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- ItemParticle formation at a continental background site: Comparison of model results with observations(München : European Geopyhsical Union, 2003) Uhrner, U.; Birmili, W.; Stratmann, F.; Wilck, M.; Ackermann, I.J.; Berresheim, H.At Hohenpeissenberg (47° 48' N, 11° 07' E, 988 m asl), a rural site 200--300~m higher than the surrounding terrain, sulphuric acid concentrations, particle size distributions, and other trace gas concentrations were measured over a two and a half year period. Measured particle number concentrations and inferred particle surface area concentrations were compared with box-model simulations for 12 carefully selected data sets collected during the HAFEX experiment (Birmili et al., 2003). The 12 cases were selected after meteorological and aerosol dynamical criteria in order to justify the use of a box-model. The aerosol model included a binary sulphuric acid water nucleation scheme. Calculated nucleation rates were corrected with a factor to match measured and calculated particle number concentrations. For the investigated 12 data sets, the correction factors were smallest for measurements made under stable thermal stratification and low wind conditions, i.e. conditions that are frequently encountered during winter. Correction factors were largest for measurements made under strong convective conditions. Our comparison of measured and simulated particle size distributions suggests that the particle formation process maybe strongly influenced by mixing processes driven by thermal convection and/or wind sheer.
- ItemHygroscopic properties of different aerosol types over the Atlantic and Indian Oceans(München : European Geopyhsical Union, 2003) Maßling, A.; Wiedensohler, A.; Busch, B.; Neusüß, C.; Quinn, P.; Bates, T.; Covert, D.Hygroscopic properties of atmospheric particles were studied in the marine tropospheric boundary layer over the Atlantic and Indian Oceans during two consecutive field studies: the Aerosols99 cruise (Atlantic Ocean) from 15 January to 20 February 1999, and the INDOEX cruise (Indian Ocean Experiment) from 23 February to 30 March 1999. The hygroscopic properties were compared to optical and chemical properties, such as absorption, chemical inorganic composition, and mass concentration of organic and elemental carbon, to identify the influence of these parameters on hygroscopicity. During the two field studies, four types of aerosol-sampling instruments were used on board the NOAA (National Oceanic and Atmospheric Administration) Research Vessel Ronald H. Brown: Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA), seven-stage cascade impactor, two-stage cascade impactor, and Particle Soot Absorption Photometer (PSAP). The HTDMA was used to determine the hygroscopic properties of atmospheric particles at initial dry sizes (Dp) of 50, 150, and 250 nm and at relative humidities (RH) of 30, 55, 75, and 90%. Simultaneously, a seven-stage cascade impactor of which 3 stages were in the sub-mm size range was used to determine the molar composition of the major inorganic ions such as ammonium and sulfate ions. A two-stage cascade impactor (1 in the sub-mm size range, 1 in the sup-mm size range) was used to determine the mass concentration of organic and elemental carbon. The PSAP was used (at a wavelength of 565 nm) to measure the light absorption coefficient of the aerosol. During the two field studies, air masses of several different origins passed the ship's cruise path. The occurrence of different air masses was classified into special time periods signifying the origin of the observed aerosol. All time periods showed a group of particles with high hygroscopic growth. The measured average hygroscopic growth factors defined by the ratio of dry and wet particle diameter at 90% RH ranged from 1.6 to 2.0, depending on the dry particle size and on the type of air mass. Particles with low hygroscopic growth occurred only when continentally influenced air masses arrived at the ship's position. Distinctions in hygroscopic growth of particles of different air masses were more significant for small relative humidities (30% or 55% RH). High concentrations of elemental carbon corresponded with high light absorption coefficients and with the occurrence of less-hygroscopic and nearly hydrophobic particle fractions in the hygroscopic growth distributions. A key finding is that clean marine air masses that had no land contact for five to six days could clearly be distinguished from polluted air masses that had passed over a continent several days before reaching the ship.
- ItemDependence of solar radiative forcing of forest fire aerosol on ageing and state of mixture(München : European Geopyhsical Union, 2003) Fiebig, M.; Stohl, A.; Wendisch, M.; Eckhardt, S.; Petzold, A.During airborne in situ measurements of particle size distributions in a forest fire plume originating in Northern Canada, an accumulation mode number mean diameter of 0.34 mm was observed over Lindenberg, Germany on 9 August 1998. Realizing that this is possibly the largest value observed for this property in a forest fire plume, scenarios of plume ageing by coagulation are considered to explain the observed size distribution, concluding that the plume dilution was inhibited in parts of the plume. The uncertainties in coagulation rate and transition from external to internal mixture of absorbing forest fire and non-absorbing background particles cause uncertainties in the plume's solar instantaneous radiative forcing of 20-40% and of a factor of 5-6, respectively. Including information compiled from other studies on this plume, it is concluded that the plume's characteristics are qualitatively consistent with a radiative-convective mixed layer.
