs (Toll et al., 2019).”
InfluentialStability-dependent increases in liquid water with droplet number in the Arctic
Murray-Watson, R. J., & Gryspeerdt, E. (2022) · Atmospheric chemistry and physics · doi:10.5194/acp-22-5743-2022 · Cited by 24
Meyer, K., Platnick, S. E., Holz, R. E., Dutcher, S., Quinn, G., & Nagle, F. (2020) · Remote Sensing · doi:10.3390/rs12244096 · Cited by 24
Hu, X., Ge, J., Du, J., Li, Q., Huang, J., & Fu, Q. (2021) · Atmospheric measurement techniques · doi:10.5194/amt-14-1743-2021 · Cited by 23
“To reduce this uncertainty, accurate long-term observations are important to characterize low-level clouds and understand their climate feedbacks (Garrett and Zhao, 2013; Toll et al., 2019; Turner et al., 2007).”
BackgroundAtmospheric aerosols and their role in climate change
Haywood, J. (2021) · Elsevier eBooks · doi:10.1016/b978-0-12-821575-3.00030-x · Cited by 23
Hu, S., Zhu, Y., Rosenfeld, D., Mao, F., Lü, X., Pan, Z., Zang, L., & Gong, W. Y. (2021) · Journal of Geophysical Research Atmospheres · doi:10.1029/2020jd033852 · Cited by 23
“, enhancing the clouds albedo) in the background of pristine marine clouds but negative in relatively polluted marine and continental backgrounds (Toll et al., 2019).”
BackgroundMiller, R. M., Rauber, R. M., Girolamo, L. D., Rilloraza, M., Fu, D., McFarquhar, G. M., Nesbitt, S. W., Ziemba, L. D., Woods, S., & Thornhill, K. L. (2023) · Atmospheric chemistry and physics · doi:10.5194/acp-23-8959-2023 · Cited by 22
“…shipping pollution on marine clouds and precipitation has been explored in recent decades (Petzold et al., 2008; Rosenfeld et al., 2008; Stevens and Feingold, 2009; Coggon et al., 2012; Juwono et al., 2013; Russell et al., 2013; Gryspeerdt et al., 2019; Toll et al., 2019; Manshausen et al., 2022).”
BackgroundSnow-induced buffering in aerosol–cloud interactions
Michibata, T., Suzuki, K., & Takemura, T. (2020) · Atmospheric chemistry and physics · doi:10.5194/acp-20-13771-2020 · Cited by 22
Diurnal Patterns in the Observed Cloud Liquid Water Path Response to Droplet Number Perturbations
Smalley, K. M., Lebsock, M., & Eastman, R. M. (2024) · Geophysical Research Letters · doi:10.1029/2023gl107323 · Cited by 21
Pandey, S. K., Vinoj, V., & Panwar, A. (2019) · Atmospheric Pollution Research · doi:10.1016/j.apr.2019.12.017 · Cited by 21
“Cooling credits” are not a viable climate solution
Diamond, M., Wanser, K., & Boucher, O. (2023) · Climatic Change · doi:10.1007/s10584-023-03561-w · Cited by 20
“2013) and large industrial centers (Hobbs et al. 1980; Toll et al. 2019; Trofimov et al. 2020).”
The Fall and Rise of the Global Climate Model
Mülmenstädt, J., & Wilcox, L. J. (2021) · Journal of Advances in Modeling Earth Systems · doi:10.1029/2021ms002781 · Cited by 19
“In the observed atmosphere, the liquid water path responds weakly to aerosols (Malavelle et al., 2017; Toll et al., 2019) or perhaps slightly decreases (Gryspeerdt et al.”
BackgroundThe Radiative and Cloud Responses to Sea Salt Aerosol Engineering in GFDL Models
Mahfouz, N., Hill, S. A., Guo, H., & Ming, Y. (2023) · Geophysical Research Letters · doi:10.1029/2022gl102340 · Cited by 19
“to aerosol perturbation could be either positive, negative, or neutral, depending upon the competing effects of microphysics involved (e.g., Christensen et al., 2022; Hoffmann & Feingold, 2021; Manshausen et al., 2022; Mülmenstädt et al., 2020; Sato et al., 2018; Toll et al., 2019).”
BackgroundHirasawa, H., Kushner, P. J., Sigmond, M., Fyfe, J. C., & Deser, C. (2022) · Journal of Climate · doi:10.1175/jcli-d-21-0795.1 · Cited by 24
“CAM5 overestimates the enhancement of cloud liquid water path in response to aerosol perturbations from tropospheric volcanic aerosols, which may result in an overestimation of the aerosol – cloud lifetime effect (Malavelle et al. 2017; Toll et al. 2019).”
