Atmospheric Chemistry and Physics Discussions
www.atmos-chem-phys-discuss.net
1680-7367
1680-7375
9
3
2009
10.5194/acpd-9-10913-2009
http://www.atmos-chem-phys-discuss.net/9/10913/2009/
http://www.atmos-chem-phys-discuss.net/9/10913/2009/acpd-9-10913-2009.html
http://www.atmos-chem-phys-discuss.net/9/10913/2009/acpd-9-10913-2009.pdf
10913
10956
2009-05-04
Atmospheric nanoparticle observations in the low free troposphere during upward orographic flows at Izaña Mountain Observatory
S. RodrÃguez
srodriguez@inm.es
Y. González
E. Cuevas
R. Ramos
P. M. Romero
J. Abreu-Afonso
A. Redondas
Izaña Atmospheric Research Centre, AEMET, Associated Unit to CSIC "Studies on Atmospheric Pollution", La Marina 20, Planta 6, E38071, Santa Cruz de Tenerife, Canary Islands, Spain
University of Huelva, Associated Unit to CSIC "Air Pollution", Campus El Carmen, E21071, Huelva, Spain
Institute for Environmental Assessment and Water Research IDAEA, CSIC, Jordi Girona 18, 08034, Barcelona, Spain
This study investigates the processes and conditions favouring the formation
of nanoparticles (diameter <10 nm) which are frequently observed on high
mountains reaching the low free troposphere. This was done through an
analysis of a data set collected at Izaña Global Atmospheric Watch
Observatory (Canary Islands; 2367 m a.s.l.). This high
mountain supersite is located well above the stratocumulus layer
characteristic of the subtropical oceanic tropospheres. At night, when the
catabic flow regime is well established, free troposphere aerosols were
measured. The development of orographic buoyant upward flows during daylight
resulted in an increase of water vapour, SO<sub>2</sub> and NO<sub>y</sub>
concentrations. These ascending airflows perturbed the free troposphere and
resulted in high concentrations of 3–10 nm particles (N<sub>3-10</sub>) due to new
particle formation. An analysis of the 5-min average time series allowed
the identification of two main types of N<sub>3-10</sub> event. In Type I events a
linear relationship between N<sub>3-10</sub> and SO<sub>2</sub> was observed (<i>r</i><sup>2</sup>
coefficients 0.70–0.95 and a mean slope of 11 cm<sup>−3</sup>· ppt<sup>−1</sup>
for 5-min averaged data; SO<sub>2</sub> concentrations from tens to hundreds of
ppt). These particles seem to be formed during upward transport (probably
within or after the outflows of clouds located below Izaña). During Type
II events, no correlation between SO<sub>2</sub> and N<sub>3-10</sub> was observed and
3–10 nm particles were formed in-situ at noon and during the afternoon due
to the condensation of vapours linked to photochemistry. New particle
formation was observed almost every day owing to the favourable conditions
associated with the entry of boundary layer air in the low free troposphere,
even if SO<sub>2</sub> concentrations are rather low at Izaña (tens to
hundreds of ppt). The low surface area of pre-existing particles, low
temperature and high radiation intensity clearly favoured the formation of
nanoparticles. The low surface area of pre-existing particles in the upward
flows is furthered by in-cloud particles scavenging in the stratocumulus
layer typically located below Izaña. The higher temperature and the
presence of coarse Saharan dust particles decrease the efficiency of the new
particle formation mechanisms in summer. Thus, the "N<sub>3-10</sub> versus
SO<sub>2</sub>" slope (for <i>r</i><sup>2</sup>>0.7 cases) was higher in autumn and winter (~15 cm<sup>−3</sup>· ppt<sup>−1</sup> as average) than in summer
(2–8 cm<sup>−3</sup>· ppt<sup>−1</sup>). These field observations suggest that elevated
mounts that reaches the free troposphere may acts as source regions for new
particles.
