Supplement of Vertical and horizontal variability of PM 10 source contributions in Barcelona during SAPUSS

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Supplement of Atmos. Chem. Phys., 16, 6785 6804, 2016 http://www.atmos-chem-phys.net/16/6785/2016/ doi:10.5194/acp-16-6785-2016-supplement Author(s) 2016. CC Attribution 3.0 cense. Supplement of ertical and horizontal variability of PM 10 source contributions in rcelona during SAPUSS Mariola Brines et al. Correspondence to: M. Brines (mariola.brines@idaea.csic.es) The copyright of individual parts of the supplement might differ from the CC-BY 3.0 licence.

Table S1: Average entration of PM 10 analysed species at each site (RS, UB, TM and TC). RS UB TM TC PM 10 (µgm -3 ) 30.7 25.9 24.8 21.8 (µgm -3 ) 3.7 2.5 2.5 2.2 (µgm -3 ) 1.4 0.9 0.7 0.5 C total (µgm -3 ) 5.8 3.4 3.1 2.7 +OM (µgm -3 ) 7.6 5.2 4.9 5.2 CO = 3 (µgm -3 ) 1.1 0.9 0.7 SiO 2 (µgm -3 ) 1.9 1.3 1.5 1.3 Al 2 O 3 (µgm -3 ) 0. 5 0.5 (µgm -3 ) 0.7 0.5 (µgm -3 ) 0.3 (µgm -3 ) 0.3 (µgm -3 ) 0.1 (µgm -3 ) 1.1 0.9 1.2 0.7 SO 2-4 (µgm -3 ) 2.8 2.8 2.7 2.3 NO - 3 (µgm -3 ) 2.6 2.2 2.4 1.6 (µgm -3 ) 1.3 1.2 NH + 4 (µgm -3 ) 0.9 0.7 0.7 0.5 (ngm -3 ) 0.3 Be (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Sc (ngm -3 ) 0.1 <0.1 <0.1 <0.1 (ngm -3 ) 20.1 19.9 15.4 13.8 (ngm -3 ) 6.4 5.9 6.8 4.9 (ngm -3 ) 6.7 4.6 1.9 (ngm -3 ) 9.3 9.4 6.8 5.3 Co (ngm -3 ) 0.1 (ngm -3 ) 4.8 5.2 2.9 2.5 (ngm -3 ) 23.9 15.9 8.3 5.3 (ngm -3 ) 41.1 61.9 27.9 23.8 (ngm -3 ) 0.1 0.1 <0.1 0.1 Ge (ngm -3 ) <0.1 <0.1 (ngm -3 ) 0.3 0.3 (ngm -3 ) 0.5 0.5 0.5 (ngm -3 ) 0.5 0.5 (ngm -3 ) 2.9 2.3 2.2 1.5 Y (ngm -3 ) 0.5 0.3 <0.1 <0.1 Zr (ngm -3 ) 5.8 2.7 5.1 5.3 Nb (ngm -3 ) <0.1 0.1 <0.1 <0.1 Mo (ngm -3 ) 6.1 4.8 3.8 <0.1 (ngm -3 ) 0.1 0.1 0.1 0.1 (ngm -3 ) 5.8 4.6 2.1 2.9 (ngm -3 ) 2.5 1.8 1.3 Cs (ngm -3 ) <0.1 <0.1 <0.1 <0.1 (ngm -3 ) 10.9 13.0 5.6 4.1 (ngm -3 ) 0.3 Ce (ngm -3 ) 0.7 0.5 Pr (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Nd (ngm -3 ) <0.1 <0.1 1

Table S1 (cont.) RS UB TM TC Sm (ngm -3 ) 0.1 0.1 <0.1 <0.1 Eu (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Gd (ngm -3 ) 0.1 0.1 <0.1 <0.1 Tb (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Dy (ngm -3 ) 0.1 0.1 <0.1 <0.1 Ho (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Er (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Tm (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Yb (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Lu (ngm -3 ) <0.1 <0.1 <0.1 <0.1 Hf (ngm -3 ) 0.1 0.1 <0.1 <0.1 Ta (ngm -3 ) <0.1 <0.1 <0.1 <0.1 W (ngm -3 ) 0.1 0.1 0.1 <0.1 Tl (ngm -3 ) <0.1 <0.1 <0.1 <0.1 (ngm -3 ) 6.6 6.8 4.9 5.1 Bi (ngm -3 ) 0.3 0.3 0.1 Th (ngm -3 ) 0.1 0.1 0.1 0.1 U (ngm -3 ) 0.1 0.1 <0.1 0.1 Table S2: Sum of the chemical species contributions to each PMF factor. Exhaust Road Mineral Aged Heavy oil Industrial Sulfate trate & wear dust marine 3 1.17 0.76 9 0 0.59 0.79 9 2