BackgroundSong, C., McCoy, D. T., Eidhammer, T., Gettelman, A., McCoy, I. L., Watson‐Parris, D., Wall, C. J., Elsaesser, G. S., & Wood, R. (2024) · Geophysical Research Letters · doi:10.1029/2024gl108663 · Cited by 18
“Process understanding and observations suggest that cloud adjustments could lead to increased or decreased cloud amount and optical thickness (Ackerman et al., 2004; Glassmeier et al., 2021; Toll et al., 2019; Wood, 2007).”
BackgroundAn Overview of Aerosol‐Cloud Interactions
Gordon, H., Glassmeier, F., & McCoy, D. T. (2023) · Geophysical monograph · doi:10.1002/9781119700357.ch2 · Cited by 18
Zhang, J., Chen, Y., Yamaguchi, T., & Feingold, G. (2024) · Atmospheric chemistry and physics · doi:10.5194/acp-24-10425-2024 · Cited by 17
“…2023; Smalley et al., 2024) and polar-orbiting satellites (e.g., Di-amond et al., 2020; Zhang and Feingold, 2023) have indicated diurnal variation in cloud adjustments to aerosol perturbations, such that LWP adjustments become more negative in the afternoon Through extrapolating the Terra (late d”
Ge, W., Prime, N., Smith, S. J., Liu, J., Ren, Y., Zhou, Y., Wu, H., Wang, X., & Chen, G. (2025) · Environmental Pollution · doi:10.1016/j.envpol.2025.125669 · Cited by 16
Qiu, S., Zheng, X., Painemal, D., Terai, C. R., & Zhou, X. (2024) · Atmospheric chemistry and physics · doi:10.5194/acp-24-2913-2024 · Cited by 16
“Previous studies have utilized various methods based on the effective radius threshold (e.g., Gryspeerdt et al., 2019; Toll et al., 2019; Zhang et al., 2022) and the rain rate threshold (e.g., Duong et al., 2011; Terai et al., 2015) from satellite retrievals. our study, we validate these two…”
MethodAdjustments to Climate Perturbations—Mechanisms, Implications, Observational Constraints
Quaas, J., Andrews, T., Bellouin, N., Block, K., Boucher, O., Ceppi, P., Dagan, G., Doktorowski, S., Eichholz, H. M., Forster, P. M. D. F., et al. (2024) · AGU Advances · doi:10.1029/2023av001144 · Cited by 23
Self-citationGoren, T., Choudhury, G. G., Kretzschmar, J. G., & McCoy, I. L. (2025) · Atmospheric chemistry and physics · doi:10.5194/acp-25-3413-2025 · Cited by 16
“N d joint histograms in an inverted-V-shaped pattern (Arola et al., 2022; Dipu et al., 2022; Glassmeier et al., 2021; Gryspeerdt et al., 2019; Mül-menstädt et al., 2024; Possner et al., 2020)”
Simulation of Aerosol Indirect Effects on Cloud Streets Over the Northwestern Pacific Ocean
Wu, C., & Chen, J. (2021) · Journal of Geophysical Research Atmospheres · doi:10.1029/2020jd034325 · Cited by 15
“Many studies applied different definitions for the cloudy area, such as using a minimum LWP (e.g., Jiang et al., 2006; Jiang et al., 2009; Koren et al., 2009; Seigel, 2014) or optical depth (Jiang et al., 2009).”
BackgroundInfluentialZhang, K., Zuo, Z., Suarez‐Gutierrez, L., & Bu, L. (2024) · npj Climate and Atmospheric Science · doi:10.1038/s41612-024-00567-8 · Cited by 14
Jia, Y., Andersen, H., & Čermák, J. (2024) · Atmospheric chemistry and physics · doi:10.5194/acp-24-13025-2024 · Cited by 18
Global evidence of aerosol-induced invigoration in marine cumulus clouds
Douglas, A., & L’Ecuyer, T. (2021) · Atmospheric chemistry and physics · doi:10.5194/acp-21-15103-2021 · Cited by 14
Shen, Z., Ming, Y., & Held, I. M. (2020) · Science Advances · doi:10.1126/sciadv.abb5297 · Cited by 14
Dipu, S., Schwarz, M., Ekman, A. M. L., Gryspeerdt, E., Goren, T., Sourdeval, O., Mülmenstädt, J., & Quaas, J. (2022) · Tellus B · doi:10.16993/tellusb.27 · Cited by 13
Self-citationRapid saturation of cloud water adjustments to shipping emissions
Manshausen, P., Watson‐Parris, D., Christensen, M. W., Jalkanen, J.-P., & Stier, P. (2023) · Atmospheric chemistry and physics · doi:10.5194/acp-23-12545-2023 · Cited by 13
Self-citationCalderón, S. M., Tonttila, J., Buchholz, A., Joutsensaari, J., Komppula, M., Leskinen, A., Hao, L., Moisseev, D. N., Pullinen, I., Tiitta, P., et al. (2022) · Atmospheric chemistry and physics · doi:10.5194/acp-22-12417-2022 · Cited by 12
Hidden Large Aerosol‐Driven Cloud Cover Effect Over High‐Latitude Ocean
Wang, X., Mao, F., Zhu, Y., Rosenfeld, D., Pan, Z., Zang, L., Lü, X., Liu, F., & Gong, W. Y. (2024) · Journal of Geophysical Research Atmospheres · doi:10.1029/2023jd039312 · Cited by 12
“…resulting in the accumulation of cloud water, thereby prolonging cloud coverage and lifetime (Albrecht, 1989); on the other hand, the reduced r e results in enhanced evaporation and diminished sedimentation, leading to a reduction in cloud water (Ackerman et al., 2004; Toll et al., 2019).”
