Constraining the aerosol influence on cloud liquid water path

The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. In recent years, significant progress has been made in constraining this forcing using observations, but uncertainty still remains, particularly in the adjustments of cloud properties to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity) in the relationship. However, the Nd-LWP relationship is negative in the majority of regions, suggesting that aerosol induced LWP reductions could offset a significant fraction of the radiative forcing from aerosol-cloud interactions (RFaci). However, variations in the Nd-LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd-LWP relationship overestimates the Nd impact on LWP. As such, the estimate of LWP changes due to aerosol in this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP