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Abstract Aerosol‐cloud interactions (ACI) pose the largest uncertainty for climate projection. Among many challenges of understanding ACI, the question of whether ACI can be deterministically predicted has not been explicitly answered. Here we attempt to answer this question by predicting cloud droplet number concentration Nc from aerosol number concentration Na and ambient conditions using a data‐driven framework. We use aerosol properties, vertical velocity fluctuations, and meteorological states from the ACTIVATE field observations (2020–2022) as predictors to estimate Nc. We show that the campaign‐wide Nc can be successfully predicted using machine learning models despite the strongly nonlinear and multi‐scale nature of ACI. However, the observation‐trained machine learning model fails to predict Nc in individual cases while it successfully predicts Nc of randomly selected data points that cover a broad spatiotemporal scale. This suggests that, within a data‐driven framework, the Nc prediction is uncertain at fine spatiotemporal scales.

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved Na product to in situNa data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11 separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter Na agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged Na. We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged Na and the lidar + polarimeter vertically resolved Na are of similar magnitude and represent a significant improvement upon current remote sensing estimates of Na.