Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 8 24 2008 10.5194/acp-8-7405-2008 http://www.atmos-chem-phys.net/8/7405/2008/ http://www.atmos-chem-phys.net/8/7405/2008/acp-8-7405-2008.html http://www.atmos-chem-phys.net/8/7405/2008/acp-8-7405-2008.pdf 7405 7417 2008-12-12 Direct determination of highly size-resolved turbulent particle fluxes with the disjunct eddy covariance method and a 12 – stage electrical low pressure impactor A. Schmidt andres.schmidt@uni-muenster.de O. Klemm Institute of Landscape Ecology – Climatology, University of Münster, Robert-Koch-Str. 26, 48149 Münster, Germany During summer 2007, turbulent vertical particle mass and number fluxes were measured for a period of 98 days near the city centre of Münster in north-west Germany. For this purpose, a valve controlled disjunct eddy covariance system was mounted at 65 m a.g.l. on a military radio tower. The concentration values for 11 size bins with aerodynamic diameters (D50) from 0.03 to 10 μm were measured with an electrical low pressure impactor. After comparison with other fluxes obtained from 10 Hz measurements with the classical eddy covariance method, the loss of information concerning high frequent parts of the flux could be stated as negligible. The results offer an extended insight in the turbulent atmospheric exchange of aerosol particles by highly size-resolved particle fluxes covering 11 size bins and show that the city of Münster acts as a relevant source for aerosol particles. Significant differences occur between the fluxes of the various particle size classes. While the total particle number flux shows a pattern which is strictly correlated to the diurnal course of the turbulence regime and the traffic intensity, the total mass flux exhibits a single minimum in the evening hours when coarse particles start to deposit. As a result, a mean mass deposition of about 10 mg m−2 per day was found above the urban test site, covering the aerosol size range from 40 nm to 2.0 μm. By contrast, the half-hourly total number fluxes accumulated over the lower ELPI stages range from −4.29×107 to +1.44×108 particles m−2 s−1 and are clearly dominated by the sub-micron particle fraction of the impactor stages with diameters between 40 nm and 320 nm. The averaged number fluxes of particles with diameters between 2.0 and 6.4 μm show lower turbulent dynamics during daytime and partially remarkably high negative fluxes with mean deposition velocities of 2×10−3 m s−1 that appear temporary during noontime and in the evening hours. Altaratz, O., Koren, I., Reisin, T., Kostinski, A., Feingold, G., Levin, Z., and Yin, Y.: Aerosols' influence on the interplay between condensation, evaporation and rain in warm cumulus cloud, Atmos. Chem. Phys., 8, 15–24, 2008. Andreae, M. O., Jones, C. D., and Cox, P. M.: Strong present-day aerosol cooling implies a hot future, Nature, 435, 1187–1190, 2005. Arya, S. P.: Introduction to Micrometeorology, Second Edition, Academic Press, San Diego, 420 pp., 2001. Baron, P. A. and Willeke, K.: Aerosol Measurement – Principles, Techniques, and Applications, Second Edition, John Wiley & Sons, 1172 pp., 2001. Bosveld, F. C. and Beljaars, A. C. M.: The impact of sampling rate on eddy-covariance flux estimates, Agr. Forest Meteorol., 109, 39–45, 2001. Buzorius, G., Rannik, Ü., Nilsson, E. D., Vesala, T., and Kulmala, M.: Analysis of dry deposition velocity measurement techniques for particles