References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-5625-2011

Investigation of nucleation events vertical extent: a long term study at two different altitude sites

Boulon

¹ Sellegri

¹ Hervo

¹ Picard

¹ Pichon

J.-M.

¹ Fréville

¹ Laj

Laboratoire de Météorologie Physique CNRS UMR6016, Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, France

Laboratoire de Glaciologie et Géophysique de l'Environnement, CNRS UMR5183, Saint Martin d'Héres, France

20 06 2011

11 12 5625 5639

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In this work we present an analysis of the occurrence of nucleation events during more than three years of measurements at two different rural altitude sites, the puy de Dôme research station (1465 m a.s.l.) and the Opme station (660 m a.s.l.), central France. The collected database is a unique combination of scanning mobility particle sizer (10–400 nm), air ion spectrometers (from 0.8 to 42 nm for NTP-conditions), and, neutral clusters and air ion spectrometers (from 0.8 to 42 nm for NTP-conditions) measurements at these two different altitudes nearly located research stations, from February 2007 to June 2010. The seasonality of the frequency of nucleation events was studied at the puy de Dôme station and maximum of events frequency was found during early spring and early autumn. During the measurement period, neither the particle formation rates (J2= 1.382 ± 0.195 s−1) nor the growth rates (GR1.3−20 nm = 6.20 ± 0.12 nm h−1) differ from one site to the other on average. Hovewer, we found that, on 437 sampling days in common to the two sites, the nucleation frequency was higher at the puy de Dôme station (35.9 %, 157 days) than at the low elevation station of Opme (20.8 %, 91 days). LIDAR measurements and the evolution of the potential equivalent temperature revealed that the nucleation could be triggered either (i) within the whole low tropospheric column at the same time from the planetary boundary layer to the top of the interface layer (29.2 %, 47 events), (ii) above the planetary boundary layer upper limit (43.5 %, 70 events), and (iii) at low altitude and then transported, conserving dynamic and properties, at high altitude (24.8 %, 40 events). This is the first time that the vertical extent of nucleation can be studied over a long observational period, allowing for a rigorous statistical analysis of the occurrence of nucleation over the whole lower troposphere. This work highlights the fact that nucleation can occur over a large vertical extent, at least the whole low tropospheric column, and also the fact that it occurs twice as frequently as actually detected in the planetary boundary layer. The role of sulfuric acid and ions in the nucleation process was investigated at the altitude station and no correlation was found between nucleation events and the estimated sulfuric acid concentrations. However, the contribution of ion-induced nucleation was found to be relatively high (12.49 ± 2.03 % of the total nucleation rate).

References 1

Asmi, E., Sipilä, M., Manninen, H E., Vanhanen, J., Lehtipalo, K., Gagné, S., Neitola, K., Mirme, A., Mirme, S., Tamm, E., Uin, J., Komsaare, K., Attoui, M., and Kulmala, M.: Results of the first air ion spectrometer calibration and intercomparison workshop, Atmos Chem Phys., 9, 141–154, http://dx.doi.org/10.5194/acp-9-141-2009doi:10.5194/acp-9-141-2009, 2009.

Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos Chem Phys., 5, 2497–2517, http://dx.doi.org/10.5194/acp-5-2497-2005doi:10.5194/acp-5-2497-2005, 2005.

Bolton, D.: The Computation of Equivalent Potential Temperature, Mon Weather~Rev., 108, 1046–1053, 1980.

Boulon, J., Sellegri, K., Venzac, H., Picard, D., Weingartner, E., Wehrle, G., Collaud Coen, M., Btikofer, R., Flckiger, E., Baltensperger, U., and Laj, P.: New particle formation and ultrafine charged aerosol climatology at a high altitude site in the Alps (Jungfraujoch, 3580 m a.s.l., Switzerland), Atmos. Chem. Phys., 10, 9333–9349, http://dx.doi.org/10.5194/acp-10-9333-2010doi:10.5194/acp-10-9333-2010, 2010.

Brooks, I M.: Finding Boundary Layer Top: Application of a Wavelet Covariance Tranform to Lidar Backscatter profiles, J Atmos Oceanic~Technol., 20, 1092–1105, 2003.