Alastuey, A., Querol, X., Castillo, S., Escudero, M., Avila, A., Cuevas, E., Torres, C., Romero, P. M., Exposito, F., GarcÃa, O., DÃaz, J. P., Van Dingenen, R., and Putaud, J. P.: Characterisation of TSP and PM$_2.5$ at Izaña and Santa Cruz de Tenerife (Canary Islands, Spain) during a Saharan Dust Episode (July 2002), Atmos. Environ., 39, 4715–4728, 2005.
Allan, J. D., Alfarra, M. R., Bower, K. N., Coe, H., Jayne, J. T., Worsnop, D. R., Aalto, P. P., Kulmala, M., Hyötyläinen, T., Cavalli, F., and Laaksonen, A.: Size and composition measurements of background aerosol and new particle growth in a Finnish forest during QUEST 2 using an Aerodyne Aerosol Mass Spectrometer, Atmos. Chem. Phys., 6, 315–327, 2006.
Clarke, A. D., Varner, J. L., Eisele, F., Maudin, R. L., Tarnner, D., and Litchy, M.: Particle production in the remote marine atmosphere: cloud outflow and subsidence during ACE-1, J. Geophys. Res., 103, 16396–16409, 1998.
Dentener, F., Carmichael, G. R., Zhang, Y., Lelieveld, J., and Crutzen, P. J.: Role of mineral dust as a reactive surface in the global atmosphere, J. Geophys. Res., 101, 22869–22889, 1996.
Fischer, H., Nikitas, C., Parchatka, U., Zenker, T., Harris, G. W., Matuska, P., Schmitt, R., Mihelcic, D., Muesgen, P., Paetz, H. W., Schultz, M., and Volz-Thomas, A.: Trace gas measurements during the oxidizing capacity of the troposphere campaign 1993 at Izaña, J. Geophys. Res., 103, 13505–13518, 1998.
Font, I.: El tiempo atmosférico en las islas Canarias. Servicio Nacional de MeteorologÃa, 96 pp., 1956.
Easter, R. C. and Peters, L. K.: Binary homogeneous nucleation: temperature and relative humidity fluctuations, nonlinearity and aspects of new particle production in the atmosphere, J. Appl. Meteorol., 33, 775–784, 1994.
Eisele, F. L. and McMurry, P. H.: Recent Progress in Understanding Particle Nucleation and Growth, Philos. T. Roy. Soc. B., 352(1350), 191–200, 1997.
Fiedler, V., Dal Maso, M., Boy, M., Aufmhoff, H., Hoffmann, J., Schuck, T., Birmili, W., Hanke, M., Uecker, J., Arnold, F., and Kulmala, M.: The contribution of sulphuric acid to atmospheric particle formation and growth: a comparison between boundary layers in Northern and Central Europe, Atmos. Chem. Phys., 5, 1773–1785, 2005.
Hegg, D. A., Radke, L. F., and Hobbs, P. V.: Measurements of aitken nuclei and cloud condensation nuclei in the marine atmosphere and their relation to the DMS-cloud-climate hypothesis, J. Geophys. Res., 96, 18727–18733, 1991.
Henning, S., Weingartner, E., Schmidt, S., Wendisch, M., Gäggeler, H. W., and Baltenspenger, U.: Size-dependent aerosol activation at the high-alpine site Jungfraujoch (3580 m~a.s.l.), Tellus, 54B, 82–95, 2002.
Kanawade, V. and Tripathi, S. N.: Evidence for the role of ion-induced particle formation during an atmospheric nucleation event observed in Tropospheric Ozone Production about the Spring Equinox (TOPSE), J. Geophys. Res., 111, D02209, doi:10.1029/2005JD006366, 2006.
Kesik, M., Ambus, P., Baritz, R., Brüggemann, N., Butterbach-Bahl, K., Damm, M., Duyzer, J., Horváth, L., Kiese, R., Kitzler, B., Leip, A., Li, C., Pihlatie, M., Pilegaard, K., Seufert, S., Simpson, D., Skiba, U., Smiatek, G., Vesala, T., and Zechmeister-Boltenstern, S.: Inventories of N<sub>2</sub>O and NO emissions from European forest soils, Biogeosciences, 2, 353–375, 2005.
