Supplement of Evaluation of the performance of a particle concentrator for online instrumentation

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1 Supplement of Atmos. Meas. Tech., 7, , 1 doi:1.519/amt supplement Author(s) 1. CC Attribution 3. License. Supplement of Evaluation of the performance of a particle concentrator for online instrumentation S. Saarikoski et al. Correspondence to: S. Saarikoski (sanna.saarikoski@fmi.fi)

2 Supplements Table S1. The shift of particles size for monodisperse AS and DOS particles in the m- VACES. Particle size (nm) AS % (nm) DOS % (nm) 5 (1) 3 (5.9) (5.) 7.7 (5.) 1. (.). (.) 3.5 (7.) 3.5 (7.) 3. (.). (.)

3 Fig. S1. Time series for the size distributions of particle number (a-b), mass (c-d) and enrichment factor. (a) and (c) are for ambient and (b) and (d) for concentrated aerosol. Particle mass was calculated by using the density of 1. g cm -3.

4 ..3 Acidic particles ambient concentrated 1 Ambient (µg m -3 ) Neutral particles ambient concentrated Concentrated (µg m -3 ) Particle diameter (nm) Fig. S. Size distribution of ammonium during the period when the particles were acidic (April 1, 1) and nearly neutral (April 13, 1; am to midnight). Ambient size distributions were smoothed by one point.

5 concentrated aerosol (µg m -3 ) Hydrocarbon fragments (C x H y ) ambient aerosol (µg m -3 ) concentrated aerosol (µg m -3 ) Organic compounds with one oxygen atom (C 9 x H y O) ambient aerosol (µg m -3 ) 3 concentrated aerosol (µg m -3 ) concentrated aerosol (µg m -3 ) Organic compounds with more than one oxygen atom (C x H y O z (z>1)) ambient aerosol (µg m -3 ) Carbon clusters (C x ) ambient aerosol (µg m -3 ) concentrated aerosol (µg m -3 ) Organic compounds with one nitrogen atom (C x H y N) ambient aerosol (µg m -3 ) Fig. S3. Scatter plots of the mass fragments in ambient and concentrated OA separated into different compound classes. Carbon clusters (C x ) were measured only with the laser on and the concentration of C 1 (m/z 1) according to the fragmentation Table in Onasch et al. (1). Concentrated aerosol is divided by the average EF for organics (7.; a, c- e) and r-bc (37.1; b) (Table ). One to one ratio is shown by dash lines.

6 CH N, C H N, C 3 H N (µg m -3 ) 3 1 a) NH CH N C H N C 3 H N NH (µg m -3 ) b) EF for NH 9-Apr-1 1-Apr-1 11-Apr-1 1-Apr-1 13-Apr-1 1-Apr-1 15-Apr-1 Date Fig. S. Time series of ammonium and amines for the concentrated aerosol (a) and the enrichment factor for ammonium (b).

7 1.7 OM:OC concentrated ambient.5 O:C..35 Elemental ratio H:C concentrated ambient concentrated ambient x1-3 1 N:C concentrated ambient 1 1 Diurnal hour Fig. S5. Diurnal trends for OM:OC, O:C, H:C and N:C for concentrated and ambient OA.