Crumeyrolle, S., Manninen, H E., Sellegri, K., Roberts, G., Gomes, L., Kulmala, M., Weigel, R., Laj, P., and Schwarzenboeck, A.: New particle formation events measured on board the ATR-42 aircraft during the EUCAARI campaign, Atmos Chem Phys., 10, 6721–6735, http://dx.doi.org/10.5194/acp-10-6721-2010doi:10.5194/acp-10-6721-2010, 2010.

Dal~Maso, M., Kulmala, M., Lehtinen, K. E J., Mäkelä, J., Aalto, P., and O'Dowd, C.: Condensation and coagulation sinks and formation of nucleation mode particles in coastal and boreal forest boundary layer, J Geophys Res., 107(D19), 8097, http://dx.doi.org/10.1029/2001JD001053doi:10.1029/2001JD001053, 2002.

Draxler, R R. and Rolph, G D.: HYSPLIT (Hybrid Single-Particle Langrangian Integrated Trajectory) Model access via NOAA ARL READY website (http://www.arl.noaa.gov/ready/hysplit4.html), NOAA Air Resources Laboratory, Silver Spring, MD, 2003.

Hamburger, T., McMeeking, G., Minikin, A., Birmili, W., Dall'Osto, M., O'Dowd, C., Flentje, H., Henzing, B., Junninen, H., Kristensson, A., de~Leeuw, G., Stohl, A., Burkhart, J F., Coe, H., Krejci, R., and Petzold, A.: Overview of the synoptic and pollution situation over Europe during the EUCAARI-LONGREX field campaign, Atmos Chem Phys., 11, 1065–1082, http://dx.doi.org/10.5194/acp-11-1065-2011doi:10.5194/acp-11-1065-2011, 2010.

Hirsikko, A., Laakso, L., Hõrrak, U., Aalto, P., Kerminen, V.-M., and Kulmala, M.: Annual and size dependant variation of growth rates and ion concentrations in boreal forest, Boreal. Environ. Res., 10, 357–369, 2005.

Iida, K., Stolzenburg, M., McMurry, P H., Dunn, M J., Smith, J N., Eisele, F., and Keady, P.: Contribution of ion-induced nucleation to new particle formation: Methodology and its application to atmospheric observations in Boulder, Colorado, J Geophys Res., 111, D23 201, http://dx.doi.org/10.1029/2006JD007167doi:10.1029/2006JD007167, 2006.

Kerminen, V.-M., Petäjä, T., Manninen, H E., Paasonen, P., Nieminen, T., Sipilä, M., Junninen, H., Ehn, M., Gagné, S., Laakso, L., Riipinen, I., Vehkamäki, H., Kurten, T., Ortega, I K., Dal~Maso, M., Brus, D., Hyvärinen, A., Lihavainen, H., Leppä, J., Lehtinen, K. E J., Mirme, A., Mirme, S., Hõrrak, U., Berndt, T., Stratmann, F., Birmili, W., Wiedensohler, A., Metzger, A., Dommen, J., Baltensperger, U., Kiendler-Scharr, A., Mentel, T F., Wildt, J., Winkler, P M., Wagner, P E., Petzold, A., Minikin, A., Plass-Dülmer, C., Pöschl, U., Laaksonen, A., and Kulmala, M.: Atmospheric nucleation: highlights of the EUCAARI project and future directions, Atmos Chem Phys., 10, 10829–1048, http://dx.doi.org/10.5194/acp-10-10829-2010doi:10.5194/acp-10-10829-2010, 2010.

Komppula, M., Lihavainen, H., Hatakka, J., Paatero, J., Aalto, P., Kulmala, M., and Viisanen, Y.: Observations of new particle formation and size distributions at two different heights and surroundings in subarctic area in northern Finland, J Geophys Res., 108(D9), 4295, 2003.

Kulmala, M., Vehkamäki, H., Petäjä, T., Dal~Maso, M., Lauri, A., Kerminen, V.-M., Birmili, W., and McMurry, P.: Formation and growth rates of ultrafine atmospheric particles: a review of observations, J Aerosol~Sci., 35, 143–176, 2004.

