Supplementary material to "Retrieval of the Sea Spray Aerosol Mode from Submicron Particle Size Distributions and Supermicron Scattering during LASIC"

Improved quantification of sea spray aerosol concentration and size is important for determining aerosol effects on clouds and the climate, though attempts to accurately capture the size distribution of the sea spray mode remain limited by the availability of supermicron size distributions. In this work, we introduce a new approach to retrieving lognormal mode fit parameters for a sea spray aerosol mode by combining submicron size distributions with supermicron scattering measurements using a Mie inversion. Submicron size distributions were measured by an ultra-highsensitivity aerosol spectrometer (UHSAS), and supermicron scattering was taken as the difference between < 10 mu m and < 1 mu m three-wavelength integrating nephelometer measurements (NEPH). This UHSAS-NEPH method was applied during background marine periods of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign on Ascension Island (November 2016-May 2017), when the contribution of sea spray aerosol was expected to represent a large fraction of the aerosol mass and total scattering. Lognormal sea spray modal parameters were retrieved from comparisons between nephelometer measurements and a lookup table of Mie theory-simulated scattering coefficients for lowerror solutions that minimized the 0.4-1 mu m residual in the UHSAS size distribution. We evaluated the UHSAS-NEPH method with a set of clean marine measurements in the North Atlantic that included supermicron size and chemical measurements, showing that measured supermicron size distributions are needed to constrain the sea spray number concentration but that mass concentration was reasonably characterized using supermicron scattering. For LA-SIC, the UHSAS-NEPH method retrieved sea spray mode properties for approximately 88% of the background marine times when the scattering variability and total particle concentration were low ( < +/- 5Mm(-1) and < 400 cm(-3), respectively), with mass mean diameter ranging from 0.6 to 1.9 mu m (1.47 +/- 0.17 mu m), modal width ranging from 1.1 to 3.97 (2 :4 +/- 0 :3), and mass concentration ranging from 0.18 to 23.0 mu gm(-3) (8.37. +/- 4.1 mu gm(-3)). The measured nephelometer scattering at three wavelengths was found to constrain the mode width marginally at the largest particle sizes in the absence of additional size and chemical measurements for defining parameters for the Mie solutions. Comparing UHSAS-NEPH retrievals to those of a fitting algorithm applied only to the submicron UHSAS number size distribution showed that correlations between retrieved mass concentration and the available mass-based sea spray tracers (coarse scattering, wind speed, and chloride) are low when supermicron measurements are not considered. This work demonstrates the added value of supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available observationally constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available.