Abstract. Aerosol intercomparisons are inherently complex, as they convolve instrument-dependent detection efficiencies vs. size (which often change with pressure, temperature, or humidity) and variations on the sampled aerosol population, in addition to differences in chemical detection principles (e.g., including inorganic-only nitrate vs. inorganic plus organic nitrate for two instruments). The NASA Atmospheric Tomography Mission (ATom) spanned four separate aircraft deployments, which sampled the remote marine troposphere from 86° S to 82° N over different seasons with a wide range of aerosol concentrations and compositions. Aerosols were quantified with a set of carefully characterized and calibrated instruments, some based on particle sizing and some on composition measurements. This study aims to provide a critical evaluation of the size-related factors impacting aerosol intercomparisons, and of aerosol quantification during ATom, with a focus on the Aerosol Mass Spectrometer (AMS). The volume determined from physical sizing instruments is compared in detail with that derived from the chemical measurements of the AMS and the Single Particle Soot Photometer (SP2). Special attention was paid to characterize the upper end of the AMS size-dependent transmission with in-field calibrations, which we show to be critical for accurate comparisons across instruments with inevitably different size cuts. Observed differences between campaigns emphasize the importance of characterizing AMS transmission for each instrument and field study for meaningful interpretation of instrument comparisons. Good agreement was found between the composition-based volume (including AMS-quantified sea salt) and that derived from the size spectrometers. The very clean conditions during most of ATom resulted in substantial statistical noise (i.e., precision error), which we show to be substantially reduced by averaging at several-minute time intervals. The AMS captured, on average, 95 ± 15 % of the standard PM1 volume. These results support the absence of significant unknown biases and the appropriateness of the accuracy estimates for AMS total mass/volume for the mostly aged air masses encountered in ATom. The particle size ranges that contribute chemical composition information to the AMS and complementary composition instruments are investigated, to inform their use in future studies.;