- ItemNew-particle formation events in a continental boundary layer: First results from the SATURN experiment(München : European Geopyhsical Union, 2003) 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.; Stohl, A.During the SATURN experiment, which took place from 27 May to 14 June 2002, new particle formation in the continental boundary layer was investigated. Simultaneous ground-based and tethered-balloon-borne measurements were performed, including meteorological parameters, particle number concentrations and size distributions, gaseous precursor concentrations and SODAR and LIDAR observations. Newly formed particles were observed inside the residual layer, before the break-up process of the nocturnal inversion, and inside the mixing layer throughout the break-up of the nocturnal inversion and during the evolution of the planetary boundary layer.
- ItemField measurements of hygroscopic properties and state of mixing of nucleation mode particles(München : European Geopyhsical Union, 2002) Väkevä, M.; Kulmala, M.; Stratmann, F.; Hämeri, K.An Ultrafine Tandem Differential Mobility Analyser (UF-TDMA) has been used in several field campaigns over the last few years. The investigations were focused on the origin and properties of nucleation event aerosols, which are observed frequently in various environments. This paper gives a summary of the results of 10 nm and 20 nm particle hygroscopic properties from different measurement sites: an urban site, an urban background site and a forest site in Finland and a coastal site in western Ireland. The data can be classified in four hygroscopic growth classes: hydrofobic, less-hygroscopic, more-hygroscopic and sea-salt. Similar classification has been earlier presented for Aitken and accumulation mode particles. In urban air, the summertime 10 nm particles showed varying less-hygroscopic growth behaviour, while winter time 10 nm and 20 nm particles were externally mixed with two different hygroscopic growth modes. The forest measurements revealed diurnal behaviour of hygroscopic growth, with high growth factors at day time and lower during night. The urban background particles had growth behaviour similar to the urban and forest measurement sites depending on the origin of the observed particles. The coastal measurements were strongly affected by air mass history. Both 10 nm and 20 nm particles were hygroscopic in marine background air. The 10 nm particles produced during clean nucleation burst periods were hydrofobic. Diurnal variation and higher growth factors of 10 nm particles were observed in air affected by other source regions. External mixing was occasionally observed at all the sites, but incidents with more than two growth modes were extremely rare.
- ItemOut of Africa: High aerosol concentrations in the upper troposphere over Africa(München : European Geopyhsical Union, 2003) Heintzenberg, J.; Hermann, M.; Theiss, D.In the year 2000, six flights (three southbound and three northbound) of the CARIBIC project were conducted between Germany and two destinations in the southern hemisphere (Windhoek, Namibia and Cape Town, South Africa). In the present report, results on particle number concentrations are discussed in three size ranges (>4 nm, >12 nm, and >18 nm particle diameter) during the unique transequatorial Africa flights. The flights covered a total of about 80 h in May, July, and December. Thus, no claim can be made for long-term representativeness of the aerosol data. Nevertheless, they are the first upper systematic tropospheric transequatorial aerosol profiles over Africa. The average aerosol results show a broad maximum, roughly symmetrical to the equator, which compares well in latitudinal extent to a maximum of CO concentrations measured on the same flights. This export of continental surface aerosol to the upper troposphere will be dispersed on a global scale both with the easterly flow near the equator and with the westerlies in the adjacent subtropical regions. There was strong evidence of recent new particle formation before aerosol arrival at flight level, in particular during the time periods between 9:00 and 13:00 local time over Africa. Direct and indirect climate effects of the respective particulate matter remain to be investigated by future flights with the ongoing extension of the CARIBIC payload towards size-resolved measurements above 100 nm particle diameter. At the same time global chemical transport models and aerosol dynamics models need to be extended to be able to reproduce the CARIBIC findings over Africa.
- ItemThe Hohenpeissenberg aerosol formation experiment (HAFEX): A long-term study including size-resolved aerosol, H2SO4, OH, and monoterpenes measurements(München : European Geopyhsical Union, 2003) Birmili, W.; Berresheim, H.; Plass-Dülmer, C.; Elste, T.; Gilge, S.; Wiedensohler, A.; Uhrner, U.Ambient aerosol size distributions (>3 nm) and OH, H2SO4, and terpene concentrations were measured from April 1998 to August 2000 at a rural continental site in southern Germany. New particle formation (NPF) events were detected on 18% of all days, typically during midday hours under sunny and dry conditions. The number of newly formed particles correlated significantly with solar irradiance and ambient levels of H2SO4. A pronounced anti-correlatation of NPF events with the pre-existing particle surface area was identified in the cold season, often associated with the advection of dry and relatively clean air masses from southerly directions (Alps). Estimates of the particle formation rate based on observations were around 1 cm-3 s-1, being in agreement with the predictions of ternary homogeneous H2SO4-NH3-H2O nucleation within a few orders of magnitude. The experimentally determined nucleation mode particle growth rates were on average 2.6 nm h-1, with a fraction of 0.7 nm h-1 being attributed to the co-condensation of H2SO4-H2O-NH3. The magnitude of nucleation mode particle growth was neither significantly correlated to H2SO4, nor to the observed particle formation rate. Turn-over rate calculations of measured monoterpenes and aromatic hydrocarbons suggest that especially the oxidation products of monoterpenes have the capacity to contribute to the growth of nucleation mode particles. Although a large number of precursor gases, aerosol and meteorological parameters were measured, the ultimate key factors controlling the occurence of NPF events could not be identified.
