The aerosol impact on liquid water path (LWP) is a key uncertainty in the overall climate impact of aerosol. However, despite a significant effort in this area, the size of the effect remains poorly constrained, and even the sign is unclear. Recent studies have shown that the relationship between droplet number concentration (Nd) and LWP is an unreliable measure of the impact of Nd variations on LWP due to the difficulty in establishing causality. In this work, we use satellite observations of the short-term development of clouds to examine the role of Nd perturbations in LWP variations. Similar to previous studies, an increase followed by a general decrease in LWP with increasing Nd is observed, suggesting an overall negative LWP response to Nd and a warming LWP adjustment to aerosol. However, the Nd also responds to the local environment, with aerosol production, entrainment from the free troposphere and wet scavenging all acting to modify the Nd. Many of these effects act to further steepen the Nd-LWP relationship and obscure the causal Nd impact on LWP. Using the temporal development of clouds to account for these feedbacks in the Nd-LWP system, a weaker negative Nd-LWP relationship is observed over most of the globe. This relationship is highly sensitive to the initial cloud state, illuminating the roles of different processes in shaping the Nd-LWP relationship. The nature of the current observing system limits this work to a single time period for observations, highlighting the need for more frequent observations of key cloud properties to constrain cloud behaviour at process timescales.

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Data-driven quantification and parameterization of cloud physics in general, and of aerosol-cloud interactions in particular, rely on input data from observations or detailed simulations. These data sources have complementary limitations in terms of their spatial and temporal coverage and resolution; simulation data has the advantage of readily providing causality but cannot represent the full process complexity. In order to base data-driven approaches on comprehensive information, we therefore need ways to integrate different data sources.  We discuss how the classical statistical technique of Gaussian-process emulation can be combined with specifically initialized ensembles of detailed cloud simulations (large-eddy simulations, LES) to provide a framework for evaluating data-driven descriptions of cloud characteristics and processes across different data sources. We specifically illustrate this approach for integrating LES and satellite data of aerosol-cloud interactions in subtropical stratocumulus cloud decks. We furthermore explore the extension of our framework to ground-based observations of Arctic mixed-phase clouds.@en