Kulmala, M., Riipinen, I., Sipilä, M., Manninen, H E., Petäjä, T., Junninen, H., Dal~Maso, M., Mordas, G., Mirme, A., Vana, M., Hirsikko, A., Laakso, L., Harrison, R., Hanson, I., Leung, C., Lehtinen, K. E J., and Kerminen, V.-M.: Towards direct measurements of atmospheric nucleation, Science, 318a, 89–92, 2007.

Lehtinen, K. E J., Dal~Maso, M., Kulmala, M., and Kerminen, V.-M.: Estimating nucleation rates from apparent particle formation rates and vice versa: Revised formulation of the Kerminen-Kulmala equation, J Aerosol~Sci., 38, 988–994, http://dx.doi.org/10.1016/j/jaerosci.2007.06.009doi:10.1016/j/jaerosci.2007.06.009, 2007.

Mäkelä, J M., Riihelä, M., Ukkonen, A., Jokinen, V., and Keskinen, J.: Comparison of mobility equivalent diameter with Kelvin-Thomson diameter using ion mobility data, J Chem Phys., 105, 1562–1571, 1996.

Manninen, H E., Nieminen, T., Asmi, E., Gagné, S., Häkkinen, S., Lehtipalo, K., Aalto, P., Kivekäs, N., Vana, M., Mirme, A., Mirme, S., Hõrrak, U., Plass-Dülmer, C., Stange, G., Kiss, G., Hoffer, A., Moerman, M., Henzing, B., Brinkenberg, M., Kouvarakis, G N., Bougiatioti, K., O'Dowd, C., Ceburnis, D., Arneth, A., Svenningsson, B., Swietlicki, E., Tarozzi, L., Decesari, S., Sonntag, A., Birmili, W., Wiedensohler, A., Boulon, J., Sellegri, K., Laj, P., Baltensperger, U., Laaksonen, A., Joutsensaari, J., Petäjä, T., Kerminen, V.-M., and Kulmala, M.: EUCAARI ion spectrometer measurements at 12 European sites – analysis of new-particle formation events, Atmos Chem Phys., 10, 7907–7927, http://dx.doi.org/10.5194/acp-10-7907-2010doi:10.5194/acp-10-7907-2010, 2010.

Metzger, A., Verheggen, B., Dommen, J., Duplissy, J., Prevot, A S., Weingartner, E., Riipinen, I., Kulmala, M., V., S D., Carslaw, K S., and Baltensperger, U.: Evidence for the role of organics in aerosol particle formation under atmospheric conditions, P. Natl. Acad. Sci. USA, 107, 6646–6651, http://dx.doi.org/10.1073/pnas.0911330107doi:10.1073/pnas.0911330107, 2010.

Mirme, A., Tamm, A., Mordas, G., Vana, M., Uin, J., Mirme, S., Bernotas, T., Laakso, L., Hirsikko, A., and Kulmala, M.: A wide range multi-channel Air Ion Spectrometer, Boreal Environ. Res., 12, 247–264, 2007.

Nieminen, T., Paasonen, P., Manninen, H E., Kerminen, V.-M., and Kulmala, M.: Parameterization of ion-induced nucleation rates based on ambient observations, Atmos Chem Phys., 10, 21697–21720, http://dx.doi.org/10.5194/acpd-10-21697-2010doi:10.5194/acpd-10-21697-2010, 2010.

Nilsson, E D. and Kulmala, M.: The potential for atmospheric mixing processes to enhance the binary nucleation rate, J Geophys Res., 103(D1), 1381–1389, http://dx.doi.org/10.1029/97JD02629doi:10.1029/97JD02629, 1998.

Nilsson, E D., Rannik, U., Kulmala, M., Buzorius, G., and O'Dowd, C D.: Effects of continental boundary layer evolution, convection, turbulence and entrainment, on aerosol formation, Tellus B, 53B, 441–461, 2001.

