References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-11-19143-2011

Mass-spectrometric identification of primary biological particle markers: indication for low abundance of primary biological material in the pristine submicron aerosol of Amazonia

Schneider

¹ Freutel

¹ Zorn

S. R.

¹ ² Chen

² Farmer

D. K.

³ Jimenez

J. L.

³ Martin

S. T.

² Artaxo

⁴ Wiedensohler

⁵ Borrmann

¹ ⁶

Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany

School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA

Dept. of Chem. & Biochem. & CIRES, University of Colorado, Boulder, CO, USA

Applied Physics Department, Institute of Physics, University of São Paulo, Brazil

Leibniz Institute for Tropospheric Research, Leipzig, Germany

Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Germany

05 07 2011

11 7 19143 19178

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys-discuss.net/11/19143/2011/acpd-11-19143-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/11/19143/2011/acpd-11-19143-2011.pdf

The abundance of marker compounds for primary biological particles in submicron aerosol was investigated by means of aerosol mass spectrometry. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker peaks were identified. The identified marker peaks were compared with mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the Central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker peaks places upper limits of 7.5 % for amino acids and 5.6 % for carbohydrates on the contribution of primary biological aerosol particles (PBAPs) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m<sup>−3</sup>. Carbohydrates and protein amino acids make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAPs mass fraction of about 20 % to the submicron organic aerosol.

References 1

Aiken,~A C., Salcedo,~D., Cubison,~M J., Huffman,~J A., DeCarlo,~P F., Ulbrich,~I M., Docherty,~K S., Sueper,~D., Kimmel,~J R., Worsnop,~D R., Trimborn,~A., Northway,~M., Stone,~E A., Schauer,~J J., Volkamer,~R M., Fortner,~E., de Foy,~B., Wang,~J., Laskin,~A., Shutthanandan,~V., Zheng,~J., Zhang,~R., Gaffney,~J., Marley,~N A., Paredes-Miranda,~G., Arnott,~W P., Molina,~L T., Sosa,~G., and Jimenez,~J L.: Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part~1: Fine particle composition and organic source apportionment, Atmos. Chem. Phys., 9, 6633–6653, http://dx.doi.org/10.5194/acp-9-6633-2009doi:10.5194/acp-9-6633-2009, 2009.

Alfarra,~M R., Prevot,~A S H., Szidat,~S., Sandradewi,~J., Weimer,~S., Lanz,~V A., Schreiber,~D., Mohr,~M., and Baltensperger,~U.: Identification of the mass spectral signature of organic aerosols from wood burning emissions, Environ. Sci. Technol., 41, 5770–5777, http://dx.doi.org/10.1021/es062289bdoi:10.1021/es062289b, 2007.

Allan,~J D., Jimenez,~J L., Williams,~P I., Alfarra,~M R., Bower,~K N., Jayne,~J T., Coe,~H., and Worsnop,~D R.: Quantitative sampling using an Aerodyne aerosol mass spectrometer – 1 Techniques of data interpretation and error analysis, J Geophys. Res.-Atmos., 108, 4090, 2003.

Allan,~J D., Delia,~A E., Coe,~H., Bower,~K N., Alfarra,~M R., Jimenez,~J L., Middlebrook,~A M., Drewnick,~F., Onasch,~T B., Canagaratna,~M R., Jayne,~J T., and Worsnopf,~D R.: A~generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data, J Aerosol. Sci., 35, 909–922, 2004.

Beyer,~H. and Walter,~W.: Lehrbuch der organischen Chemie, Hirzel, Stuttgart, 1988.

von Blohn,~N., Mitra,~S K., Diehl,~K., and Borrmann,~S.: The ice nucleating ability of pollen: Part III: New laboratory studies in immersion and contact freezing modes including more pollen types, Atmos. Res., 78, 182–189, http://dx.doi.org/10.1016/j.atmosres.2005.03.008doi:10.1016/j.atmosres.2005.03.008, 2005.