Table S3: Explained variation for each element and each factor. In bold are the species that most contribute to each factor. Exhaust Road Aged Heavy Mineral & wear dust marine oil Industrial Sulfate trate F1 F2 F3 F4 F5 F6 F7 F8 Residuals PM 10 0.16 0.10 0.16 0.15 2 5 0.13 0.15 8 SiO 2 +CO 3 2 3 0.33 0 1 0 0 5 0.16 Al 2 O 3 0 0.35 2 0 0 0 0 2 0 2 0.37 7 6 7 0 0 6 0.15 9 0.11 0.18 0.10 0 0.10 8 0.13 3 1 1 8 0.75 9 0 3 0 4 0 0.13 0 8 6 3 0 3 7 1 4 0.19 0 0 6 1 0 9 2- SO 4 4 1 0.17 2 8 0 0.39 0 8 0.16 0.16 0.10 3 5 0.31 0 6 0.13 7 9 5 3 3 1 0 0 0.12 1 3 4 0 0.71 6 0 0.11 4 6 0.10 3 2 0 7 1 0 0.30 0.18 3 0 3 5 3 4 0 4 7 0.19 0 0 0 4 0 0 0.10 0.14 7 0 0 1 4 9 3 4 0.19 5 6 7 2 0.15 1 8 0.17 3 1 0.34 0 0 0.13 7 8 0.13 3 6 0.36 4 3 5 0.12 3 9 0.13 3 0.17 0.18 6 3 0 6 0.14 0.13 4 0.12 0 0 0.19 0 0.10 2 0.39 7 0 0 0 8 0.16 0 0.30 0.53 3 0 0 1 1 9 3 0.11 0 8 3 5 0 0.50 7 0 8 0 0.30 6 0.11 8 4 9 1 0.11 0.10 1 2 0.14 4 3 0.19 0.12 0.15 0.13 0.13 7 6 0.12 6 0 5 0.19 6 9 0.15 0 0 5 0 0.11 0.34 - NO 3 0 0 0 0 1 0 0 0.97 2 4 1 7 0.52 0 4 0 6 5 + NH 4 0 1 0 0 0 3 0.73 0.10 0.13 8 7 0.12 0 2 0 3 0 9 0.33 7 6 4 0 9 0.10 0.11 0.19 3

PM 10 modelled (μg m -3 ) 70 60 50 40 30 20 10 0 y = 286x - 0.7972 R² = 0.929 0 10 20 30 40 50 60 70 PM 10 measured (μg m -3 ) Figure S1: Modelled (by means of PMF) versus measured PM 10 entrations. 4

Figure S2: Temporal variation of the 8 PMF factors (vehicle exhaust and wear, road dust, mineral, marine, heavy oil, industrial, sulfate and nitrate) and the calculated contributions of Saharan dust, background mineral dust and anthropogenic marine sulfate during the study period. 5

Figure S2 (cont.) 6

Figure S2 (cont.) 7

The polar plots were obtained with the OPENAIR package of R. These plots represent the entration (in our case of certain PMF factors extracted from PM 10 filters) depending on the wind direction and speed. Note that for the sites located in the city (RS, UB and TM) the wind data used is that measured at the Faculty of Physics as it is representative of the city conditions. The wind components applied to the TC site are those measured at the nearby Fabra Observatory. Figure S3: Polar plots representations of the eight PMF factor at each site, calculated sea salt and anthropogenic marine sulfate contributions. Note the different entration scales. 8

Figure S3 (cont.) Figure S4: Average diurnal trends of temperature, wind speed and wind direction during two different regional episodes (REG_1: 29/9-2/10 and REG_2: 14/10-17/10). 9

PMF 9 factors solution The PMF solutions with nine factors showed the same factors shown with the eight solution, with an additional nine one called "-SUL", composed mainly of lenium and Sulfate (see Figure S5) and lacking of any clear temporal trends. sulfate 00 entration (g/g) Figure S5: PMF profile of the sulfate factor. Table S4 shows that most of the factors were broadly conservative. In some stations (TM, TC) the road traffic, mineral and vehicle exhaust and wear are mixed up. The eight factor solution was found more appropriate. Table S4: Temporal correlation coefficients for the factors found in the 8 and 9 factor solution. 8 factor PMF solution 1 ehicle exhaust and wear RS UB TM TC Correlation with same factor found in the 9 factor solution 0.9 2 Road dust 0.9 0.5 0.5 3 Mineral 0.7 4 Aged marine 0.9 0.9 0.7 5 Heavy Oil 0.9 0.7 6 Industrial 0.9 0.7 0.7 7 Sulfate 0.9 0.9 8 trate 0.9 0.7 10

entration (g/g) entration (g/g) entration (g/g) entration (g/g) entration (g/g) entration (g/g) entration (g/g) entration (g/g) 00 00 00 00 00 00 00 00 ehicle exhaust & wear Road dust Aged marine trate Mineral Industrial Heavy oil Sulfate entration (g/g) 00 sulfate Figure S6: Profiles of the each PMF 9 factors solution. 11