Kim, C. S., Adachi, M., Okuyama, K., and Seinfeld, J. H.: Effect of NO<sub>2</sub> on Particle Formation in SO<sub>2</sub>/H<sub>2</sub>O/air Mixtures by Ion-Induced and Homogenous Nucleation, Aerosol Sci. Tec., 36, 941–952, 2002.
Kleissl, J., Honrath, R. E., Dziobak, M. P., Tanner, D., Val MartÃn, M., Owen, R. C., and Helmig, D.: Occurrence of upslope flows at the Pico mountaintop observatory: A case study of orographic flows on a small, volcanic island, J. Geophys. Res., 112, D10S35, doi:10.1029/2006JD007565, 2007.
Kulmala, M., Pirjola, L., and Mäkela, J. M.: Stable sulphate clusters as a source of new atmospheric particles, Nature, 404, 66–69, 2000.
Kulmala, M., Laakso, L., Lehtinen, K. E. J., Riipinen, I., Dal Maso, M., Anttila, T., Kerminen, V.-M., Hõrrak, U., Vana, M., and Tammet, H.: Initial steps of aerosol growth, Atmos. Chem. Phys., 4, 2553–2560, 2004.
Kulmala, M., Lehtinen, K. E. J., Laakso, L., Mordas, G., and Hämeri, K.: On the existence of neutral atmospheric clusters, Boreal Environ. Res., 10, 79–87, 2005.
Kulmala, M., Lehtinen, K. E. J., and Laaksonen, A.: Cluster activation theory as an explanation of the linear dependence between formation rate of 3 nm particles and sulphuric acid concentration, Atmos. Chem. Phys., 6, 787–793, 2006.
Kulmala, M. and Tammet, H.: Finnish–Estonian air ion and aerosol workshops, Boreal Environ. Res., 12, 237–245, 2007.
Kulmala, M. and Kerminen, V. M.: On the formation and growth of atmospheric nanoparticles, Atmos. Res., 90, 132–150, 2008.
Laaksonen, A., Kulmala, M., O'Dowd, C. D., Joutsensaari, J., Vaattovaara, P., Mikkonen, S., Lehtinen, K. E. J., Sogacheva, L., Dal Maso, M., Aalto, P., Petäjä, T., Sogachev, A., Yoon, Y. J., Lihavainen, H., Nilsson, D., Facchini, M. C., Cavalli, F., Fuzzi, S., Hoffmann, T., Arnold, F., Hanke, M., Sellegri, K., Umann, B., Junkermann, W., Coe, H., Allan, J. D., Alfarra, M. R., Worsnop, D. R., Riekkola, M.-L., Hyötyläinen, T., and Viisanen, Y.: The role of VOC oxidation products in continental new particle formation, Atmos. Chem. Phys., 8, 2657–2665, 2008.
Lee, S.-H., Wilson, J. C., Baumgardner, D., Herman, R. L., Weinstock, E. M., LaFleur, B. G., Kok, G., Anderson, B., Lawson, P., Baker, B., Strawa, A., Pittman, J. V., Reeves, J. M., and Bui, T. P.: NPF observed in the tropical/subtropical cirrus clouds, J. Geophys. Res., 109, D02009, doi:10.1029/2004JD005033, 2004
Maring, H., Savoie, D. L., Izaguirre, M. A., McCormick, C., Arimoto, R., Prospero, J. M., and Pilinis, C.: Aerosol physical and optical properties and their relationship to aerosol composition in the free troposphere at Izaña, Tenerife, Canary Islands, during July 1995, J. Geophys. Res., 105, 14677–14700, 2000.