Campos,~M G R., Bogdanov,~S., de Almeida-Muradian,~L B., Szczesna,~T., Mancebo,~Y., Frigerio,~C., and Ferreira,~F.: Pollen composition and standardisation of analytical methods, J. Apicult. Res., 47, 154–161, 2008.

Canagaratna,~M R., Jayne,~J T., Jimenez,~J L., Allan,~J D., Alfarra,~M R., Zhang,~Q., Onasch,~T B., Drewnick,~F., Coe,~H., Middlebrook,~A., Delia,~A., Williams,~L R., Trimborn,~A M., Northway,~M J., DeCarlo,~P F., Kolb,~C E., Davidovits,~P., and Worsnop,~D R.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, 2007.

Chen,~Q., Farmer,~D K., Schneider,~J., Zorn,~S R., Heald,~C L., Karl,~T G., Guenther,~A., Allan,~J D., Robinson,~N., Coe,~H., Kimmel,~J R., Pauliquevis,~T., Borrmann,~S., Poschl,~U., Andreae,~M O., Artaxo,~P., Jimenez,~J L., and Martin,~S T.: Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin, Geophys. Res. Lett., 36, L20806, http://dx.doi.org/10.1029/2009gl039880doi:10.1029/2009gl039880, 2009.

Cubison,~M J., Ortega,~A M., Hayes,~P L., Farmer,~D K., Day,~D., Lechner,~M J., Brune,~W H., Apel,~E., Diskin,~G S., Fisher,~J A., Fuelberg,~H E., Hecobian,~A., Knapp,~D J., Mikoviny,~T., Riemer,~D., Sachse,~G W., Sessions,~W., Weber,~R J., Weinheimer,~A J., Wisthaler,~A., and Jimenez,~J L.: Effects of aging on organic aerosol from open biomass burning smoke in aircraft and lab studies, Atmos. Chem. Phys. Discuss., 11, 12103–12140, http://dx.doi.org/10.5194/acpd-11-12103-2011doi:10.5194/acpd-11-12103-2011, 2011.

Czerwieniec,~G A., Russell,~S C., Tobias,~H J., Pitesky,~M E., Fergenson,~D P., Steele,~P., Srivastava,~A., Horn,~J M., Frank,~M., Gard,~E E., and Lebrilla,~C B.: Stable isotope labeling of entire Bacillus atrophaeus spores and vegetative cells using bioaerosol mass spectrometry, Anal. Chem., 77, 1081–1087, http://dx.doi.org/10.1021/Ac0488098doi:10.1021/Ac0488098, 2005.

DeCarlo,~P F., Kimmel,~J R., Trimborn,~A., Northway,~M J., Jayne,~J T., Aiken,~A C., Gonin,~M., Fuhrer,~K., Horvath,~T., Docherty,~K S., Worsnop,~D R., and Jimenez,~J L.: Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer, Anal. Chem., 78, 8281–8289, 2006.

Deguillaume,~L., Leriche,~M., Amato,~P., Ariya,~P A., Delort,~A.-M., Pöschl,~U., Chaumerliac,~N., Bauer,~H., Flossmann,~A I., and Morris,~C E.: Microbiology and atmospheric processes: chemical interactions of primary biological aerosols, Biogeosciences, 5, 1073–1084, http://dx.doi.org/10.5194/bg-5-1073-2008doi:10.5194/bg-5-1073-2008, 2008.

Diehl,~K., Quick,~C., Matthias-Maser,~S., Mitra,~S K., and Jaenicke,~R.: The ice nucleating ability of pollen – Part~I: Laboratory studies in deposition and condensation freezing modes, Atmos. Res., 58, 75–87, 2001.

Diehl,~K., Matthias-Maser,~S., Jaenicke,~R., and Mitra,~S K.: The ice nucleating ability of pollen – Part~II: Laboratory studies in immersion and contact freezing modes, Atmos. Res., 61, 125–133, 2002.

