Atmospheric Chemistry and Physics Discussions
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2009
10.5194/acpd-9-20063-2009
http://www.atmos-chem-phys-discuss.net/9/20063/2009/
http://www.atmos-chem-phys-discuss.net/9/20063/2009/acpd-9-20063-2009.html
http://www.atmos-chem-phys-discuss.net/9/20063/2009/acpd-9-20063-2009.pdf
20063
20101
2009-09-25
Measured and predicted aerosol light scattering enhancement factors at the high alpine site Jungfraujoch
R. Fierz-Schmidhauser
P. Zieger
M. Gysel
L. Kammermann
P. F. DeCarlo
U. Baltensperger
E. Weingartner
ernest.weingartner@psi.ch
Laboratory of Atmospheric Chemistry, Paul Scherrer Institut, Villigen, Switzerland
Ambient relative humidity (RH) determines the water content of
atmospheric aerosol particles and thus has an important influence on
the amount of visible light scattered by particles. The RH dependence
of the particle light scattering coefficient (σ<sub>sp</sub>) is
therefore an important variable for climate forcing calculations. We
used a humidification system for a nephelometer which allows for the
measurement of σ<sub>sp</sub> at a defined RH in the range of
20–95%. In this paper we present measurements of light scattering
enhancement factors <i>f</i>(RH)=σ<sub>sp</sub>(RH)/σ<sub>sp</sub>(dry)
from a 1-month campaign (May 2008) at the high alpine site
Jungfraujoch (3580 m a.s.l.), Switzerland. At this site,
<i>f</i>(RH=85%) varied between 1.2 and 3.3. Measured <i>f</i>(RH) agreed well
with <i>f</i>(RH) calculated with Mie theory using measurements of the size
distribution, chemical composition and hygroscopic diameter growth
factors as input. Good <i>f</i>(RH) predictions at RH<85% were also
obtained with a simplified model, which uses the Ångström
exponent of σ<sub>sp</sub>(dry) as input. RH influences further
intensive optical aerosol properties. The backscatter fraction
decreased by about 30% from 0.128 to 0.089, and the single scattering
albedo increased on average by 0.05 at 85% RH compared to dry
conditions. These changes in σ<sub>sp</sub>, backscatter fraction and
single scattering albedo have a distinct impact on the radiative
forcing of the Jungfraujoch aerosol.
Alfarra,~M R., Paulsen,~D., Gysel,~M., Garforth,~A A., Dommen,~J., Prévôt,~A S H., Worsnop,~D R., Baltensperger,~U., and Coe,~H.: A~mass spectrometric study of secondary organic aerosols formed from the photooxidation of anthropogenic and biogenic precursors in a reaction chamber, Atmos. Chem. Phys., 6, 5279–5293, 2006.
Anderson,~T L. and Ogren,~J A.: Determining aerosol radiative properties using the TSI 3563 integrating nephelometer, Aerosol Sci. Tech., 29, 57–69, 1998.
Baltensperger,~U., Gäggeler,~H W., Jost,~D T., Emmenegger,~M., and Nägeli,~W.: Continuous background aerosol monitoring with the epiphaniometer, Atmos. Environ., 25A (3/4), 629–634, 1991.
Baltensperger,~U., Gäggeler,~H W., Jost,~D T., Lugauer,~M., Schwikowski,~M., Weingartner,~E., and Seibert,~P.: Aerosol climatology at the high-alpine site Jungfraujoch, Switzerland, J Geophys. Res., 102(D16), 19707–19715, 1997.
Baltensperger,~U., Schwikowski,~M., Jost,~D T., Nyeki,~S., Gäggeler,~H W., and Poulidas,~O.: Scavenging of the atmospheric constituents in mixed phase clouds at the high-alpine site Jungfraujoch Part~I: Basic concept and aerosol scavenging by clouds, Atmos. Environ., 32(23), 3975–3983, 1998.
Bohren,~C. and Huffmann,~D.: Absorption and Scattering of Light by Small Particles, Wiley-VCH, New York, USA, 2004.
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(2), 185–222, 2007.
Carrico,~C M., Rood,~M J., and Ogren,~J A.: Aerosol light scattering properties at Cape Grim, Tasmania, during the First Aerosol Characterization Experiment (ACE~1), J Geophys. Res., 103, 16565–16574, 1998.
Carrico,~C M., Kus,~P., Rood,~M J., Quinn,~P K., and Bates,~T S.: Mixtures of pollution, dust, sea salt, and volcanic aerosol during ACE-Asia: Radiative properties as a~function of relative humidity, J Geophys. Res., 108(D23), 8650, doi:10.1029/2003JD003405, 2003.
Charlson,~R J., Schwartz,~S E., Hales,~J M., Cess,~R D., Coakley,~J A., Jr., Hansen,~J E., and Hofmann,~D J.: Climate forcing by anthropogenic aerosols, Science, 255, 423–430, 1992.
Collaud Coen,~M., Weingartner,~E., Schaub,~D., Hueglin,~C., Corrigan,~C., Henning,~S., Schwikowski,~M., and Baltensperger,~U.: Saharan dust events at the Jungfraujoch: detection by wavelength dependence of the single scattering albedo and first climatology analysis, Atmos. Chem. Phys., 4, 2465–2480, 2004.
Collaud Coen,~M., Weingartner,~E., Nyeki,~S., Cozic,~J., Henning,~S., Verheggen,~B., Gehrig,~R., and Baltensperger,~U.: Long-term trend analysis of aerosol variables at the high-alpine site Jungfraujoch, J Geophys. Res., 112, D13213, doi:10.1029/2006JD007995, 2007.
Collaud Coen, M., Weingartner, E., Apituley, A., Ceburnis, D., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmidhauser, R., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech. Discuss., 2, 1725–1770, 2009.
Cozic,~J., Verheggen,~B., Weingartner,~E., Crosier,~J., Bower,~K N., Flynn,~M., Coe,~H., Henning,~S., Steinbacher,~M., Henne,~S., Collaud Coen,~M., Petzold,~A., and Baltensperger,~U.: Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch, Atmos. Chem. Phys., 8, 407–423, 2008.
Day,~D E. and Malm,~W C.: Aerosol light scattering measurements as a~function of relative humidity: A~comparison between measurements made at three different sites, Atmos. Environ., 35, 5169–5176, 2001.
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(24), 8281–8289, 2006.
Dinar,~E., Mentel,~T F., and Rudich,~Y.: The density of humic acids and humic like substances (HULIS) from fresh and aged wood burning and pollution aerosol particles, Atmos. Chem. Phys., 6, 5213–5224, 2006.
Fierz-Schmidhauser, R., Zieger, P., Wehrle, G., Jefferson, A., Ogren, J. A., Baltensperger, U., and Weingartner, E.: Measurement of relative humidity dependent light scattering of aerosols, Atmos. Meas. Tech. Discuss., 2, 2161–2190, 2009.
Gosse,~S F., Wang,~M., Labrie,~D., and Chylek,~P.: Imaginary part of the refractive index of sulfates and nitrates in the 0.7–2.6-\unit\mu m spectral region, Appl. Optics, 36(16), 3622–3634, 1997.
Gysel,~M., McFiggans,~G B., and Coe,~H.: Inversion of tandem differential mobility analyser (TDMA) measurements, J Aerosol Sci., 40, 134–151, 2009.
Hale,~G M. and Querry,~M R.: Optical constants of water in the 200-nm to 200-\unit\mu m wavelength region, Appl. Optics, 12, 3, 555–563, 1973.
Haywood,~J M. and Shine,~K P.: The effect of anthropogenic sulfate and soot aerosol on the clear sky planetary radiation budget, Geophys. Res. Lett., 22(5), 603–606, 1995.
Hess,~M., Koepke,~P., and Schult,~I.: Optical properties of aerosols and clouds: The software package OPAC, B Am. Meteorol. Soc., 79(5), 831–844, 1998.
Hummel,~J R. and Reck,~R A.: A~global surface model, J Appl. Meteorol., 18(3), 239–253, 1979.
IPCC: Climate Change 2007 – The Physical Science Basis, edited by: Solomon,~S., Cambridge University Press, New York, 2007.
Kim,~J., Yoon,~S.-C., Jefferson,~A., and Kim,~S.-W.: Aerosol hygroscopic properties during Asian dust, pollution, and biomass burning episodes at Gosan, Korea in April 2001, Atmos. Environ., 40, 1550–1560, 2006.
Koloutsou-Vakakis,~S., Carrico,~C M., Kus,~P., Rood,~M J., Li,~Z., and Shrestha,~R.: Aerosol properties at a~midlatitude Northern Hemisphere continental site, J Geophys. Res., 106(D3), 3019–3032, 2001.
Kotchenruther,~R A. and Hobbs,~P V.: Humidification factors of aerosols from biomass burning in Brazil, J Geophys. Res., 103(D24), 32081–32089, 1998.
Li-Jones,~X., Maring,~H B., and Prospero,~J M.: Effect of relative humidity on light scattering by mineral dust aerosol as measured in the marine boundary layer over the tropical Atlantic Ocean, J Geophys. Res., 103(D23), 31113–31121, 1998.
Li,~J., Wong,~J G D., Dobbie,~J S., and Chylek,~P.: Parameterization of the optical properties of sulfate aerosols, J Atmos. Sci., 58(2), 193–209, 2001.
Lide,~D R.: Handbook of Chemistry and Physics, 89th (Internet Version 2009), CRC Press/Taylor and Francis, Boca Raon, Fl, 2008.
Lugauer,~M., Baltensperger,~U., Furger,~M., Gäggeler,~H W., Jost,~D T., Schwikowski,~M., and Wanner,~H.: Aerosol transport to the high Alpine sites Jungfraujoch (3454 \unitm asl) and Colle Gnifetti (4452 \unitm asl), Tellus, 50B, 76–92, 1998.
Mie,~G.: Beiträge zur Optik trüber Medien, speziell kolloidaler Metalllösungen, Ann. Phys., 25(4), 377–445, 1908.
Nessler,~R., Weingartner,~E., and Baltensperger,~U.: Adaptation of dry nephelometer measurements to ambient conditions at the Jungfraujoch, Environ. Sci. Technol., 39, 2219–2228, 2005a.
Nessler,~R., Weingartner,~E., and Baltensperger,~U.: Effect of humidity on aerosol light absorption and its implications for extinction and the single scattering albedo illustrated for a~site in the lower free troposphere, J Aerosol Sci., 36, 958–972, 2005b.
Nyeki,~S., Baltensperger,~U., Colbeck,~I., Jost,~D T., Weingartner,~E., and Gäggeler,~H W.: The Jungfraujoch high-alpine research station (3454 \unitm) as a~background clean continental site for the measurement of aerosol parameters, J Geophys. Res., 103(D6), 6097–6107, 1998.
Palmer,~K F. and Williams,~D.: Optical constants of sulfuric acid; application to the clouds of Venus?, Appl. Optics, 14(1), 208–219, 1975.
Petters,~M D. and Kreidenweis,~S M.: A~single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, 2007.
Schwartz,~S E.: The whitehouse effect – shortwave radiative forcing of climate by anthropogenic aerosols: An overview, J Aerosol Sci., 27, 359–382, 1996.
Schwikowski,~M., Seibert,~P., Baltensperger,~U., and Gäggeler,~H W.: A~study of an outstanding Saharan dust event at the high-alpine site Jungfraujoch, Switzerland, Atmos. Environ., 29(15), 1829–1842, 1995.
Sheridan,~P J. and Ogren,~J A.: Observation of the vertical and regional variability of aerosol optical properties over central and eastern North America, J Geophys. Res., 104(D14), 16793–16805, 1999.
Sheridan,~P J., Delene,~D J., and Ogren,~J A.: Four years of continuous surface aerosol measurements from the Department of Energy's Atmospheric Radiation Program Southern Great Plains Cloud and Radiation Testbed site, J Geophys. Res., 106, 20735–20747, 2001.
Sjogren,~S., Gysel,~M., Weingartner,~E., Alfarra,~M R., Duplissy,~J., Cozic,~J., Crosier,~J., Coe,~H., and Baltensperger,~U.: Hygroscopicity of the submicrometer aerosol at the high-alpine site Jungfraujoch, 3580 \unitm a.s.l., Switzerland, Atmos. Chem. Phys., 8, 5715–5729, 2008.
Stokes,~R H. and Robinson,~R A.: Interactions in Aqueous Nonelectrolyte Solutions,~I SoluteSolvent Equilibria, J Phys. Chem., 70, 2126–2130, 1966.
Tang,~I N.: Chemical and size effects of hygroscopic aerosols on light scattering coefficients, J Geophys. Res., 101, 19245–19250, 1996.
Toon,~O B., Pollack,~J B., and Khare,~B N.: Optical-constants of several atmospheric aerosol species – ammonium-sulfate, aluminium-oxide, and sodium-chloride, J Geophys. Res.-Oc. Atm., 81(33), 5733–5748, 1976.
Topping,~D O., McFiggans,~G B., and Coe,~H.: A~curved multi-component aerosol hygroscopicity model framework: Part~2 – Including organic compounds, Atmos. Chem. Phys., 5, 1223–1242, 2005.
Wang,~W., Rood,~M J., Carrico,~C M., Covert,~D S., Quinn,~P K., and Bates,~T S.: Aerosol optical properties along the northeast coast of North America during the New England Air Quality Study – Intercontinental Transport and Chemical Transformation 2004 campaign and the influence of aerosol composition, J Geophys. Res., 112, D10S23, doi:10.1029/2006JD007579, 2007.
Weingartner,~E., Nyeki,~S., and Baltensperger,~U.: Seasonal and diurnal variation of aerosol size distributions (10$<D<$750 \unitnm) at a~high-alpine site (Jungfraujoch 3580 \unitm asl), J Geophys. Res., 104(D21), 26809–26820, 1999.
Weingartner,~E., Gysel,~M., and Baltensperger,~U.: Hygroscopicity of aerosol particles at low temperatures, 1 New low-temperature H-TDMA instrument: Setup and first applications, Environ. Sci. Technol., 36, 55–62, 2002.
Weingartner,~E., Saathoff,~H., Schnaiter,~M., Streit,~N., Bitnar,~B., and Baltensperger,~U.: Absorption of light by soot particles: Determination of the absorption coefficient by means of aethalometers, J Aerosol Sci., 34, 1445–1465, 2003.
Wiscombe,~W J. and Grams,~G W.: The backscattered fraction in two-stream approximations, J Atmos. Sci., 33, 2440–2451, 1976.
WMO/GAW: Aerosol Measurement Procedures Guidelines and Recommendations, World Meteorological Organization Global Atmosphere Watch, Geneva, Switzerland, 2003.
Yan,~P., Pan,~X L., Tang,~J., Zhou,~X J., Zhang,~R J., and Zeng,~L M.: Hygroscopic growth of aerosol scattering coefficient: A~comparative analysis between urban and suburban sites at winter in Beijing, Particuology, 7, 52–60, 2009.