Abstract
Aerosol liquid water content (ALWC) plays an important role in climate and public health by influencing aerosol formation, chemical composition, and toxicity. However, ALWC remains sparsely measured and poorly constrained across space and time, despite its large variability. In this study, we derived a high-resolution (1 km × 1 km, daily) ALWC dataset for the contiguous US from 2000 to 2019. The dataset was generated by training machine learning (ML) models on outputs from a chemical transport model (GEOS-Chem) to capture the thermodynamic relationships between ALWC and relevant predictors, then applying these relationships to high-resolution, biased-corrected input datasets. Compared with GEOS-Chem simulations, the ML-based dataset better captures daily variations and spatial heterogeneity in ALWC. The predicted ALWC levels are highest in the Midwest US and lowest in the Western US, largely driven by regional differences in PM2.5 concentration, chemical composition, temperature, and relative humidity. Over the study period, ALWC declined significantly across most regions, driven primarily by the reduction in sulfate. We further demonstrate that ALWC provides a physically meaningful constraint for interpreting variability in water-soluble iron, a health-relevant fraction of aerosol metals, highlighting the potential value of this dataset for future studies of aerosol toxicity and epidemiological exposure.
Similar content being viewed by others
Data availability
Daily mean PM2.5, 8-h maximum ozone, and NO2 datasets at 1 km × 1 km resolution are publicly available from NASA Earthdata (PM2.5: https://doi.org/10.7927/g2n9-ca10; O3: https://doi.org/10.7927/5tht-jg22; NO2: https://doi.org/10.7927/rz28-p167). Annual mean aerosol composition data, including SO42−, NO3−, NH4+, and OC, are publicly available at https://doi.org/10.7927/7wj3-en73. Daily maximum and minimum temperatures are from Daymet (Daily Surface Weather Data on a 1-km Grid for North America, Version 4 R1): https://doi.org/10.3334/ORNLDAAC/2129. Daily mean RH on a 4 km × 4 km grid are from PRISM (the Parameter-elevation Relationships on Independent Slope Model, https://prism.oregonstate.edu). The 1 km daily ALWC data generated in this study for the years 2000, 2005, 2010, 2015, and 2019 are deposited in Harvard Dataverse at https://doi.org/10.7910/DVN/ADNPBD; Due to the large file size (~30GB per year), data for other years are available upon request from the corresponding author.
References
Bian, Y. X., Zhao, C. S., Ma, N., Chen, J. & Xu, W. Y. A study of aerosol liquid water content based on hygroscopicity measurements at high relative humidity in the North China Plain. Atmos. Chem. Phys. 14, 6417–6426 (2014).
Pye, H. O. T. et al. On the implications of aerosol liquid water and phase separation for organic aerosol mass. Atmos. Chem. Phys. 17, 343–369 (2017).
Faust, J. A., Wong, J. P. S., Lee, A. K. Y. & Abbatt, J. P. D. Role of aerosol liquid water in secondary organic aerosol formation from volatile organic compounds. Environ. Sci. Technol. 51, 1405–1413 (2017).
Wang, X. et al. The secondary formation of inorganic aerosols in the droplet mode through heterogeneous aqueous reactions under haze conditions. Atmos. Environ. 63, 68–76 (2012).
Ravishankara, A. R. Heterogeneous and multiphase chemistry in the troposphere. Science 276, 1058–1065 (1997).
Wong, J. P. S. et al. Fine particle iron in soils and road dust is modulated by coal-fired power plant sulfur. Environ. Sci. Technol. 54, 7088–7096 (2020).
Wang, Y. et al. Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility. Atmos. Chem. Phys. 20, 2161–2175 (2020).
Elias, T. et al. Enhanced extinction of visible radiation due to hydrated aerosols in mist and fog. Atmos. Chem. Phys. 15, 6605–6623 (2015).
Wu, Z. J. et al. Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime. Atmos. Chem. Phys. 16, 1123–1138 (2016).
Jin, X. et al. Significant contribution of organics to aerosol liquid water content in winter in Beijing, China. Atmos. Chem. Phys. 20, 901–914 (2020).
Kuang, Y. et al. A novel method for calculating ambient aerosol liquid water content based on measurements of a humidified nephelometer system. Atmos. Meas. Tech. 11, 2967–2982 (2018).