- ItemThe impact of multiphase reactions of NO2 with aromatics: A modelling approach(München : European Geopyhsical Union, 2002) Lahoutifard, N.; Ammann, M.; Gutzwiller, L.; Ervens, B.; George, Ch.The impact of multiphase reactions involving nitrogen dioxide (NO2) and aromatic compounds was simulated in this study. A mechanism (CAPRAM 2.4, MODAC Mechanism) was applied for the aqueous phase reactions, whereas RACM was applied for the gas phase chemistry. Liquid droplets were considered as monodispersed with a mean radius of 0.1 µm and a liquid content (LC) of 50 µg m-3. The multiphase mechanism has been further extended to the chemistry of aromatics, i.e. reactions involving benzene, toluene, xylene, phenol and cresol have been added. In addition, reaction of NO2 with dissociated hydroxyl substituted aromatic compounds has also been implemented. These reactions proceed through charge exchange leading to nitrite ions and therefore to nitrous acid formation. The strength of this source was explored under urban polluted conditions. It was shown that it may increase gas phase HONO levels under some conditions and that the extent of this effect is strongly pH dependent. Especially under moderate acidic conditions (i.e. pH above 4) this source may represent more than 75% of the total HONO/NO2 - production rate, but this contribution drops down close to zero in acidic droplets (as those often encountered in urban environments).
- ItemLong term measurements of submicrometer urban aerosols: Statistical analysis for correlations with meteorological conditions and trace gases(München : European Geopyhsical Union, 2003) Wehner, B.; Wiedensohler, A.Long-term measurements (over 4 years) of particle number size distributions (submicrometer particles, 3-800 nm in diameter), trace gases (NO, NO2, and O3), and meteorological parameters (global radiation, wind speed and direction, atmospheric pressure, etc.) were taken in a moderately polluted site in the city of Leipzig (Germany). The resulting complex data set was analyzed with respect to seasonal, weekly, and diurnal variation of the submicrometer aerosol. Car traffic produced a peak in the number size distribution at around 20 nm particle diameter during morning rush hour on weekdays. A second peak at 10-15 nm particle diameter occurred around noon during summer, confirmed by high correlation between concentration of particles less than 20 nm and the global radiation. This new-particle formation at noon was correlated with the amount of global radiation. A high concentration of accumulation mode particles (between 100 and 800 nm), which are associated with large particle-surface area, might prevent this formation. Such high particle concentration in the ultrafine region (particles smaller than 20 nm in diameter) was not detected in the particle mass, and thus, particle mass concentration is not suitable for determining the diurnal patterns of particles. In summer, statistical time series analysis showed a cyclic pattern of ultrafine particles with a period of one day and confirmed the correlation with global radiation. Principal component analysis (PCA) revealed a strong correlation between the particle concentration for 20-800 nm particles and the NO- and NO2-concentrations, indicating the influence of combustion processes on this broad size range, in particular during winter. In addition, PCA also revealed that particle concentration depended on meteorological conditions such as wind speed and wind direction, although the dependence differed with particle size class.
- ItemAerosol number size distributions from 3 to 500 nm diameter in the arctic marine boundary layer during summer and autumn(Copenhagen : Blackwell Munksgaard, 1996) Covert, D.S.; Wiedensohler, A.; Aalto, P.; Heintzenberg, J.; Mcmurry, P.H.; Leck, C.Aerosol physics measurements made onboard the Swedish icebreaker Oden in the late Summer and early Autumn of 1991 during the International Arctic Ocean Expedition (IAOE-91) have provided the first data on the size distribution of particles in the Arctic marine boundary layer (MBL) that cover both the number and mass modes of the size range from 3 to 500 nm diameter. These measurements were made in conjunction with atmospheric gas and condensed phase chemistry measurements in an effort to understand a part of the ocean-atmosphere sulfur cycle. Analysis of the particle physics data showed that there were three distinct number modes in the submicrometric aerosol in the Arctic MBL. These modes had geometric mean diameters of around 170 nm. 45 nm and 14 nm referred to as accumulation, Aitken and ultrafine modes, respectively. There were clear minima in number concentrations between the modes that appeared at 20 to 30 nm and at 80 to 100 nm. The total number concentration was most frequently between 30 and 60 particles cm-3 with a mean value of around 100 particles cm-3, but the hourly average concentration varied over two to three orders of magnitude during the 70 days of the expedition. On average, the highest concentration was in the accumulation mode that contained about 45% of the total number, while the Aitken mode contained about 40%. The greatest variability was in the ultrafine mode concentration which is indicative of active, earby sources (nucleation from the gas phase) and sinks; the Aitken and accumulation mode concentrations were much less variable. The ultrafine mode was observed about two thirds of the time and was dominant 10% of the time. A detailed description and statistical analysis of the modal aerosol parameters is presented here.