Abstract. Single-particle mass spectrometry (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 < 0.2 µm for
accumulation-mode studies and D > 2 µm for coarse-mode
analysis. 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.