Guo, H. et al. Fine-particle water and pH in the southeastern United States. Atmos. Chem. Phys. 15, 5211–5228 (2015).
Tan, W. et al. Profiling aerosol liquid water content using a polarization lidar. Environ. Sci. Technol. 54, 3129–3137 (2020).
Fountoukis, C. & Nenes, A. ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+—Ca2+—Mg2+—NH4+—Na+—SO42-—NO3-—Cl-—H2O aerosols. Atmos. Chem. Phys. 7, 4639–4659 (2007).
Nguyen, T. K. V., Zhang, Q., Jimenez, J. L., Pike, M. & Carlton, A. G. Liquid water: ubiquitous contributor to aerosol mass. Environ. Sci. Technol. Lett. 3, 257–263 (2016).
Nenes, A. et al. Aerosol acidity and liquid water content regulate the dry deposition of inorganic reactive nitrogen. Atmos. Chem. Phys. 21, 6023–6033 (2021).
Carlton, A. G., Christiansen, A. E., Flesch, M. M., Hennigan, C. J. & Sareen, N. Multiphase atmospheric chemistry in liquid water: impacts and controllability of organic aerosol. Acc. Chem. Res. 53, 1715–1723 (2020).
Sareen, N., Waxman, E. M., Turpin, B. J., Volkamer, R. & Carlton, A. G. Potential of aerosol liquid water to facilitate organic aerosol formation: assessing knowledge gaps about precursors and partitioning. Environ. Sci. Technol. 51, 3327–3335 (2017).
Miao, R. et al. Model bias in simulating major chemical components of PM2.5 in China. Atmos. Chem. Phys. 20, 12265–12284 (2020).
Wyat Appel, K., Bhave, P. V., Gilliland, A. B., Sarwar, G. & Roselle, S. J. Evaluation of the community multiscale air quality (CMAQ) model version 4.5: sensitivities impacting model performance; Part II—particulate matter. Atmos. Environ. 42, 6057–6066 (2008).
Di, Q. et al. NASA Socioeconomic Data and Applications Center (SEDAC). (2021).
Wei, J. et al. Long-term mortality burden trends attributed to black carbon and PM2·5 from wildfire emissions across the continental USA from 2000 to 2020: a deep learning modelling study. Lancet Planet. Health 7, e963–e975 (2023).
Amini, H. et al. Hyperlocal super-learned PM2.5 components across the contiguous US. Preprint at Research Square https://doi.org/10.21203/rs.3.rs-1745433/v2 (2022).
Meng, X., Hand, J. L., Schichtel, B. A. & Liu, Y. Space-time trends of PM2.5 constituents in the conterminous United States estimated by a machine learning approach, 2005–2015. Environ. Int. 121, 1137–1147 (2018).
Thornton, M. M., Shrestha, R., Wei, Y., Thornton, P. E. & Kao, S. C. (ORNL Distributed Active Archive Center, 2020).
Thornton, P. E. et al. Gridded daily weather data for North America with comprehensive uncertainty quantification. Sci. Data 8, 190 (2021).
Pan, D. et al. Regime shift in secondary inorganic aerosol formation and nitrogen deposition in the rural United States. Nat. Geosci. 17, 617–623 (2024).
Pilinis, C., Seinfeld, J. H. & Grosjean, D. Water content of atmospheric aerosols. Atmos. Environ. 23, 1601–1606 (1989).
Edgerton, E. S. et al. The southeastern aerosol research and characterization study: part II. Filter-based measurements of fine and coarse particulate matter mass and composition. J. Air Waste Manag. Assoc. 55, 1527–1542 (2005).
Edgerton, E. S. et al. The southeastern aerosol research and characterization study, Part 3: continuous measurements of fine particulate matter mass and composition. J. Air Waste Manag. Assoc. 56, 1325–1341 (2006).
Hansen, D. A. et al. The southeastern aerosol research and characterization study: Part 1—overview. J. Air Waste Manag. Assoc. 53, 1460–1471 (2003).
Kim, P. S. et al. Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model. Atmos. Chem. Phys. 15, 10411–10433 (2015).
Battaglia, M. A. Jr., Douglas, S. & Hennigan, C. J. Effect of the urban heat island on aerosol pH. Environ. Sci. Technol. 51, 13095–13103 (2017).