Duplissy,~J., DeCarlo,~P F., Dommen,~J., Alfarra,~M R., Metzger,~A., Barmpadimos,~I., Prevot,~A S H., Weingartner,~E., Tritscher,~T., Gysel,~M., Aiken,~A C., Jimenez,~J L., Canagaratna,~M R., Worsnop,~D R., Collins,~D R., Tomlinson,~J., and Baltensperger,~U.: Relating hygroscopicity and composition of organic aerosol particulate matter, Atmos. Chem. Phys., 11, 1155–1165, http://dx.doi.org/10.5194/acp-11-1155-2011doi:10.5194/acp-11-1155-2011, 2011.

Elbert,~W., Taylor,~P E., Andreae,~M O., and Pöschl,~U.: Contribution of fungi to primary biogenic aerosols in the atmosphere: wet and dry discharged spores, carbohydrates, and inorganic ions, Atmos. Chem. Phys., 7, 4569–4588, http://dx.doi.org/10.5194/acp-7-4569-2007doi:10.5194/acp-7-4569-2007, 2007.

Fergenson,~D P., Pitesky,~M E., Tobias,~H J., Steele,~P T., Czerwieniec,~G A., Russell,~S C., Lebrilla,~C B., Horn,~J M., Coffee,~K R., Srivastava,~A., Pillai,~S P., Shih,~M T P., Hall,~H L., Ramponi,~A J., Chang,~J T., Langlois,~R G., Estacio,~P L., Hadley,~R T., Frank,~M., and Gard,~E E.: Reagentless detection and classification of individual bioaerosol particles in seconds, Anal. Chem., 76, 373–378, http://dx.doi.org/10.1021/Ac034467edoi:10.1021/Ac034467e, 2004.

Fraser,~M P. and Lakshmanan,~K.: Using levoglucosan as a~molecular marker for the long-range transport of biomass combustion aerosols, Environ. Sci. Technol., 34, 4560–4564, http://dx.doi.org/10.1021/es991229ldoi:10.1021/es991229l, 2000.

Freutel,~F.: Identifizierung charakteristischer massenspektrometrischer Marker für primäre biologische Aerosolpartikel, M.S Thesis, University Mainz, 2009.

Graham,~B., Guyon,~P., Maenhaut,~W., Taylor,~P E., Ebert,~M., Matthias-Maser,~S., Mayol-Bracero,~O L., Godoi,~R H M., Artaxo,~P., Meixner,~F X., Moura,~M A L., Rocha,~C., Van Grieken,~R., Glovsky,~M M., Flagan,~R C., and Andreae,~M O.: Composition and diurnal variability of the natural Amazonian aerosol, J. Geophys. Res.-Atmos., 108, 4765, http://dx.doi.org/10.1029/2003jd004049doi:10.1029/2003jd004049, 2003a. %

Graham,~B., Guyon,~P., Maenhaut,~W., Taylor,~P E., Ebert,~M., %Matthias-Maser,~S., Mayol-Bracero,~O L., Godoi,~R H M., Artaxo,~P., %Meixner,~F X., Moura,~M A L., Rocha,~C., Van Grieken,~R., Glovsky,~M M., %Flagan,~R C., and Andreae,~M O.: Composition and diurnal variability of the %natural Amazonian aerosol, J. Geophys. Res.-Atmos., 108, %http://dx.doi.org/10.1029/2003jd004049doi:10.1029/2003jd004049, 2003b.\blackbox\bfThe same DOI as the reference %before – please check.