Marti, J. J, Weber, R. J., McMurry, P. H., Eisele, F., Tanner, D., and Jefferson, A.: New particle formation at a remote continental site: Assessing the contributions of SO<sub>2</sub> and organic precursors, J. Geophys. Res., 102, 6331–6339, 1997.
O'Dowd, C. D., Aalto, P., Hmeri, K., Kulmala, M., and Hoffmann, T.: Aerosol Formation: Atmospheric Particles from Organic Vapours, Nature, 416, 497–498, 2002.
Perry, K. D. and Hobbs, P. V. Further evidence for particle nucleation in clean air adjacent to marine cumulus clouds, J. Geophys. Res., 99, 22803–22818, 1994.
Pirjola, L.: Effects of the increased UV radiation and biogenic VOC emissions on the ultrafine sulphate aerosol formation, J. Aerosol. Sci., 30, 355–367, 1999.
Chiapello, I., Prospero, J. M., Herman, J. R., and Hsu, N. C.:. Detection of mineral dust over the North Atlantic Ocean and Africa with Nimbus 7 TOMS, J. Geophys. Res., 104, 9277–9291, 1999.
Putaud, J. P., Van Dingenen, R., Mangoni, M., Virkkula, A., Raes, F., Maring, H., Prospero, J. M., Swietlicki, E., Berg, O. H., Hillamo, and Mäkela, T.: Chemical mass closure and assessment of the origin of the submicron aerosol in the marine boundary layer and the free troposphere at Tenerife during ACE-2, Tellus, 52B, 141–168, 2000.
Raes, F., Van Dingenen, R., Cuevas, E., Van Velthoven, F. J. V., and Prospero, J. M.: Observations of aerosols in the free troposphere and marine boundary layer of the subtropical Northeast Atlantic: discussion of processes determining their size distribution, J. Geophys. Res., 102, 21315–21328, 1997.
RodrÃguez, S., Van Dingenen, R., Putaud, J. P., Martins-Dos Santos, S., and Roselli, D.: Nucleation and growth of new particles in the rural atmosphere of Northern Italy–-Relationship to air quality monitoring, Atmos. Environ., 39, 6734–6746, 2005.
Schröder, F. P., Kärcher, B., Fiebig, M., and Petzold, A.: Aerosol states in the free troposphere at northern midlatitudes, J. Geophys. Res., 107(D21), 8126, doi:10.1029/2000JD000194, 2002.
Tolocka, M. P., Lake, D. A., Johnston, M. V., and Wexler, A. S.: Ultrafine nitrate particle events in Baltimore observed by real-time single particle mass spectrometry, Atmos. Environ., 38, 3215–3223, 2004.
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, 2009.
Van Dingenen, R., Putaud, J.-P., Martins-Dos Santos, S., and Raes, F.: Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy) during the first MINATROC campaign, Atmos. Chem. Phys., 5, 2203–2226, 2005.
Wiedensohler, A., Hansson, H. C., Orsini, D., Wendisch, M., Wagner, F., Bower, K. N., Choularton, T. W., Wells, M., Parkin, M., Acker, A., Wieprecht, W., Fachini, M. C., Lind, J. A., Fuzzi, S., Arends, B. G., and Kulmala, M.: Nighttime formation and occurrence of new particles associated with orographic clouds, Atmos. Environ., 31, 2545–2559, 1997.
Weber, R. J. and McMurry, P. H.: Fine particle size distribution at the Mauna Loa Observatory, Hawaii, J. Geophys. Res., 101, 14767–14775, 1996.
Weber, R. J., Marti, J. J., McMurry, P. H., Eisele, F. L., Tanner, D. J., and Jefferson, A.: Measurements of new particle formation and ultra fine particle growth at a clean continental site, J. Geophys. Res., 102, 4375–4385, 1997.
Weingartner, E., Nyeki, S., and Baltensperger, U.: Seasonal and diurnal variation of aerosol size distributions (10<D<750 nm) at a high-alpine site (Jungfraujoch 3580 m~a.s.l.), J. Geophys. Res., 104, D21, 26809–26820, 1999.