R. Fröhlich et al. Correspondence to: A. Prévôt

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1 Supplement of Atmos. Chem. Phys. Discuss.,, 1, doi:19/acpd----supplement Author(s). CC Attribution. License. Supplement of Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (5 m a.s.l.) chemical composition, origins and organic aerosol sources R. Fröhlich et al. Correspondence to: A. Prévôt (andre.prevot@psi.ch) The copyright of individual parts of the supplement might differ from the CC-BY. licence.

2 Roman Fröhlich: Supplement Table S1. Applied a value ranges with reasoning. season a range HOA reason for a range a range BBOA reason for a range summer a <.1: no good separation OOAs a >.7: mixing HOA & OOA autumn 1.. a >.: mixing winter 1 / 1 HOA & OOA..5 a >.5: mixing HOA & BBOA spring 1..5 a <.: large background in a >.5: mixing HOA & OOA summer 1.. a <.: worse separation OOAs..1 a >.1: decrease of m/z & mixing OOA & BBOA.. a >.: mixing HOA & BBOA Table S. Ratios of HOA to EBC for all seasons. season BBOA HOA OOA (I/II) summer 1. % 1. %.1 % /.1 % autumn 1.5 %. %. % winter 1 / 1.9 %. %.5 %. % spring % 5.9 % 1.1 % summer 1.9 %. % 1.1 % % /.1 %

3 Roman Fröhlich: Supplement SMPS mass (μg/m ) SMPS mass (μg/m ) Orthogonal linear fit through origin y = 1.x R =.7 Summer 1 ACSM PM 1 total mass + EBC (μg/m ) Orthogonal linear fit through origin y = 1.x R =.9 Winter 1/1 SMPS mass (μg/m ) SMPS mass (μg/m ) Orthogonal linear fit through origin y = 1.x R =.57 Fall ACSM PM 1 total mass + EBC (μg/m ) Orthogonal linear fit through origin y =.97x R =. Spring ACSM PM 1 total mass + EBC (μg/m ) ACSM PM 1 total mass + EBC (μg/m ) SMPS mass (μg/m ) Orthogonal linear fit through origin y =.9 x R =. Summer 1 SMPS mass (μg/m ) Orthogonal linear fit through origin y =.9911x R =.7 Full period ACSM PM 1 total mass + EBC (μg/m ) ACSM PM 1 total mass + EBC (μg/m ) Fig. S1. Correlation plots of mass estimated from the SMPS measurements versus mass measured by the ToF-ACSM plus equivalent black carbon in µg/m for all seasons. The bottom right panel shows the correlation for the full period. Slopes close to 1 all over the year lead to a constant collection efficiency of 1. 1x1 - NO y /CO red: below threshold -> FT black: above threshold -> IL red: below threshold -> FT black: above threshold -> IL Rn (Bq/m ) UTC Fig. S. NO y/co (upper panel) and Rn concentrations during the same >1-month example period. Applied thresholds are indicated in red. Concentrations above the threshold are considered influenced by PBL air masses. A comparison shows largely the same result for both criteria with Rn showing slightly more PBL influence.

4 Roman Fröhlich: Supplement Average daily NR-PM1 concentration time y = A*exp(-invTau*x) A = 1. ±. invtau = -.9 ± Average daily temperature ( C) Fig. S. Daily average PM 1 in µg/m plotted against daily average temperature T in C. Data is coloured by date. A strong exponential increase at above zero temperatures is observed. It is noted that obviously the exponential function must level off when full vertical mixing with PBL air is reached. 51% 9% south west Ø.7 ug/m 1% Ø.17 ug/m Ø.7 ug/m north Ø.1 ug/m Ø. ug/m % 9% Ø. ug/m summer 1 summer 1 7% Fig. S. Frequency of air mass origin during summer 1 (left) and 1 (right) including average mass concentrations. Air mass origin was calculated according to the description in Sect..5. North includes clusters # & # 7, south includes clusters #, # & # 5 and west includes cluster # as shown in Fig. 5.

