European Aerosol Phenomenology -- 8: Harmonised Source Apportionment of Organic Aerosol using 22 Year-long ACSM/AMS Datasets

TL;DR

This study developed a harmonised source apportionment protocol for long-term organic aerosol data across Europe, enabling detailed source identification and quantification to support air quality and climate research.

Contribution

It introduces a state-of-the-art, harmonised source apportionment protocol applied to 22 years of European aerosol data, improving source identification accuracy.

Findings

Oxygenated OA constitutes 71.1% of submicron OA mass on average.

Solid fuel combustion-related OA contributes 16% annually, mainly in winter.

The protocol provides robust, consistent source apportionment across diverse sites.

Abstract

Organic aerosol (OA) is a key component to total submicron particulate matter (PM1), and comprehensive knowledge of OA sources across Europe is crucial to mitigate PM1 levels. Europe has a well-established air quality research infrastructure from which yearlong datasets using 21 aerosol chemical speciation monitors (ACSMs) and 1 aerosol mass spectrometer (AMS) were gathered during 2013-2019. It includes 9 non-urban and 13 urban sites. This study developed a state-of-the-art source apportionment protocol to analyse long-term OA mass spectrum data by applying the most advanced source apportionment strategies (i.e., rolling PMF, ME-2, and bootstrap). This harmonised protocol enables the quantifications of the most common OA components such as hydrocarbon-like OA (HOA), biomass burning OA (BBOA), cooking-like OA (COA), more oxidised-oxygenated OA (MO-OOA), and less oxidised-oxygenated OA (LO-OOA). Other components such as coal combustion OA (CCOA), solid fuel OA (SFOA: mainly mixture of coal and peat combustion), cigarette smoke OA (CSOA), sea salt (mostly inorganic but part of the OA mass spectrum), coffee OA, and ship industry OA could also be separated at a few specific sites. Oxygenated OA (OOA) components make up most of the submicron OA mass (average = 71.1%, a range of 43.7-100%). Solid fuel combustion-related OA components (i.e., BBOA, CCOA, and SFOA) are still considerable with in total 16.0% yearly contribution to the OA, yet mainly during winter months (21.4%). Overall, this comprehensive protocol works effectively across all sites governed by different sources and generates robust and consistent source apportionment results. Our work presents a comprehensive overview of OA sources in Europe with a unique combination of high time resolution and long-term data coverage (9-36 months), providing essential information to improve/validate air quality, health impact, and climate models.