smaller than 100 nm, J. Aerosol Sci., 34, 747–764, 2003. Dekati Ltd.: ELPI user manual, Version 4.01, Tampere, Finland, 152 pp., 2006. Donaldson, K., Lia, X. Y., and MacNeea, W.: Ultrafine (nanometre) particle mediated lung injury, J. Aerosol Sci., 29, 553–560, 1998. Donaldson, K., Brown, D., Clouter, A., Duffin, R., MacNee, W., Renwick, L., Tran, L., and Stone, V.: The pulmonary toxicology of ultrafine particles, J. Aerosol Med., 15, 213–220, 2002. Dorsey, J. R., Nemitz, E., Gallagher, M. W., Fowler, D., Williams, P. I., Bower, K. N., and Beswick, K. M.: Direct measurements and parameterisation of aerosol flux, concentration and emission velocity above a city, Atmos. Environ., 36, 791–800, 2002. Foken, T., Göckede, M., Mauder, M., Mahrt, L., Amiro, B. D., and Munger, J. W.: Post-field data quality control, in: Lee, X., Massman, W., and Law, B.: Handbook of Micrometeorology: A Guide for Surface Flux Measurement and Analysis, Kluwer Academic Publishers, Dordrecht, 181–208, 2004. Foken, T.: Angewandte Meteorologie Mikrometeorologische Methoden, Second Edition, Springer, Berlin, Heidelberg, 326 pp., 2006. Finnigan, J. J., Clement, R., Malhi, Y., Leuning, R., and Cleugh, H. A.: A re-evaluation of long-term flux measurement techniques. Part I: Averaging and coordinate rotation, Bound.-Lay. Meteorol., 107, 1–48, 2003. Fratini, G., Ciccioli, P., Febo, A., Forgione, A., and Valentini, R.: Size-segregated fluxes of mineral dust from a desert area of northern China by eddy covariance, Atmos. Chem. Phys., 7, 2839–2854, 2007. Gaman, A., Rannik, Ü., Aalto, P., Pohja, T., Siivola, E., Kulmala, M., and Vesala, T.: Relaxed Eddy Accumulation System for Size-Resolved Aerosol Particle Flux Measurements. J. Atmos. Ocean. Tech., 21, 933–943, 2004. Gietl, J. K., Tritscher, T., and Klemm, O.: Size-segregated analysis of PM$_10 $ at two sites, urban and rural, in Münster (Germany) using five-stage Berner type impactors, Atmos. Environ., 42, 5721–5727, 2008. Gilman, D. L., Fuglister, F. J., and Mitchell Jr., J. M.: On the Power Spectrum of "Red Noise", J. Atmos. Sci., 20, 182–184, 1963. Harris, S. J. and Maricq, M. M.: Signature size distributions for diesel and gasoline engine exhaust particulate matter, J. Aerosol Sci., 32, 749–764, 2001. Hatzianastassiou, N., Wobrock, W., and Flossmann, A. I.: The effect of cloud-processing of aerosol particles on clouds and radiation, Tellus B, 50, 478–490, 1998. Hatzianastassiou, N., Matsoukas, C., Drakakis, E., Stackhouse Jr., P. W., Koepke, P., Fotiadi, A., Pavlakis, K. G., and Vardavas, I.: The direct effect of aerosols on solar radiation based on satellite observations, reanalysis datasets, and spectral aerosol optical properties from Global Aerosol Data Set (GADS), Atmos. Chem. Phys., 7, 2585–2599, 2007. Haugen, D. A.: Effects of sampling rates and averaging periods on meteorological measurements, Proc. Fourth Symp. on Meteorological Observations and Instrumentation, Denver, CO, 15–18, 1978. Held, A., Nowak, A., Wiedensohler, A., and Klemm, O.: Field measurements and size-resolved model simulations of turbulent particle transport to a forest canopy, J. Aerosol Sci., 37, 786–798, 2006. Held, A., Niessner, R., Bosveld, F., Wrzesinsky, T., and Klemm, O.: Evaluation and Application of an Electrical low pressure impactor in disjunct eddy covariance aerosol flux measurements, Aerosol Sci. Tech., 41, 510–519, 2007. Hendriks, D. M. D., Dolman, A. J., van der Molen, M. K., and van Huissteden, J.: A compact and stable eddy covariance set-up for methane measurements using off-axis integrated cavity output spectroscopy, Atmos. Chem. Phys., 8, 431–443, 2008. Ito, K., Christensen, W. F., Eatough, D. J., Henry, R. C., Kim, E., Laden, F., Lall, R., Larson, T. V., Neas, L., Hopke, P. K., and Thurston, G. D.: PM source apportionment and health effects: 2. An investigation of intermethod variability in associations between source-apportioned fine particle mass and daily mortality in Washington, DC, J. Expo. Sci. Env. Epid., 16, 300–310, 2006. Kerminen, V.-M., Pakkanen, T. A., Mäkelä, T., Hillamo, R. E., Sillanpää, M., Rönkkö T., Virtanen, A., Keskinen, J., Pirjola, L., Hussein, T. and Hämeri, K.: Development of particle number size distribution near a major road in Helsinki during an episodic inversion situation, Atmos. Environ., 41, 1759–1767, 2007. Keskinen, J., Pietarinen, K., and Lehtimäki, M.: Electrical Low Pressure Impactor, J. Aerosol Sci. 23, 353–360, 1992. Koren, I., Oreopoulos, L., Feingold, G., Remer, L. A., and Altaratz, O.: How small is a small cloud?, Atmos. Chem. Phys., 8, 3855–3864, 2008. Kramm, G. and Dlugi, R.: Modelling of the Vertical Fluxes of Nitric Acid, Ammonia, and Ammonium Nitrate, J. Atmos. Chem., 18, 319–357, 1994. Lenschow, D. H., Mann, J., and Kristensen, L.: How long is long enough when measuring fluxes and other turbulence statistics?, J. Atmos. Ocean. Tech., 11, 661–673, 1994. Longley, I. D., Gallagher, M. W., Dorsey, J. R. and Flynn, M.: A case-study of fine particle concentrations and fluxes measured in a busy street canyon in Manchester, UK, Atmos. Environ., 38, 3595–3603, 2004. Maricq, M., Podsiadlik, D., and Chase, R.: Examination of the Size-Resolved and Transient Nature of Motor Vehicle Particle Emissions, Environ. Sci. Technol., 33, 1618–1626, 1999. Marjamäki, M., Keskinen, J., Chen, D.-R., and Pui, D. Y. H.: Performance Evaluation of the Electrical Low-Pressure Impactor (ELPI), J. Aerosol Sci., 31, 249–261, 2000. Marjmäki, M., Lemmetty, M., and Keskinen, J.: ELPI Response and Data Reduction I: Response Functions. Aerosol Sci. Tech., 39, 575–582, 2005. Mårtensson, E. M., Nilsson, E. D., Buzorius, G., and Johansson, C.: Eddy covariance measurements and parameterisation of traffic related particle emissions in an urban environment, Atmos. Chem. Phys., 6, 769–785, 2006. Pakkanen, T. A., Makela, T., Hillamo, R. E., Virtanen, A., Ronkko, T., Keskinen, J., Pirjola, L., Parviainen, H., Hussein, T., and Hameri, K.: Monitoring of black carbon and size-segregated particle number concentrations at 9-m and 65-m distances from a major road in Helsinki, Boreal Environ. Res., 11, 296–310, 2006. Panofsky, H. A. and Brier, G. W.: Some Applications of Statistics to Meteorology, The Pennsylvania State University Press, University Park, 224 pp., 1958. Petelski, T.: Marine aerosol fluxes over open sea calculated from vertical concentration gradients, J. Aerosol Sci., 34, 359–371, 2003. Pope, C. A. III, Burnett, R. T., Thun, M. J., Calle, E. E., Krewski, D., Ito, K., and Thurston, G. D.: Lung Cancer, Cardiopulmonary Mortality, and Long-term Exposure to Fine Particulate Air Pollution, J. Am. Med. Assoc., 287, 1132–1141, 2002. Priestley, M. B.: Spectral Analysis and Time Series, Vol. 1 Univariate Series, Academic Press, London, 1981. Pryor, S. C., Larsen, S. E., Sørensen, L. L., Barthelmie, R. J., Grönholm, T., Kulmala, M., Launiainen, S., Rannik, Ü., and