Daily Trends and Source Apportionment of Ultrafine Particulate Mass (PM 0.1 ) Over an Annual Cycle in a Typical California City

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1 Daily Trends and Source Apportionment of Ultrafine Particulate Mass (PM 0.1 ) Over an Annual Cycle in a Typical California City Toshihiro Kuwayama, Chris R. Ruehl, and Michael J. Kleeman* Department of Civil and Environmental Engineering, University of California at Davis, One Shields Avenue, Davis, California 95616, United States *Corresponding Author. Tel.: ; fax; address: mjkleeman@ucdavis.edu (M.J. Kleeman). Supporting Information ICPMS Sample Extraction Method ICPMS utilized half of the Teflon filters for the extraction process. 30 ml of 75% acetone/25% 1N nitric acid solution was added to the sample vial along with the filter. Acetone was present to remove the metals from the Teflon membrane while the nitric acid kept the ph of the solution low so that metals did not adhere to the sides of the container. Samples were sonicated followed by evaporation of the acetone using nitrogen leaving samples in 4 ml of nitric acid. Previous studies have shown that the method determines total metal concentrations in PM samples that are in very good agreement with results from ICPMS analysis conducted with full HF acid digestion at elevated temperature and pressure [19]. Table S1. Linear regression analysis summary for PM 0.1 Masstosurface area and particle numbertosurface area. Region Type Rural Rural Rural Urban Urban Seasons Summer Summer* Winter Summer Winter Locations Coalinga Coalinga Coalinga Fresno Fresno R 2 (MSA) R 2 (NSA) * MSA NSA High emissions episode PM 0.1 masstosurface area correlation Particle numbertosurface area correlation

2 Table S2. QAQC for 10% sample reruns. 8.34E Pb 3.52E Sb Sn 2.74E Cd Ag 1.17E Mo 1.85E Sr 2.94E Br 2.92E As 1.66E Zn 9.55E Cu 1.98E Ni 1.02E Fe Mn 7.65E Cr V 7.30E Ti 7.45E K 7.45E Cl 7.54E S 2.81E P 1.77E Mg 1.72E Na 3.08E EC 4.31E Pyro 2.10E OC MDL (μg/m 3 ) RSQ Slope (Origin = 0,0) Species 8.34E Pb 3.52E Sb Sn 2.74E Cd Ag 1.17E Mo 1.85E Sr 2.94E Br 2.92E As 1.66E Zn 9.55E Cu 1.98E Ni 1.02E Fe Mn 7.65E Cr V 7.30E Ti 7.45E K 7.45E Cl 7.54E S 2.81E P 1.77E Mg 1.72E Na 3.08E EC 4.31E Pyro 2.10E OC MDL (μg/m 3 ) RSQ Slope (Origin = 0,0) Species

3 Table S3. Daily average species mass from the PMF factor profiles. Species PMF Daily Average Contributions (μg m 3 ) Factor 1 Factor 2 Factor 3 Factor 4 Factor 5 OC 8.28E E E E E04 Pyro 3.12E E E E E04 EC 4.62E E E E E04 Na 4.18E E E06 Mg 2.57E E E05 P 2.17E E E E05 S 2.75E E E E04 Cl 1.76E E E06 K 6.90E E06 Ti 3.89E E E E06 V 1.22E E E E07 Cr 1.69E E E E E06 Mn 2.29E E E E06 Fe 2.51E E E E E04 Ni 7.44E E E E E05 Cu 2.50E E03 Zn 9.91E E E03 As 2.74E E E E E07 Br 7.95E E E E06 Sr 2.72E E06 Mo 3.50E E E E E07 Ag 1.61E E E E E06 Cd 4.47E E E E07 Sn 7.25E E E E E06 Sb 1.39E E E E E07 Pb 6.68E E E E E05

4 (a) Factor 1: Old Diesel Engines 0.06 (b) Factor 2: Residential Wood Smoke PM 0.1 EC Mass Concentration, μg/m (c) Factor 3: Rail (d) Factor 4: Regional Traffic (Gasoline + Diesel Engines) (e) Factor 5: Brake Wear/Paved Road Dust DEC JAN FEB MAR APR MAY JUN JUL AUG SEP OCT Months ( ) Figure S1. Factor contributions to PM 0.1 EC mass concentrations observed at Sacramento, California between October 26, 2009 and November 3, 2010.

5 (a) Factor 1: Old Diesel Engines (b) Factor 2: Residential Wood Smoke 1.00 PM 0.1 OC Mass Concentration, μg/m (c) Factor 3: Rail (d) Factor 4: Regional Traffic (Gasoline + Diesel Engines) (e) Factor 5: Brake Wear/Paved Road Dust 0 DEC JAN FEB MAR APR MAY JUN JUL AUG SEP OCT Months ( ) Figure S2. Factor contributions to PM 0.1 OC mass concentrations observed at Sacramento, California between October 26, 2009 and November 3, 2010.

6 (a) Factor 1: Old Diesel Engines (b) Factor 2: Residential Wood Smoke 0.01 PM 0.1 S Mass Concentration, μg/m 3 No Contribution (c) Factor 3: Rail (d) Factor 4: Regional Traffic (Gasoline + Diesel Engines) 0.01 (e) Factor 5: Brake Wear/Paved Road Dust 0.01 DEC JAN FEB MAR APR MAY JUN JUL AUG SEP OCT Months ( ) Figure S3. Factor contributions to PM 0.1 S mass concentrations observed at Sacramento, California between October 26, 2009 and November 3, 2010.

7 0.075 (a) Factor 1: Old Diesel Engines (b) Factor 2: Residential Wood Smoke 50 PM 0.1 Other Mass Concentration, μg/m (c) Factor 3: Rail (d) Factor 4: Regional Traffic (Gasoline + Diesel Engines) (e) Factor 5: Brake Wear/Paved Road Dust DEC JAN FEB MAR APR MAY JUN JUL AUG SEP OCT Months ( ) Figure S4. Factor contributions to PM 0.1 other mass concentrations observed at Sacramento, California between October 26, 2009 and November 3, Other chemical components include: Na, Mg, P, Cl, K, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Br, Sr, Mo, Ag, Cd, Sn, Sb, and Pb.

8 Monthly Average Sulfur Dioxide, ppb Monthly Average Sulfur Dioxide, ppb PreCTMP Implementation Fine Sulfur Ultrafine Sulfur Monthly Average Ultrafine Sulfur, μg/m Dates Figure S5. Fine and ultrafine sulfur trends observed at Sacramento, California PreCTMP Implementation Sulfur Dioxide Ultrafine Sulfur Monthly Average Ultrafine Sulfur, μg/m Dates Figure S6. Sulfur dioxide and ultrafine sulfur trends at SacramentoDel Paso Manor and Downtown Sacramento, respectively.

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