Graham,~B., Guyon,~P., Taylor,~P E., Artaxo,~P., Maenhaut,~W., Glovsky,~M M., Flagan,~R C., and Andreae,~M O.: Organic compounds present in the natural Amazonian aerosol: characterization by gas chromatography-mass spectrometry, J. Geophys. Res.-Atmos., 108, http://dx.doi.org/10.1029/2003jd003990doi:10.1029/2003jd003990, 2003b. %

Graham,~B., Guyon,~P., Taylor,~P E., Artaxo,~P., Maenhaut,~W., %Glovsky,~M M., Flagan,~R C., and Andreae,~M O.: Organic compounds present %in the natural Amazonian aerosol: characterization by gas chromatography-mass %spectrometry, J. Geophys. Res.-Atmos., 108, 4766, http://dx.doi.org/10.1029/2003jd003990doi:10.1029/2003jd003990, %2003d.\blackbox\bfThe same DOI as the reference before – please check.

Hinds,~W C.: Aerosol Technology – Properties, Behaviour, and Measurements of Airborne Particles, 2nd edn., John Wiley & Sons, Inc., New York, 1999.

Hogrefe,~O., Drewnick,~F., Lala,~G G., Schwab,~J J., and Demerjian,~K L.: Development, operation and applications of an aerosol generation, calibration and research facility, Aerosol Sci. Technol., 38, 196–214, http://dx.doi.org/10.1080/02786820390229516doi:10.1080/02786820390229516, 2004.

Hoose,~C., Kristjansson,~J E., and Burrows,~S M.: How important is biological ice nucleation in clouds on a~global scale?, Environ. Res. Lett., 5, 024009, http://dx.doi.org/10.1088/1748-9326/5/2/024009doi:10.1088/1748-9326/5/2/024009, 2010.

Huffman,~J A., Docherty,~K S., Aiken,~A C., Cubison,~M J., Ulbrich,~I M., DeCarlo,~P F., Sueper,~D., Jayne,~J T., Worsnop,~D R., Ziemann,~P J., and Jimenez,~J L.: Chemically-resolved aerosol volatility measurements from two megacity field studies, Atmos. Chem. Phys., 9, 7161–7182, http://dx.doi.org/10.5194/acp-9-7161-2009doi:10.5194/acp-9-7161-2009, 2009.

Huffman,~J A., Treutlein,~B., and Pöschl,~U.: Fluorescent biological aerosol particle concentrations and size distributions measured with an Ultraviolet Aerodynamic Particle Sizer (UV-APS) in Central Europe, Atmos. Chem. Phys., 10, 3215–3233, http://dx.doi.org/10.5194/acp-10-3215-2010doi:10.5194/acp-10-3215-2010, 2010.

Iannone,~R., Chernoff,~D I., Pringle,~A., Martin,~S T., and Bertram,~A K.: The ice nucleation ability of one of the most abundant types of fungal spores found in the atmosphere, Atmos. Chem. Phys., 11, 1191–1201, http://dx.doi.org/10.5194/acp-11-1191-2011doi:10.5194/acp-11-1191-2011, 2011.

Jaenicke,~R.: Abundance of cellular material and proteins in the atmosphere, Science, 308, 73–73, 2005.

Jaenicke,~R., Matthias-Maser,~S., and Gruber,~S.: Omnipresence of biological material in the atmosphere, Environ. Chem., 4, 217–220, http://dx.doi.org/10.1071/en07021doi:10.1071/en07021, 2007.

Jones,~A M. and Harrison,~R M.: The effects of meteorological factors on atmospheric bioaerosol concentrations – a~review, Sci. Total Environ., 326, 151–180, http://dx.doi.org/10.1016/j.scitotenv.2003.11.021doi:10.1016/j.scitotenv.2003.11.021, 2004.

Kroll,~J H., Smith,~J D., Che,~D L., Kessler,~S H., Worsnop,~D R., and Wilson,~K R.: Measurement of fragmentation and functionalization pathways in the heterogeneous oxidation of oxidized organic aerosol, Phys. Chem. Chem. Phys., 11, 8005–8014, http://dx.doi.org/10.1039/B905289edoi:10.1039/B905289e, 2009.