Haywood, J., Boucher, O., Lennard, C., Storelvmo, T., Tilmes, S., & Visioni, D. (2025) · Frontiers in Climate · doi:10.3389/fclim.2025.1507479 · Cited by 12
Sensitivity of Radiative Fluxes to Aerosols in the ALADIN-HIRLAM Numerical Weather Prediction System
Rontu, L., Gleeson, E., Pérez, D. M., Nielsen, K. P., & Toll, V. (2020) · Atmosphere · doi:10.3390/atmos11020205 · Cited by 12
“The direct radiative effect of aerosols on weather and climate is much better quantified than indirect effects [19,20] because of the greater physical understanding of the aerosol radiative effects compared to the impact of aerosols on clouds and precipitation.”
BackgroundSelf-citationGlaciation of liquid clouds, snowfall, and reduced cloud cover at industrial aerosol hot spots
Toll, V., Rahu, J., Keernik, H., Trofimov, H., Voormansik, T., Manshausen, P., Hung, E., Michelson, D. B., Christensen, M. W., Post, P., et al. (2024) · Science · doi:10.1126/science.adl0303 · Cited by 11
Self-citationAerosol-cloud interactions in liquid clouds
Quaas, J., & Gryspeerdt, E. (2022) · Elsevier eBooks · doi:10.1016/b978-0-12-819766-0.00019-5 · Cited by 11
Self-citationAndersen, H., Čermák, J., Stirnberg, R., Fuchs, J., Kim, M., & Pauli, E. (2021) · Tellus B · doi:10.1080/16000889.2021.1971925 · Cited by 11
“Also, climate-system effects of aerosols are particularly pronounced in China and over adjacent seas (Andersen et al. 2017; Hasekamp et al. 2019; Toll et al. 2019).”
BackgroundHassan, T., Allen, R. J., Liu, W., Shim, S., van Noije, T., Sager, P. L., Oshima, N., Deushi, M., Randles, C. A., & O’Connor, F. M. (2022) · Communications Earth & Environment · doi:10.1038/s43247-022-00476-9 · Cited by 11
Zhao, J., Ma, X., Quaas, J., & Jia, H. (2024) · Atmospheric chemistry and physics · doi:10.5194/acp-24-9101-2024 · Cited by 10
“4”
Self-citation
Metadata
- Authors
- Toll, V., Christensen, M., Quaas, J., & Bellouin, N.
- Affiliations
- University of Tartu (EE)
- University of Oxford (GB)
- Leipzig University (DE)
- University of Reading (GB)
- Corresponding author
- Toll, Velle
- Venue
- Nature
- Published
- 2019-07-31
- Volume
- 572
- Issue
- 7767
- Pages
- 51-55
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- OpenAlex
- W2965102826
- Cited by
- 254
- References
- 66
- Citations by year
- 2026: 17 · 2025: 32 · 2024: 40 · 2023: 45 · 2022: 42 · 2021: 41 · 2020: 31 · 2019: 6
- FWCI
- 15.44
- Type
- journal article
- Language
- en
- Update notices
- correction (2020-01-03)
- Open access
- Licence
- Locations
- Nature (publishedVersion)
- PubMed (publishedVersion)
- CentAUR (University of Reading) (acceptedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Funders
- University of Reading
- Eesti Teadusagentuur (PSG202)
- Natural Environment Research Council (NE/L013746/1, NE/L013479/1)
- Topics
- Physical Sciences › Environmental Science › Global and Planetary Change › Atmospheric aerosols and clouds
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
- Physical Sciences › Environmental Science › Global and Planetary Change › Climate Change and Geoengineering
- Keywords
- anthropogenic aerosols, cloud water content, aerosol-cloud interactions, cloud droplet number concentration, cloud evaporation, climate cooling effect, global warming, climate sensitivity
- MeSH terms
- Aerosols, Air Pollution, Human Activities, Models, Theoretical, Rain, Temperature, Water, Greenhouse Effect, Uncertainty, Climate Change
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