8 Fraction in concentrated OA.1 HOA CH3O C3H5 C3H7 CH7 CH9 CH5 CH3 CO C3H3 C5H9 CHN CH3 C5H11 C5H7 CH9 CH11 C3H3O.1 C5H1C3H CH3O CH CH5 CH CHO C3H5O CH5 C7H7 C7H11 CH7 HO CHO C3H CHO C3H CH5O CH CH3 CH13 C7H13 C5H5 CH7O CH C7H9 C3HO CH C5H7O C5H CH13 C3H CHO C3H7O CH5O CH9 CH CH C5H3 CH1 CH11 C C3HO C9H7 C3H C3H5O CH7O j13cch5 j13cc3h7 CH5O CH1 CHO C3H3O j13cc3h9 C3HO C5H C5H9O CH HO CHO CO j13cch3o CH CH7O C5H7O CH CH3O C5HO C5H j13cch9 CHO C5HO C7H5 C7H9O C7H11O CH15 C7H1 C3HO CH7 C7H1 C3HO C7H Fraction in ambient OA Fraction in concentrated OA.1 C3H3 CH3 C3H3O CH3O CH5 C3H7C3H5 CHO C3H5O CHO CHO CH3 CH.1 C3H5O CH5O CHO CHN C3H3O CH5O CH5O C3H CHN C3HO CH5 CH7 CH3 CHO CH5O CH7O CHO C CH3O C3HO CH5 CH C3H C5H7 C3HO C3HO C5H5 C3H C5H3 CHO CH7O CH CH3O CH CH C3H7O CH7 CH5 C5H7O C9H7C7H7 CH7O C7H5 C5H5O C3HO C5HO C3HO CHO C5HO C5H7O C3H C3HO CH3O C7H9O C9H5 CH C5H C3H C3HN CHO C5H5O C7H11O C5H CH CH3NO C5H9O C3HN CH9 C3H3O3 CH9O C9H3 C7H7O CH7 CH C5H9 C3HN CH3 C5H CH C7H9 CHO CHO CH3O3 CH9 CH9 CHO3 C7HO C9H j13cch3o C7H5O CH.1CHO CH5O.1 OOA Fraction in ambient OA CO CHO CH3O Fraction in concentrated OA.1 CHO HO CH3O C3H3O CH7 C3HO CH C3H3 CHO.1 CHO C5H9 C5H7 C3H5O CH5 C CH5 CH9 C3H CH5O CH5 CH3 CH7 CHO CH9 C7H7 HO C5H7O C5H5 CH C3H CH7O CH5O C3HO C3H7O C3H3O C3H CHN CH CH5O C3H5O CH C3H CH CH CH CO j13cch3o C7H11 CH11 C7H9 CHO C3HO C3HO C5H3 C5H C5H11 C3HO CHO CH7O CHO CH3O C3H9Si C3H CH C5HO C9H7 C5H7O C5H9O CH5O C3HO CH9O CH7O C7H9O CH9 CH11 C7H11O C7H5 CH5 CH C5H1 C5H5O C7H13 CHO j13cch5 CH1 C3HO C5HO CH CH3O CHO CHO CH C9H5 CH13C9H3 CHO CH3 C5H5O CHO CH3O C5H CH7 CH3O.1CH1O C3HO C7H7O CHO.1 OOA Fraction in ambient OA CH3 CH3 C3H5 3 5 CO CH3O.1 Fig. S. Correlation of mass spectra for PMF factors for ambient and concentrated OA.

9 Fig. S7. The variation of Q/Qexpected with the value of fpeak for ambient (a) and concentrated (b) PMF solution.

10 Fig. S. The variation of time series and mass spectra for the PMF factors with the fpeak values from -. to 1.. Ambient (a) and concentrated (b) OA.

11 Detection of trace elements HR-AMS can detect several trace elements with lower melting and boiling points in near real-time (Salcedo et al., 1), and furthermore, the SP-AMS can detect some additional metals and trace elements due to the laser vaporizer (Onasch et al., 1). However, the concentrations of trace metals are typically very low in ambient air, especially in Finland, and therefore their real-time detection is challenging. Thus the use of a concentrator may allow the real-time detection of elements that otherwise could not be observed. Five trace elements were detected in ambient air without the m-vaces; aluminum, vanadium, iron, zinc and rubidium. Except zinc, all of the elements were most likely associated with the laser vaporization as there was a steep drop in the recorded concentrations when the laser vaporizer was switched off. Rubidium can undergo surface ionization with a tungsten vaporizer making its quantification difficult (Drewnick et al., ), similar to sodium and potassium. In this study surface ionization in tungsten vaporizer was not likely to be a confounding issue, as rubidium seemed to be totally vaporized by the laser and not hit the tungsten vaporizer, however, surface ionization can also take place on the hot surface of the r-bc particles discussed more in Carbone et al. (1). Slow evaporation is another issue related to the detection of semi-refractory elements with the AMS, requiring special data analysis procedures (Salcedo et al., 1). Zinc signals were consistent with slow evaporation at tungsten vaporizer the ratio of closed to open being around.7 and.5 for ambient and concentrated aerosol, respectively (Fig. S9). However, a part of the difference could be due to the uncertainty in the detection of low signal for Zn. Trace elements gave rather similar EFs to the other species measured, however, the standard deviations for EFs were large probably due to the high uncertainty associated with the determination of their low ambient concentrations (Table ). Of all the elements, rubidium had the smallest enrichment factor and aluminum the highest. EFs were calculated for the most abundant isotopes (m/z.9 for Al, m/z 5.9 for V, m/z for Fe, m/z.91 for Rb), except for zinc that was detected at the isotope Zn (m/z 7.95). All the other isotopes of V, Fe and Zn could not be resolved from the