Zhang, Q. et al. Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes. Geophys. Res. Lett. 34, L13801 (2007).
Hand, J. L., Schichtel, B. A., Malm, W. C. & Pitchford, M. L. Particulate sulfate ion concentration and SO2 emission trends in the United States from the early 1990s through 2010. Atmos. Chem. Phys. 12, 10353–10365 (2012).
Shah, V. et al. Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States. Proc. Natl. Acad. Sci. USA 115, 8110–8115 (2018).
Ridley, D. A., Heald, C. L., Ridley, K. J. & Kroll, J. H. Causes and consequences of decreasing atmospheric organic aerosol in the United States. Proc. Natl. Acad. Sci. USA 115, 290–295 (2018).
Guo, H. et al. Fine particle pH and gas–particle phase partitioning of inorganic species in Pasadena, California, during the 2010 CalNex campaign. Atmos. Chem. Phys. 17, 5703–5719 (2017).
Fang, T. et al. Highly acidic ambient particles, soluble metals, and oxidative potential: a link between sulfate and aerosol toxicity. Environ. Sci. Technol. 51, 2611–2620 (2017).
Chen, L. C. & Lippmann, M. Effects of metals within ambient air particulate matter (PM) on human health. Inhal. Toxicol. 21, 1–31 (2009).
Abbaspour, N., Hurrell, R. & Kelishadi, R. Review on iron and its importance for human health. J. Res. Med. Sci. 19, 164–174 (2014).
Wang, R. et al. Sources, transport and deposition of iron in the global atmosphere. Atmos. Chem. Phys. 15, 6247–6270 (2015).
Ito, A. Atmospheric processing of combustion aerosols as a source of bioavailable iron. Environ. Sci. Technol. Lett. 2, 70–75 (2015).
Amini, H. et al. Hyperlocal US PM2.5 Trace Elements Super-learned. Research Square PREPRINT (Version 1). https://doi.org/10.21203/rs.3.rs-2052258/v1 (2022).
Vu, B. N. et al. Association of annual exposure to air pollution mixture on asthma hospitalizations in the United States. Am. J. Respir. Crit. Care Med. 211, 1636–1643 (2025).
Danesh Yazdi, M. et al. Long-term exposure to PM2.5 components and cardiovascular admissions in medicare patients. Environ. Res. 286, 122779 (2025).
Oakes, M. et al. Iron solubility related to particle sulfur content in source emission and ambient fine particles. Environ. Sci. Technol. 46, 6637–6644 (2012).
Zhu, Y. et al. Iron solubility in fine particles associated with secondary acidic aerosols in East China. Environ. Pollut. 264, 114769 (2020).
Shi, Z. et al. Impacts on iron solubility in the mineral dust by processes in the source region and the atmosphere: a review. Aeolian Res. 5, 21–42 (2012).
Yang, Y. & Weber, R. J. Ultrafiltration to characterize PM2.5 water-soluble iron and its sources in an urban environment. Atmos. Environ. 286, 119246 (2022).
Myriokefalitakis, S. et al. Changes in dissolved iron deposition to the oceans driven by human activity: a 3-D global modelling study. Biogeosciences 12, 3973–3992 (2015).
Zhang, B. et al. Significant contrasts in aerosol acidity between China and the United States. Atmos. Chem. Phys. 21, 8341–8356 (2021).
Sakata, K. et al. Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: the role of organic complexation of Fe with humic-like substances in controlling Fe solubility. Atmos. Chem. Phys. 22, 9461–9482 (2022).
Paris, R. & Desboeufs, K. V. Effect of atmospheric organic complexation on iron-bearing dust solubility. Atmos. Chem. Phys. 13, 4895–4905 (2013).
Paris, R., Desboeufs, K. V. & Journet, E. Variability of dust iron solubility in atmospheric waters: investigation of the role of oxalate organic complexation. Atmos. Environ. 45, 6510–6517 (2011).
Tao, Y. & Murphy, J. G. The mechanisms responsible for the interactions among oxalate, pH, and Fe dissolution in PM2.5. ACS Earth Space Chem. 3, 2259–2265 (2019).
Weber, R. J., Guo, H., Russell, A. G. & Nenes, A. High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years. Nat. Geosci. 9, 282–285 (2016).
