Abstract. Carbonaceous aerosol (total carbon, TCp) was source
apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme
(EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five
predefined fractions were apportioned based on ambient measurements:
elemental and organic carbon, from combustion of biomass (ECbb and
OCbb) and from fossil-fuel (ECff and OCff) sources, and
remaining non-fossil organic carbon (OCrnf), dominated by natural
sources. OCrnf made a larger contribution to TCp than anthropogenic sources
(ECbb, OCbb, ECff, and OCff) at four out of nine sites
in fall, reflecting the vegetative season, whereas anthropogenic sources
dominated at all but one site in winter/spring. Biomass burning
(OCbb + ECbb) was the major anthropogenic source at the central
European sites in fall, whereas fossil-fuel (OCff + ECff) sources
dominated at the southernmost and the two northernmost sites. Residential
wood burning emissions explained 30 %–50 % of TCp at most sites in the
first week of sampling in fall, showing that this source can be the dominant one,
even outside the heating season. In winter/spring, biomass burning was the
major anthropogenic source at all but two sites, reflecting increased
residential wood burning emissions in the heating season. Fossil-fuel
sources dominated EC at all sites in fall, whereas there was a shift
towards biomass burning for the southernmost sites in winter/spring. Model calculations based on base-case emissions (mainly officially reported
national emissions) strongly underpredicted observational derived levels of
OCbb and ECbb outside Scandinavia. Emissions based on a consistent
bottom-up inventory for residential wood burning (and including intermediate
volatility compounds, IVOCs) improved model results compared to the
base-case emissions, but modeled levels were still substantially
underestimated compared to observational derived OCbb and ECbb
levels at the southernmost sites. Our study shows that natural sources are a major contributor to carbonaceous
aerosol in Europe, even in fall and in winter/spring, and that residential
wood burning emissions are equally as large as or larger than that of fossil-fuel
sources, depending on season and region. The poorly constrained residential
wood burning emissions for large parts of Europe show the obvious need to
improve emission inventories, with harmonization of emission factors between
countries likely being the most important step to improve model calculations
for biomass burning emissions, and European PM2.5 concentrations in
general.