Keith Bower

Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon‐like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.

The aerosol mass spectrometer (AMS), manufactured by Aerodyne Research, Inc., has been shown to be capable of delivering quantitative information on the chemical composition and size of volatile and semivolatile fine airborne particulate matter with high time resolution. Analytical and software tools for interpreting the data from this instrument and generating meaningful, quantitative results have been developed and are presented here with a brief description of the instrument. These include the conversion of detected ion rates from the quadrupole mass spectrometer during the mass spectrum (MS) mode of operation to atmospheric mass concentrations of chemical species (in μg m −3 ) by applying calibration data. It is also necessary to correct for variations in the electron multiplier performance, and a method involving the measurement of the instrument's response to gas phase signals is also presented. The techniques for applying particle velocity calibration data and transforming signals from time of flight (TOF) mode to chemical mass distributions in terms of aerodynamic diameter (d M /dlog( D a ) distributions) are also presented. It is also possible to quantify the uncertainties in both MS and TOF data by evaluating the ion counting statistics and variability of the background signal, respectively. This paper is accompanied by part 2 of this series, in which these methods are used to process and analyze AMS results on ambient aerosol from two U.K. cities at different times of the year.