Nishita, C., Osada, K., Kido, M., and Matsunaga, K.: Nucleation mode particles in upslope valley winds at Mount Norikura, Japan: Implications for the vertical extent of new particle formation events in the lower troposphere, J Geophys Res., 113, D06 202, http://dx.doi.org/10.1029/2007JD009302doi:10.1029/2007JD009302, 2008.

Petäjä, T., Mauldin, III, R L., Kosciuch, E., McGrath, J., Nieminen, T., Boy, M., Adamov, A., Kotiaho, T., and Kulmala, M.: Sulfuric acid and OH concentrations in a boreal forest site, Atmos Chem Phys., 9, 7435–7448, http://dx.doi.org/10.5194/acp-9-7435-2009doi:10.5194/acp-9-7435-2009, 2009.

Pirjola, L., Kulmala, M., Wilck, Bischoff, A., Stratmann, F., and Otto, E.: Formation of sulphuric acid aerosols and cloud condensation nuclei : An expression for significant nucleation and model comparison, J Aerosol~Sci., 30, 1079–1094, 1999.

Shaw, G E.: Aerosols at a mountain top observatory in Arizona, J Geophys Res., 112, D07206, http://dx.doi.org/10.1029/2005JD006893doi:10.1029/2005JD006893, 2007.

Stratmann, F., Siebert, H., Spindler, G., Wehner, B., Althausen, D., Heintzenberg, J., Hellmuth, O., Rinke, R., Schmieder, U., Seidel, C., Tuch, T., Uhrner, U., Wiedensohler, A., Wandinger, U., Wendisch, M., Schell, D., and Stohl, A.: New-particle formation events in a continental boundary layer: first results from the SATURN experiment, Atmos Chem Phys., 2, 1445–1459, http://dx.doi.org/10.5194/acp-3-1445-2003doi:10.5194/acp-3-1445-2003, 2003.

Tammet, H. and Kulmala, M.: Simulation tool for atmospheric aerosol nucleation bursts, J Aerosol~Sci., 36, 173–196, 2005.

Tunved, P., Nilsson, E D., Hansson, H.-C., Ström, J., Kulmala, M., Aalto, P., and Viisanen, Y.: Aerosol characteristics of air masses in norther Europe: Influences of location, transport, sinks, and sources, J Geophys Res., 110, D07 201, http://dx.doi.org/10.1029/2004JD005085doi:10.1029/2004JD005085, 2005.

Venzac, H., Sellegri, K., and Laj, P.: Nucleation events detected at the high altitude site of the Puy de Dôme research station, France, Boreal Environ. Res., 12, 345–359, 2007.

Venzac, H., Sellegri, K., Laj, P., Villani, P., Bonasoni, P., Marioni, A., Cristofanelli, P., Calzolari, F., Fuzzi, S., Decesari, S., Facchini, M.-C., Vuillermoz, E., and Verza, G.-P.: High frequency new particle formation in the Himalayas, P. Natl. Acad. Sci. USA, 105, 15666–15671, 2008.

Venzac, H., Sellegri, K., Villani, P., Picard, D., and Laj, P.: Seasonal variation of aerosol size distributions in the free troposphere and residual layer at the puy de Dôme station, France, Atmos Chem Phys., 9, 1465–1478, http://dx.doi.org/10.5194/acp-9-1465-2009doi:10.5194/acp-9-1465-2009, 2009.

Wehner, B., Siebert, H., Ansmann, A., Ditas, F., Seifert, P., Stratmann, F., Wiedensohler, A., Apituley, A., Shaw, R. A., Manninen, H. E., and Kulmala, M.: Observations of turbulence-induced new particle formation in the residual layer, Atmos. Chem. Phys., 10, 4319–4330, http://dx.doi.org/10.5194/acp-10-4319-2010doi:10.5194/acp-10-4319-2010, 2010.

Yu, F., Wang, Z., Luo, G., and Turco, R P.: Ion-mediated nucleation as an important global source of tropospheric aerosols, Atmos Chem Phys., 8, 2537–2554, http://dx.doi.org/10.5194/acp-8-2537-2008doi:10.5194/acp-8-2537-2008, 2008.