Vesala, T.: Particle fluxes over forests: Analyses of flux methods and functional dependencies, J. Geophys. Res., 112, D07205, doi:10.1029/2006JD008066, 2007. Pryor, S. C., Gallagher, M., Sievering, H., Larsen, S. E., Barthelmie, R. J., Birsan, F., Nemitz, E., Rinne, J., Kulmala, M., Grönholm, T., Taipale, R., and Vesala, T.: A review of measurement and modelling results of particle atmosphere-surface exchange, Tellus B, 60, 42–75, 2008. Rinne, H. J. I., Delany, A. C., Greenberg, J. P., and Guenther, A. B.: A true eddy accumulation system for trace gas fluxes using disjunct eddy sampling method., J. Geophys. Res., 105, 24 791–24 798, 2000. Rinne, J., Douffet, T., Prigent, Y., and Durand, P.: Field comparison of disjunct and conventional eddy covariance techniques for trace gas ?ux measurements, Environ. Pollut., 152, 630–635, 2008. Ruuskanen, T. M., Kaasik, M., Aalto, P. P., Hõrrak, U., Vana, M., M\aaartensson, M., Yoon, Y. J., Keronen, P., Mordas, G., Ceburnis, D., Nilsson, E. D., O'Dowd, C., Noppel, M., Alliksaar, T., Ivask, J., Sofiev, M., Prank, M., and Kulmala, M.: Concentrations and fluxes of aerosol particles during the LAPBIAT measurement campaign at Värriö field station, Atmos. Chem. Phys., 7, 3683–3700, 2007. Schmidt, A., Wrzesinsky, T., and Klemm, O.: Gap Filling and Quality Assessment of CO2 and Water Vapour Fluxes above an Urban Area with Radial Basis Function Neural Networks. Bound.-Lay. Meteorol., 126, 389–413, 2008. Schwartz, J., Dockery, D. W., and Neas, L. M.: Is daily mortality associated specifically with fine particles?, J. Air. Waste Manage., 46, 927–939, 1996. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, Second Edition, J. Wiley, New York, 2006. Stull, R. B.: An Introduction to Boundary Layer Meteorol., Dordrecht, Boston, London, Kluwer Acad. Publ., 666 pp., 1988. VanReken, T. M., Rissman, T. A., Roberts, G. C., Varutbangkul, V., Jonsson, H. H., Flagan, R. C., and Seinfeld, J. H.: Toward aerosol/cloud condensation nuclei (CCN) closure during CRYSTAL-FACE, J. Geophys. Res., 108(D20), 4633, doi:10.1029/2003JD003582, 2003. Velasco, E., Pressley, S., Allwine, E., Westberg, H., and Lamb, B.: Measurements of CO2 fluxes from the Mexico City urban landscape, Atmos. Environ., 39, 7433–7446, 2005. Virtanen, A., Marjamäki, M., Ristimäki, J., and Keskinen, J.: Fine particle losses in electrical low-pressure impactor, J. Aerosol Sci., 32, 389–401, 2001. Vogt, R., Christen, A., Rotach, M. W., Roth, M., and Satyanarayana, A. N. V.: Temporal dynamics of CO2 fluxes and profiles over a Central European city, Theor. Appl. Climatol., 84, 117–126, 2006. Vong, R. J., Vickers, D., and Covert, D. S.: Eddy correlation measurements of aerosol deposition to grass, Tellus, 56B, 105–117, 2004. Webb, E. K., Pearman, G. I., ans Leuning, R.: Correction of the flux measurements for density effects due to heat and water vapour transfer, Q. J. Roy. Meteor. Soc., 106, 85–100, 1980. Wilczak, J. M., Oncley, S. P., and Stage, S. A.: Sonic anemometer tilt correction algorithms, Bound.-Lay. Meteorol., 99, 127–150, 2001. Yu, H., Kaufman, Y. J., Chin, M., Feingold, G., Remer, L. A., Anderson, T. L., Balkanski, Y., Bellouin, N., Boucher, O., Christopher, S., DeCola, P., Kahn, R., Koch, D., Loeb, N., Reddy, M. S., Schulz, M., Takemura, T., and Zhou, M.: A review of measurement-based assessments of the aerosol direct radiative effect and forcing, Atmos. Chem. Phys., 6, 613–666, 2006.