Abstract. Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. Their fundamental ability to differentiate the externally mixed particle types that constitute the atmospheric aerosol population enables a unique perspective into sources and transformation. However, quantitative measurements by SPMS systems are inherently problematic. We introduce a new technique that combines collocated measurements of aerosol composition by SPMS and size-resolved absolute particle concentrations on aircraft platforms. Quantitative number, surface area, volume, and mass concentrations are derived for climate-relevant particle types such as mineral dust, sea salt, and biomass burning smoke. Additionally, relative ion signals are calibrated to derive mass concentrations of internally mixed sulfate and organic material that are distributed across multiple particle types. The NOAA Particle Analysis by Laser Mass Spectrometry (PALMS) instrument measures size-resolved aerosol chemical composition from aircraft. We describe the identification and quantification of nine major atmospheric particle classes, including sulfate/organic/nitrate mixtures, biomass burning, elemental carbon, sea salt, mineral dust, meteoric material, alkali salts, heavy fuel oil combustion, and a remainder class. Classes can be sub-divided as necessary based on chemical heterogeneity, accumulated secondary material during aging, or other atmospheric processing. Concentrations are derived for sizes that encompass the accumulation and coarse size modes. A statistical error analysis indicates that particle class concentrations can be determined within a few minutes for abundances above ~ 10 ng m−3. Rare particle types require longer sampling times. We explore the instrumentation requirements and the limitations of the method for airborne measurements. Reducing the size resolution of the particle data increases time resolution with only a modest increase in uncertainty. The principal limiting factor to fast time response concentration measurements is statistically relevant sampling across the size range of interest, in particular, sizes D 2 μm for coarse mode analysis. We demonstrate the use of a virtual impactor to enhance sampling statistics for the inherently sparse coarse mode. Performance is compared to other airborne and ground-based composition measurements, and examples of atmospheric mineral dust concentrations are given. The wealth of information afforded by composition-resolved size distributions for all major aerosol types represents a new and powerful tool to characterize atmospheric aerosol properties in a quantitative fashion.;
