Supplement of Chemical and physical characterization of traffic particles in four different highway environments in the Helsinki metropolitan area

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Supplement of Atmos. Chem. Phys., 16, 5497 5512, 2016 http://www.atmos-chem-phys.net/16/5497/2016/ doi:10.5194/acp-16-5497-2016-supplement Author(s) 2016. CC Attribution 3.0 License. Supplement of Chemical and physical characterization of traffic particles in four different highway environments in the Helsinki metropolitan area Joonas Enroth et al. Correspondence to: Liisa Pirjola (liisa.pirjola@metropolia.fi, liisa.pirjola@helsinki.fi) The copyright of individual parts of the supplement might differ from the CC-BY 3.0 licence.

Table S1. Aerosol instrumentation used in the mobile laboratory Sniffer. Instrument Measured parameter Time resolution CPC (Condensation particle number 1 s Particle Counter, TSI) concentrations (diameter > 2.5 nm) ELPI (Electrical Low size distribution, aerodynamic 1 s Pressure Impactor, Dekati) diameter 7 nm - 10 m ELPI + Thermodenuder particle volatility in the 1 s (TD) size range 7 nm 10 m, heated to 265 ºC EEPS (Engine Exhaust size distribution, mobility 1 s Particle Sizer, model 3090, TSI) particle size 5.6-560 nm Aethalometer ( Magee black carbon in PM1 size 10 s Scientific Model AE 33) fraction DustTrak (TSI) PM2.5 1 s SP-AMS (Soot Particle Aerosol Mass Spectrometer) particle chemistry 5 s Table S2. Distances at which the traffic-related pollutant concentrations (background concentrations were first subtracted) were halved from the concentrations at the highway. Ntot PM1 BC Org NO NO2 Herttoniemi 39 26 40 24 26 56 Malmi 83 75 50 34 38 374 Itä-Pakila 8 3 9 <6 13 12 Pitkäjärvi 40 28 31 38 25 90

Table S3. The ratio of NO to NO2 as a function of distance from the highway. Distance Herttoniemi Malmi Itä- Pakila Pitkäjärvi Road 1.80 2.77 1.54 2.54 Roadside 1.14 1.40 1.29 1.69 25 1.07 1.30 1.10 1.50 50 1.06 0.91 0.50 1.27 75 1.12 0.82 0.44 0.89 100 1.20 0.68 0.34 0.78 125 0.83 0.63 0.27 0.70 150 0.57 0.21 0.61 175 0.79 0.20 0.54 200 0.27 0.14 0.49 225 0.15 0.46 250 0.15 0.46 Background 0.04 0.15 0.19 0.22 Table S3. Average particle diameter (nm) of the size distribution as a function of distance from the roadside at different locations. Measurements were carried out by the EEPS. Dave (nm) Highway Roadside 50 100 Background 0 m m m Herttoniemi 25.4 26.2 29.0 25.8 22.0 Malmi 26.9 23.4 24.2 27.5 29.8 Itä-Pakila 27.0 29.5 30.5 33.0 35.6 Pitkäjärvi 18.8 21.3 22.5 22.0 24.2

Figure S1. Total PN concentration averaged over all measurement loops at Itä-Pakila. Figure S2. Average NO concentrations for the entire dataset separated based on the division of morning and evening rush hour occasions. Red line refers to median, plus sign to mean, blue box to 25 and 75 percentiles, and black whiskers to 10 and 90 percentiles.

Figure S3. PM1 mass fractions of BC, organics, nitrate, sulfate and ammonium measured at different distances from the road at Pitkäjärvi. Background concentrations are not subtracted. Figure S4. Concentration gradients for sulfate (a), nitrate (b), ammonium (c), and chloride (d) from each of the four locations. Zero distance refers to the roadside, negative value driving on the highway, and rightmost value to background site ( 500 m from the road). Background concentration were not subtracted from the measured concentrations.

Figure S5. The composition of organic fragments at Pitkäjärvi, Itä-Pakila, Malmi and Herttoniemi for highway, roadside and background locations. CXHY + refers to hydrocarbon fragments, CXHYO + to organic fragments with one oxygen atom and CXHYOZ +, Z>1 to organic fragments with more than one oxygen atom.

Figure S6 Mass spectra for organics and rbc measured at highway, roadside, gradient, and background at Pitkäjärvi (a), the scatter plots for hydrocarbon fragments for roadside and highway (b), and gradient and roadside (c). Gradient refers to the average concentration over all distances, CXHY refers to hydrocarbon fragments, CXHYO to organic fragments with one oxygen atom, CXHYOZ, Z>1 to organic fragments with more than one oxygen atom and Cx to carbon fragments. Note different scales of the y-axes. Hydrocarbon fragments measured at background are subtracted in (b) and (c). Marker size is scaled based on the concentration in (b) and (c).

Figure S7- Mass size distribution measured at the roadside and background at Pitkäjärvi. The composition of organics is presented in insert picture. CXHY + refers to hydrocarbon fragments, CXHYO + to organic fragments with one oxygen atom and CXHYOZ +, Z>1 to organic fragments with more than one oxygen atom. m/z 36 was used as a surrogate for rbc and organics was divided into hydrocarbons and oxidized fractions based on the contributions of m/z 57 and 44 at different size fractions. Figure S8. Particle size distributions for rbc and hydrocarbons at Herttoniemi on 26th of Oct 2012. Measurements at the roadside and 30, 40 and 50 meters from the road. m/z 57 is used as a surrogate for hydrocarbon fragments and m/z 36 for rbc.

Figure S9. Concentration gradients for iron, aluminum, vanadium and zinc at Itä-Pakila and Malmi. Note difference in right side y-axes. Similar figures for Herttoniemi and Pitkäjärvi are presented in the paper. Figure S10. Distribution of emission factors EFPN for the four locations. The average fraction of HD vehicles for Herttoniemi, Malmi, Itä-Pakila and Pitkäjärvi was 2.9, 4.8, 2.8 and 8.7%, respectively, and the total vehicle count 4010, 4630, 6060 and 3720 veh/hour, respectively.