Lee,~T., Sullivan,~A P., Mack,~L., Jimenez,~J L., Kreidenweis,~S M., Onasch,~T B., Worsnop,~D R., Malm,~W., Wold,~C E., Hao,~W M., and Collett,~J L.: Chemical smoke marker emissions during flaming and smoldering phases of laboratory open burning of wildland fuels, Aerosol Sci. Technol., 44, I–V, http://dx.doi.org/10.1080/02786826.2010.499884doi:10.1080/02786826.2010.499884, 2010.

Liu,~P S K., Deng,~R., Smith,~K A., Williams,~L R., Jayne,~J T., Canagaratna,~M R., Moore,~K., Onasch,~T B., Worsnop,~D R., and Deshler,~T.: Transmission efficiency of an aerodynamic focusing lens system: Comparison of model calculations and laboratory measurements for the Aerodyne Aerosol Mass Spectrometer, Aerosol Sci. Technol., 41, 721–733, http://dx.doi.org/10.1080/02786820701422278doi:10.1080/02786820701422278, 2007.

Mahowald,~N., Jickells,~T D., Baker,~A R., Artaxo,~P., Benitez-Nelson,~C R., Bergametti,~G., Bond,~T C., Chen,~Y., Cohen,~D D., Herut,~B., Kubilay,~N., Losno,~R., Luo,~C., Maenhaut,~W., McGee,~K A., Okin,~G S., Siefert,~R L., and Tsukuda,~S.: Global distribution of \mboxatmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts, Global Biogeochem. Cy., 22, GB4026, http://dx.doi.org/10.1029/2008gb003240doi:10.1029/2008gb003240, 2008.

Martin,~S T., Andreae,~M O., Althausen,~D., Artaxo,~P., Baars,~H., Borrmann,~S., Chen,~Q., Farmer,~D K., Guenther,~A., Gunthe,~S S., Jimenez,~J L., Karl,~T., Longo,~K., Manzi,~A., Müller,~T., Pauliquevis,~T., Petters,~M D., Prenni,~A J., Pöschl,~U., Rizzo,~L V., Schneider,~J., Smith,~J N., Swietlicki,~E., Tota,~J., Wang,~J., Wiedensohler,~A., and Zorn,~S R.: An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08), Atmos. Chem. Phys., 10, 11415–11438, http://dx.doi.org/10.5194/acp-10-11415-2010doi:10.5194/acp-10-11415-2010, 2010.

Martin,~S T., Andreae,~M O., Artaxo,~P., Baumgardner,~D., Chen,~Q., Goldstein,~A H., Guenther,~A., Heald,~C L., Mayol-Bracero,~O L., McMurry,~P H., Pauliquevis,~T., Poschl,~U., Prather,~K A., Roberts,~G C., Saleska,~S R., Dias,~M A S., Spracklen,~D V., Swietlicki,~E., and Trebs,~I.: Sources and properties of Amazonian aerosol particles, Rev. Geophys., 48, Rg2002, http://dx.doi.org/10.1029/2008rg000280doi:10.1029/2008rg000280, 2010b.

Matthias-Maser,~S. and Jaenicke,~R.: The size distribution of primary biological aerosol particles with radii >0.2 μm in an urban rural influenced region, Atmos. Res., 39, 279–286, 1995.

Möhler,~O., DeMott,~P J., Vali,~G., and Levin,~Z.: Microbiology and atmospheric processes: the role of biological particles in cloud physics, Biogeosciences, 4, 1059–1071, http://dx.doi.org/10.5194/bg-4-1059-2007doi:10.5194/bg-4-1059-2007, 2007.

Möhler,~O., Georgakopoulos,~D G., Morris,~C E., Benz,~S., Ebert,~V., Hunsmann,~S., Saathoff,~H., Schnaiter,~M., and Wagner,~R.: Heterogeneous ice nucleation activity of bacteria: new laboratory experiments at simulated cloud conditions, Biogeosciences, 5, 1425–1435, http://dx.doi.org/10.5194/bg-5-1425-2008doi:10.5194/bg-5-1425-2008, 2008.