Petters, M. D. & Kreidenweis, S. M. A single parameter representation of hygroscopic growth and cloud condensation nucleus activity. Atmos. Chem. Phys. 7, 1961–1971 (2007).
Martin, R. V., Jacob, D. J., Yantosca, R. M., Chin, M. & Ginoux, P. Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols. J. Geophys. Res Atmos. https://doi.org/10.1029/2002JD002622 (2003).
King, S. M. et al. Cloud droplet activation of mixed organic-sulfate particles produced by the photooxidation of isoprene. Atmos. Chem. Phys. 10, 3953–3964 (2010).
Rickards, A. M. J., Miles, R. E. H., Davies, J. F., Marshall, F. H. & Reid, J. P. Measurements of the sensitivity of aerosol hygroscopicity and the κ parameter to the O/C ratio. J. Phys. Chem. A 117, 14120–14131 (2013).
Ervens, B. et al. CCN predictions using simplified assumptions of organic aerosol composition and mixing state: a synthesis from six different locations. Atmos. Chem. Phys. 10, 4795–4807 (2010).
Dusek, U. et al. Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events. Geophys. Res. Lett. https://doi.org/10.1029/2009GL040930 (2010).
Gunthe, S. S. et al. Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity. Atmos. Chem. Phys. 9, 7551–7575 (2009).
PRISM Group. Parameter-elevation Relationships on Independent Slope Model (PRISM) gridded data. Oregon State University, https://prism.oregonstate.edu, last accessed 07 March 2026.
Daly, C. et al. Physiographically sensitive mapping of climatological temperature and precipitation across the conterminous United States. Int. J. Climatol. 28, 2031–2064 (2008).
Spangler, K. R., Weinberger, K. R. & Wellenius, G. A. Suitability of gridded climate datasets for use in environmental epidemiology. J. Expos. Sci. Environ. Epidemiol. 29, 777–789 (2019).
Di, Q. et al. An ensemble-based model of PM2.5 concentration across the contiguous United States with high spatiotemporal resolution. Environ. Int. 130, 104909 (2019).
Di, Q. et al. NASA Socioeconomic Data and Applications Center (SEDAC). (2022).
Di, Q. et al. Assessing NO2 concentration and model uncertainty with high spatiotemporal resolution across the contiguous United States using ensemble model averaging. Environ. Sci. Technol. 54, 1372–1384 (2020).
Requia, W. J. et al. An Ensemble learning approach for estimating high spatiotemporal resolution of ground-level ozone in the contiguous United States. Environ. Sci. Technol. 54, 11037–11047 (2020).
Requia, W. J. et al. NASA Socioeconomic Data and Applications Center (SEDAC). (2021).
Amini, H. et al. NASA Socioeconomic Data and Applications Center (SEDAC). (2023).
Jimenez, J. L. & Zhang, Q. Aerosol Mass Spectrometry (AMS) Global Database. https://doi.org/10.6084/m9.figshare.3486719.v1 (2017).
Xu, L., Suresh, S., Guo, H., Weber, R. J. & Ng, N. L. Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates. Atmos. Chem. Phys. 15, 7307–7336 (2015).
Xu, L. et al. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States. Proc. Natl. Acad. Sci. USA 112, 37–42 (2015).
Acknowledgements
Research reported in this publication was supported by the National Institute on Aging of the National Institutes of Health under Award Number R01AG074357 and RF1 AG079487, and the National Science Foundation Division of Atmospheric and Geospace Sciences under AGS-2307151. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health.
Author information
Authors and Affiliations
Contributions
P.L. and B.Z. designed the study, B.Z. performed the ML model, generated the dataset, and wrote the initial manuscript. L.Y. performed the GEOS-Chem simulations. Y.Y., H.G., L.X., D.P., N.L.N., and R.J.W. provided observational data. Q.D., Y.W., J.W., and J.S. provide the high-resolution datasets of the ML model inputs. All the co-authors commented on data analysis and contributed to the writing of the manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Zhang, B., Yin, L., Yang, Y. et al. High-resolution aerosol liquid water content in the contiguous United States using machine learning. npj Clim Atmos Sci (2026). https://doi.org/10.1038/s41612-026-01371-2
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41612-026-01371-2