12 neighboring peaks or were below their detection limits. The isotopic ratio of 5 Rb and 7 Rb is shown in Fig. S1 for open and closed modes. The isotopic ratio of 7 Rb to 5 Rb was near the natural isotopic ratio of.3 for both the modes. Unfortunately, it was not possible to investigate size-dependent EFs for trace elements as they composed only a minor fraction of the total signal at each unit mass. Additionally, due to the limited data coverage from the laser vaporizer, diurnal patters for the EF could not be calculated. Aluminum, iron and rubidium correlated with r-bc. This suggests that they have similar combustion-related origins in Helsinki, mostly in the form of traffic sources, either from exhaust or non-exhaust (e.g. road dust) emissions. Zinc has been shown to be associated with regional or long-range transported air masses in Helsinki whereas vanadium has more local sources like heavy oil combustion (Pakkanen et al., 1). Besides those five trace elements that were detected in ambient air without the concentrator, three additional elements were detected only with the m-vaces. These elements were strontium, zirconium and cadmium (Fig. S11) and they were identified based on their exact m/z. Strontium was detected at m/z 7.9 and zirconium at m/z 9.95 that were their most abundant isotopes. Cadmium was observed at m/z Unfortunately, any other isotopes of these elements could not be detected, and therefore their existence could not be verified by the isotopic ratios. Of those three, only strontium seemed to be associated with r-bc and vaporized with the laser. However, because zirconium in its elemental form requires about ºC to be vaporized, one possibility is that this trace element was associated with other elements forming for example salts or oxides that could be vaporized with lower temperatures. Neither zirconium nor cadmium showed evidence of slow evaporation in tungsten vaporizer indicated by a signal in the closed mode. Strontium and zirconium did not have any clear correlation with the other species measured whereas cadmium correlated with organics and r-bc. That was unexpected as cadmium did not seem to be in the same particles with r-bc (detected also without laser). Previously cadmium has been related to several sources in Helsinki and it was found to

13 be mostly regional or long-range transported (Pakkanen et al., 1). Strontium, on the other hand, has been associated with traffic-related components from vehicle motor oil but it can also originate from crustal material. Zirconium has not been reported in Helsinki urban air before but in US it has been reported e.g. from the emission of the coal-fired boilers and in samples of geological material (Watson et al., 1995). Ambient (Hz) Concentrated (Hz) Open Closed Open Closed 1-Apr-1 Date 11-Apr-1 Fig. S9. Slow evaporation of zinc. Open and closed signal for ambient and concentrated aerosol.

14 7 Open 1 Closed 7 Rb (ng m -3, RIE=1) 5 3 y =.391*x r = Rb (ng m -3, RIE=1) 1 1 y =.37*x r = Rb (ng m, RIE=1) Rb (ng m, RIE=1) 3 Fig. S1. Scatterplot of signal from 7 Rb and 5 Rb for open and closed modes. Expected natural isotopic ratio is shown by a dash line. 1x1-3 Diff Hz/ns Strontium Ambient Raw fitted Diff Hz/ns Strontium Concentrated 7.95 Raw fitted. 5x1-3 Diff Hz/ns Zirconium Ambient. m/z.1. Raw fitted Diff Hz/ns Zirconium Concentrated m/z.1. Raw fitted. 1x1-3 Diff Hz/ns Cadmium Ambient 9. m/z Raw fitted Diff Hz/ns Cadmium Concentrated m/z Raw fitted m/z m/z Fig. S11. Strontium, zirconium and cadmium peaks for ambient and concentrated aerosol. Additional isotopes of these ions could not be detected.

15 References Carbone, S., Onasch, T., Saarikoski, S., Timonen, H., Sueper, D., Worsnop, D. R., and Hillamo, R.: Trace metals characterization with the SP-AMS: detection and quantification, in preparation, 1. Drewnick, F., Hings, S. S., Curtius, J., Eerdekens, G., Williams, J.: Measurement of fine particulate and gas-phase species during the New Year s fireworks 5 in Mainz, Germany, Atmos. Environ., 31 37,. Onasch, T. B., Trimborn, A., Fortner, E. C., Jayne, J. T., Kok, G. L., Williams, L. R., Davidovits, P., and Worsnop, D. R.: Soot Particle Aerosol Mass Spectrometer: Development, Validation, and Initial Application, Aerosol Sci. Technol.,, -17, 1. Pakkanen, T. A., Loukkola, K., Korhonen, C.H., Aurela, M., Mäkelä, T., Hillamo, R., Aarnio, P., Koskentalo, T., Kousa, A., and Maenhaut, W.: Sources and chemical composition of atmospheric fine and coarse particles in the Helsinki area, Atmos. Environ. 35, , 1. Salcedo, D., Laskin, A., Shutthanandan, V., and J.-L. Jimenez, J.-L.: Feasibility of the Detection of Trace Elements in Particulate Matter Using Online High-Resolution Aerosol Mass Spectrometry, Aerosol Sci. Technol.,, 117-1, 1. Watson, J. G., Chow, J. C., and Houch, J. E.: PM.5 chemical source profiles for vehicle exhaust, vegetative burning, geological material, and coal burning in Northwestern Colorado during 1995, Chemosphere, 3, , 199.

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