5 Roman Fröhlich: Supplement 5 JJA Average total concentra on: 9. ug/m 5.% Magadino, CH m a.s.l. DJF Average total concentra on: 1.5 ug/m.%.5%.5%.%.% 7.% Organics Sulphate Nitrate Ammonium Chloride EBC.% 1.7%.9% 5.5% 1.% Fig. S5. Relative mass contributions measured with a Q-ACSM (NR-PM 1) and an aethalometer (EBC) in the Swiss Magadino plain. Left: summer 1 (June, July & August), right: winter 1 / 1 (December, January & February). µg/m µg/m µg/m µg/m µg/m µg/m µg/m µg/m µg/m I I summer 1 summer 1 autumn 1 winter 1 / 1 spring 1 summer summer BBOA winter 1 / BBOA summer Fig. S. Time series of ME- factors OOA I (dark green), OOA II (light green) and BBOA (brown) for all seasons investigated. BBOA was only identified in winter 1/1 and summer 1.

6 Roman Fröhlich: Supplement µg/m summer µg/m µg/m µg/m µg/m µg/m µg/m µg/m µg/m µg/m HOA summer 1 HOA HOA HOA HOA autumn 1 winter 1 / 1 spring 1 summer 1 autumn 1 winter 1 / 1 spring 1 summer Fig. S7. Time series of ME- factors (orange) and HOA (grey) for all seasons investigated.

7 Roman Fröhlich: Supplement 7 OOA factors (μg/m ) summer 1 I Nitrate Sulphate Sulphate (μg/m ) Nitrate (μg/m ) OOA factors (μg/m ) summer Sulphate (μg/m ) Nitrate (μg/m ) time of day (h, UTC) 1 Fig. S. Diurnal trends of OOA I (dark green), OOA II (light green), SO (red) and NO for summer 1 (top panel) and summer 1 (bottom panel) Global Radiation > Average Global Radiation < Average (μg/m ).... a) CPC number conc. 1 b) Fig. S9. (a) (white trace) in summer 1 with background shaded by average global radiation. Blue (red) means global radiation was below (above) average during that day. (b) CPC number concentrations for the same period.

8 Roman Fröhlich: Supplement μg/m CPC (t-res: 1s) (t-res: 1-min) EBC (t-res: 1-min) HOA (t-res: 1-min) μg/m ng/m number 5 1 dat UTC Fig. S1. One-week time series of HOA (grey, time resolution: 1-min), EBC (black, time resolution: 1-min), (orange, time resolution: 1-min) and CPC number concentration (red, time resolution: 1-s) in August 1. 5 fraction of total org. signal x1 - x CSOA Faber et al. (1) m/z Fig. S11. Top: Mass spectral profile of, extracted by unconstrained PMF from only short-term peak data. Bottom: Mass spectral profile of cigarette smoke measured with an HR-ToF-AMS under laboratory conditions (adapted and recalculated to UMR from Faber et al., 1). The CSOA is only shown up to m/z 1. Correlations given in the text are calculated for m/z > (dashed line).

9 Roman Fröhlich: Supplement 9.5. I summer summer autumn fraction of total organic signal winter 1 / spring I summer summer m/z Fig. S1. Mass spectral profile of OOAs for all seasons extracted by ME-. In both summers OOAs could be split into OOA I (dark green) and OOA II (light green).

10 1 Roman Fröhlich: Supplement Summer 1 % % I 5% % PBL FT Fig. S1. Relative contributions of (dark green) and I (light green) in summer 1 in the FT and with PBL injection C1: FT C: west C: south-east C: south C5: south-west C: north-west C7: north f summer 1 comb. summer 1 I summer 1 summer 1 comb. summer 1 I summer 1 late summer 1 comb. late summer 1 late summer 1 I f f f.. Fig. S1. Triangle plots. Left: Similar to Fig. 9d including data points from a separate ME- analysis of only the late summer 1 overlapping with the summer 1 period. Right: Triangle plot separated by air mass origin after the subtraction of all POA sources identified in the ME- source apportionment. The clusters are the same as in Fig. 5.

11 Roman Fröhlich: Supplement 11 Visitors Terrace Inlet position ~1m Fig. S. Sketch of the Sphinx research station at the JFJ showing inlet location and visitors terrace (original image: courtesy of jungfraubahn.ch).

12 1 Roman Fröhlich: Supplement References 5 Faber, P., Drewnick, F., Veres, P. R., Williams, J., and Borrmann, S.: Anthropogenic sources of aerosol particles in a football stadium: Real-time characterization of emissions from cigarette smoking, cooking, hand flares, and color smoke bombs by high-resolution aerosol mass spectrometry, Atmos. Environ., 77, 1 1, 1.