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Trace element measurements in PM10–2.5, PM2.5–1.0and PM1.0–0.3 aerosol were performed with 2 h time resolutionat kerbside, urban background and rural sites during the ClearfLo winter 2012campaign in London. The environment-dependent variability of emissions wascharacterized using the Multilinear Engine implementation of the positivematrix factorization model, conducted on data sets comprising all three sitesbut segregated by size. Combining the sites enabled separation of sourceswith high temporal covariance but significant spatial variability. Separationof sizes improved source resolution by preventing sources occurring in only asingle size fraction from having too small a contribution for the model toresolve. Anchor profiles were retrieved internally by analysing data subsets,and these profiles were used in the analyses of the complete data sets of allsites for enhanced source apportionment. A total of nine different factors were resolved (notable elements inbrackets): in PM10–2.5, brake wear (Cu, Zr, Sb, Ba), othertraffic-related (Fe), resuspended dust (Si, Ca), sea/road salt (Cl), aged seasalt (Na, Mg) and industrial (Cr, Ni); in PM2.5–1.0, brake wear,other traffic-related, resuspended dust, sea/road salt, aged sea salt andS-rich (S); and in PM1.0–0.3, traffic-related (Fe, Cu, Zr, Sb,Ba), resuspended dust, sea/road salt, aged sea salt, reacted Cl (Cl), S-richand solid fuel (K, Pb). Human activities enhance the kerb-to-ruralconcentration gradients of coarse aged sea salt, typically considered to havea natural source, by 1.7–2.2. These site-dependent concentration differencesreflect the effect of local resuspension processes in London. Theanthropogenically influenced factors traffic (brake wear and othertraffic-related processes), dust and sea/road salt provide furtherkerb-to-rural concentration enhancements by direct source emissions by afactor of 3.5–12.7. The traffic and dust factors are mainly emitted inPM10–2.5 and show strong diurnal variations with concentrationsup to 4 times higher during rush hour than during night-time.Regionally influenced S-rich and solid fuel factors, occurring primarily inPM1.0–0.3, have negligible resuspension influences, andconcentrations are similar throughout the day and across the regions

Advanced source apportionment of size-resolved trace elements at multiple sites in London during winter