Mohr,~C., Huffman,~J A., Cubison,~M J., Aiken,~A C., Docherty,~K S., Kimmel,~J R., Ulbrich,~I M., Hannigan,~M., and Jimenez,~J L.: Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations, Environ. Sci. Technol., 43, 2443–2449, http://dx.doi.org/10.1021/es8011518doi:10.1021/es8011518, 2009.

Morris,~C E., Georgakopoulos,~D G., and Sands,~D C.: Ice nucleation active bacteria and their potential role in precipitation, J. Physi. IV, 121, 87–103, http://dx.doi.org/10.1051/jp4:2004121004doi:10.1051/jp4:2004121004, 2004.

Munk,~K.: Biochemie, Zellbiologie, Ökologie, Evolution, Spektrum Akademischer Verlag, Heidelberg, 2000.

Ng,~N L., Canagaratna,~M R., Zhang,~Q., Jimenez,~J L., Tian,~J., Ulbrich,~I M., Kroll,~J H., Docherty,~K S., Chhabra,~P S., Bahreini,~R., Murphy,~S M., Seinfeld,~J H., Hildebrandt,~L., Donahue,~N M., DeCarlo,~P F., Lanz,~V A., Prévôt,~A S H., Dinar,~E., Rudich,~Y., and Worsnop,~D R.: Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry, Atmos. Chem. Phys., 10, 4625–4641, http://dx.doi.org/10.5194/acp-10-4625-2010doi:10.5194/acp-10-4625-2010, 2010.

Pöschl,~U., Martin,~S T., Sinha,~B W., Chen,~Q., Gunthe,~S S., Huffman,~J A., Borrmann,~S., Farmer,~D., Garland,~R M., Helas,~G., Jimenez,~J., King,~S M., Manzi,~A., Mikhailov,~E., Pauliquevis,~T., Petters,~M D., Prenni,~A J., Roldin,~P., Rose,~D., Schneider,~J., Su,~H., Zorn,~S R., Artaxo,~P., and Andreae,~M O.: Rainforest aerosols as biogenic nuclei of clouds and precipitation in the Amazon, Science, 1513–1516, 2010.

Pratt,~K A., DeMott,~P J., French,~J R., Wang,~Z., Westphal,~D L., Heymsfield,~A J., Twohy,~C H., Prenni,~A J., and Prather,~K A.: In situ detection of biological particles in cloud ice-crystals, Nature Geosci., 2, 397–400, http://dx.doi.org/10.1038/ngeo521doi:10.1038/ngeo521, 2009.

Prenni,~A J., Petters,~M D., Kreidenweis,~S M., Heald,~C L., Martin,~S T., Artaxo,~P., Garland,~R M., Wollny,~A G., and Poschl,~U.: Relative roles of biogenic emissions and Saharan dust as ice nuclei in the Amazon Basin, Nature Geosci., 2, 401–404, http://dx.doi.org/10.1038/ngeo517doi:10.1038/ngeo517, 2009.

Russell,~S C., Czerwieniec,~G., Lebrilla,~C., Tobias,~H., Fergenson,~D P., Steele,~P., Pitesky,~M., Horn,~J., Srivastava,~A., Frank,~M., and Gard,~E E.: Toward understanding the ionization of biomarkers from micrometer particles by bio-aerosol mass spectrometry, J. Am. Soc. Mass Spectrom., 15, 900–909, 2004.

Schneider,~J., Weimer,~S., Drewnick,~F., Borrmann,~S., Helas,~G., Gwaze,~P., Schmid,~O., Andreae,~M O., and Kirchner,~U.: Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles, Int. Mass~J. Spectrom., 258, 37–49, 2006.

