Abstract. Factor analysis of aerosol mass spectrometer measurements (organic aerosol mass spectra) is often used to determine the sources of organic aerosol (OA). In this study we aim to gain insights regarding the ability of positive matrix factorization (PMF) to identify and quantify the OA sources accurately. We performed PMF and multilinear engine (ME-2) analysis on the predictions of a state-of-the-art chemical transport model (PMCAMx-SR, Particulate Matter Comprehensive Air Quality Model with extensions – source resolved) during a photochemically active period for specific sites in Europe in an effort to interpret the diverse factors usually identified by PMF analysis of field measurements. Our analysis used the predicted concentrations of 27 OA components, assuming that each of them is “chemically different” from the others. The PMF results based on the chemical transport model predictions are quite consistent (same number of factors and source types) with those of the analysis of AMS measurements. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources less than 40 %, when these sources contribute more than 20 % to the total OA. The PMF uncertainty increases for smaller source contributions, reaching a factor of 2 or even 3 for sources which contribute less than 10 % to the OA. One of the major questions in PMF analysis of AMS measurements concerns the sources of the two or more oxygenated OA (OOA) factors often reported in field studies. Our analysis suggests that these factors include secondary OA compounds from a variety of anthropogenic and biogenic sources and do not correspond to specific sources. Their characterization in the literature as low- and high-volatility factors is probably misleading, because they have overlapping volatility distributions. However, the average volatility of the one often characterized as a low-volatility factor is indeed lower than that of the other (high-volatility factor). Based on the analysis of the PMCAMx-SR predictions, the first oxygenated OA factor includes mainly highly aged OA transported from outside Europe, but also highly aged secondary OA from precursors emitted in Europe. The second oxygenated OA factor contains fresher secondary organic aerosol from volatile, semivolatile, and intermediate volatility anthropogenic and biogenic organic compounds. The exact contribution of these OA components to each OA factor depends on the site and the prevailing meteorology during the analysis period.
<p><strong>Abstract.</strong> Factor analysis of Aerosol Mass Spectrometer measurements (organic aerosol mass spectra) is often used to determine the sources of organic aerosol (OA). In this study we aim to gain insights regarding the ability of positive matrix factorization (PMF) to identify and quantify the OA sources accurately. We performed PMF and multilinear engine (ME-2) analysis on the predictions of a state-of-the-art chemical transport model (PMCAMx-SR) during a photochemically active period for specific sites in Europe in an effort to interpret the diverse factors usually identified by PMF analysis of field measurements. Our analysis used the predicted concentrations of 27 OA components, assuming that each of them is <q>chemically different</q> from the others.</p> <p> The PMF results based on the chemical transport model predictions are quite consistent (same number of factors and source types) with those of the analysis of AMS measurements. The estimated uncertainty of the contribution of fresh biomass burning is less than 30&#8201;% and of the other primary sources less than 40&#8201;%, when these sources contribute more than 20&#8201;% to the total OA. For contributions between 10 and 20&#8201;% the corresponding uncertainties increase to 50&#8201;%. Finally, when these sources are small (less than 10&#8201;% of the OA) the corresponding error is a factor of two or even three.</p> <p> One of the major questions in PMF analysis of AMS measurements concerns the sources of the two or more oxygenated OA (OOA) factors often reported in field studies. Our analysis suggests that these factors include secondary OA compounds from a variety of anthropogenic and biogenic sources and do not correspond to specific sources. Their characterization in the literature as low and high volatility factors is probably misleading, because they have overlapping volatility distributions. However, the average volatility of the one often characterized as low-volatility factor is indeed lower than that of the other (high volatility factor). Based on the analysis of the PMCAMx-SR predictions, the first oxygenated OA factor includes mainly highly-aged OA transported from outside Europe, but also highly aged secondary OA from precursors emitted in Europe. The second oxygenated OA factor contains fresher SOA from volatile, semi-volatile, and intermediate volatility anthropogenic and biogenic organic compounds. The exact contribution of these OA components to each OA factor depends on the site and the prevailing meteorology during the analysis period.</p>
Abstract. Secondary organic aerosol (SOA) is a major fraction of the total organic aerosol (OA) in the atmosphere. SOA is formed by the partitioning onto pre-existent particles of low vapor pressure products of the oxidation of volatile, intermediate volatility, and semivolatile organic compounds. Oxidation of the precursor molecules results in a myriad of organic products making the detailed analysis of smog chamber experiments difficult and the incorporation of the corresponding results into chemical transport models (CTMs) challenging. The volatility basis set (VBS) is a framework that has been designed to help bridge the gap between laboratory measurements and CTMs. The parametrization of SOA formation for the VBS has been traditionally based on fitting yield measurements of smog chamber experiments. To reduce the uncertainty of this approach we developed an algorithm to estimate the SOA product volatility distribution, effective vaporization enthalpy, and effective accommodation coefficient combining SOA yield measurements with thermograms (from thermodenuders) and areograms (from isothermal dilution chambers) from different experiments and laboratories. The algorithm is evaluated with “pseudo-data” produced from the simulation of the corresponding processes assuming SOA with known properties and introducing experimental error. One of the novel features of our approach is that the proposed algorithm estimates the uncertainty of the predicted yields for different atmospheric conditions (temperature, SOA concentration levels, etc.). The predicted yield uncertainty is significantly less than that of the estimated volatility distributions for all conditions tested.
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