Silva,~P J. and Prather,~K A.: Interpretation of mass spectra from organic compounds in aerosol time-of-flight mass spectrometry, Anal. Chem., 72, 3553–3562, 2000.

Simoneit,~B R T., Schauer,~J J., Nolte,~C G., Oros,~D R., Elias,~V O., Fraser,~M P., Rogge,~W F., and Cass,~G R.: Levoglucosan, a~tracer for cellulose in biomass burning and atmospheric particles, Atmos. Environ., 33, 173–182, 1999.

Spiteller,~G.: Massenspektrometrishe Strukturanalyse organischer Verbindungen, Verlag Chemie, Weinheim, 1966.

Spracklen,~D V., Carslaw,~K S., Merikanto,~J., Mann,~G W., Reddington,~C L., Pickering,~S., Ogren,~J A., Andrews,~E., Baltensperger,~U., Weingartner,~E., Boy,~M., Kulmala,~M., Laakso,~L., Lihavainen,~H., Kivekäs,~N., Komppula,~M., Mihalopoulos,~N., Kouvarakis,~G., Jennings,~S G., O'Dowd,~C., Birmili,~W., Wiedensohler,~A., Weller,~R., Gras,~J., Laj,~P., Sellegri,~K., Bonn,~B., Krejci,~R., Laaksonen,~A., Hamed,~A., Minikin,~A., Harrison,~R M., Talbot,~R., and Sun,~J.: Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation, Atmos. Chem. Phys., 10, 4775–4793, http://dx.doi.org/10.5194/acp-10-4775-2010doi:10.5194/acp-10-4775-2010, 2010.

Sun,~Y., Zhang,~Q., Macdonald,~A M., Hayden,~K., Li,~S M., Liggio,~J., Liu,~P S K., Anlauf,~K G., Leaitch,~W R., Steffen,~A., Cubison,~M., Worsnop,~D R., van Donkelaar,~A., and Martin,~R V.: Size-resolved aerosol chemistry on Whistler Mountain, Canada with a high-resolution aerosol mass spectrometer during INTEX-B, Atmos. Chem. Phys., 9, 3095–3111, http://dx.doi.org/10.5194/acp-9-3095-2009doi:10.5194/acp-9-3095-2009, 2009.

Taylor,~P E., Flagan,~R C., Valenta,~R., and Glovsky,~M M.: Release of allergens as respirable aerosols: a~link between grass pollen and asthma, J. Allergy Clin. Immunol., 109, 51–56, http://dx.doi.org/10.1067/mai.2002.120759doi:10.1067/mai.2002.120759, 2002.

Taylor,~P E., Flagan,~R C., Miguel,~A G., Valenta,~R., and Glovsky,~M M.: Birch pollen rupture and the release of aerosols of respirable allergens, Clin. Exp. Allergy, 34, 1591–1596, http://dx.doi.org/10.1111/j.1365-2222.2004.02078.xdoi:10.1111/j.1365-2222.2004.02078.x, 2004.

Tuch,~T M., Haudek,~A., Müller,~T., Nowak,~A., Wex,~H., and Wiedensohler,~A.: Design and performance of an automatic regenerating adsorption aerosol dryer for continuous operation at monitoring sites, Atmos. Meas. Tech., 2, 417–422, http://dx.doi.org/10.5194/amt-2-417-2009doi:10.5194/amt-2-417-2009, 2009.

Watson,~J D., Baker,~T A., Bell,~S P., Gann,~A A F., Levine,~M., and Losick,~R M.: Molecular biology of the gene, 6th ed., Benjamin Cummings, 880 pp., 2007.

Yttri,~K E., Dye,~C., and Kiss,~G.: Ambient aerosol concentrations of sugars and sugar-alcohols at four different sites in Norway, Atmos. Chem. Phys., 7, 4267–4279, http://dx.doi.org/10.5194/acp-7-4267-2007doi:10.5194/acp-7-4267-2007, 2007.