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    MALTE - Model to predict new aerosol formation in the lower troposphere
    (München : European Geopyhsical Union, 2006) Boy, M.; Hellmuth, O.; Korhonen, H.; Nilsson, E.D.; ReVelle, D.; Turnipseed, A.; Arnold, F.; Kulmala, M.
    The manuscript presents a detailed description of the meteorological and chemical code of Malte – a model to predict new aerosol formation in the lower troposphere. The aerosol dynamics are achieved by the new developed UHMA (University of Helsinki Multicomponent Aerosol Model) code with kinetic limited nucleation as responsible mechanism to form new clusters. First results indicate that the model is able to predict the on- and offset of new particle formation as well as the total aerosol number concentrations that were in good agreement with the observations. Further, comparison of predicted and measured H2SO4 concentrations showed a satisfactory agreement. The simulation results indicated that at a certain transitional particle diameter (2–7 nm), organic molecules can begin to contribute significantly to the growth rate compared to sulphuric acid. At even larger particle sizes, organic molecules can dominate the growth rate on days with significant monoterpene concentrations. The intraday vertical evolution of newly formed clusters and particles in two different size ranges resulted in two maxima at the ground. These particles grow around noon to the detectable size range and agree well with measured vertical profiles.
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    Columnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part III: Preliminary results on physicochemical model performance using two "clean air mass" reference scenarios
    (München : European Geopyhsical Union, 2006) Hellmuth, O.
    In Paper I of four papers, a revised columnar high-order model to investigate gas-aerosol-turbulence interactions in the convective boundary layer (CBL) was proposed. In Paper II, the model capability to predict first-, second- and third-order moments of meteorological variables in the CBL was demonstrated using available observational data. In the present Paper III, the high-order modelling concept is extended to sulphur and ammonia chemistry as well as to aerosol dynamics. Based on the previous CBL simulation, a feasibility study is performed using two "clean air mass" scenarios with an emission source at the ground but low aerosol background concentration. Such scenarios synoptically correspond to the advection of fresh post-frontal air in an anthropogenically influenced region. The aim is to evaluate the time-height evolution of ultrafine condensation nuclei (UCNs) and to elucidate the interactions between meteorological and physicochemical variables in a CBL column. The scenarios differ in the treatment of new particle formation (NPF), whereas homogeneous nucleation according to the classical nucleation theory (CNT) is considered. The first scenario considers nucleation of a binary system consisting of water vapour and sulphuric acid (H2SO4) vapour, the second one nucleation of a ternary system additionally involving ammonia (NH3). Here, the two synthetic scenarios are discussed in detail, whereas special attention is payed to the role of turbulence in the formation of the typical UCN burst behaviour, that can often be observed in the surface layer. The intercomparison of the two scenarios reveals large differences in the evolution of the UCN number concentration in the surface layer as well as in the time-height cross-sections of first-order moments and double correlation terms. Although in both cases the occurrence of NPF bursts could be simulated, the burst characteristics and genesis of the bursts are completely different. It is demonstrated, that observations from the surface layer alone are not conclusive to elucidate the origin of newly formed particles. This is also true with respect to the interpretation of box modelling studies. The binary and ternary NPF bursts observed in the surface layer differ with respect to burst amplitude and phase. New particles simulated in the binary scenario are formed in the forenoon in the upper part of the growing CBL, followed by turbulence-induced top-down transport. Hence, with respect to the burst observation site in the surface layer, new particles are formed ex situ. In opposite to this, the ternary case reveals a much more complex pattern. Here, NPF is initiated in the early morning hours in the surface layer, when temperature (T) is low and relative humidity (RH), sulphur dioxide (SO2) and NH3 concentrations are high, hence new particles are formed in situ. Shortly after that, ex situ NPF in the free troposphere sets in, followed by entrainment and top-down diffusion of newly formed particles into the surface layer. Altogether, these processes mainly contribute to the formation of a strong burst in the morning hours in the ternary scenario. While the time-height cross-section of the binary nucleation rate resembles a "blob"-like evolution pattern, the ternary one resembles a "sucking tube"-like pattern. The time-height cross-sections of the flux pattern and double correlations could be plausibly interpreted in terms of CBL turbulence and entrainment/detrainment processes both in the binary and in the ternary case. Although the present approach is a pure conceptual one, it shows the feasibility to simulate gas-aerosol-turbulence interactions in the CBL. Prior to a dedicated verification/validation study, further attempts are necessary to consider a more advanced description of the formation and activation of thermodynamically stable clusters according to modern concepts proposed by Kulmala et al. (2000), Kulmala (2003) and Kulmala et al. (2004a).
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    Columnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part II: Meteorological characterisation
    (München : European Geopyhsical Union, 2006) Hellmuth, O.
    While in Paper I of four papers a revised columnar high-order modelling approach to investigate gas-aerosol-turbulence interactions in the convective boundary layer (CBL) was deduced, in the present Paper II the model capability to predict the evolution of meteorological CBL parameters is demonstrated. Based on a model setup to simulate typical CBL conditions, predicted first-, second- and third-order moments were shown to agree very well with those obtained from in situ and remote sensing turbulence measurements such as aircraft, SODAR and LIDAR measurements as well as with those derived from ensemble-averaged large eddy simulations and wind tunnel experiments. The results show, that the model is able to predict the meteorological CBL parameters, required to verify or falsify, respectively, previous hypothesis on the interaction between CBL turbulence and new particle formation.
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    The contribution of sulphuric acid to atmospheric particle formation and growth: A comparison between boundary layers in Northern and Central Europe
    (München : European Geopyhsical Union, 2005) Fiedler, V.; Dal Maso, M.; Boy, M.; Aufmhoff, H.; Hoffmann, J.; Schuck, T.; Birmili, W.; Hanke, M.; Uecker, J.; Arnold, F.; Kulmala, M.
    Atmospheric gaseous sulphuric acid was measured and its influence on particle formation and growth was investigated building on aerosol data. The measurements were part of the EU-project QUEST and took place at two different measurement sites in Northern and Central Europe (Hyytiälä, Finland, March-April 2003 and Heidelberg, Germany, March-April 2004). From a comprehensive data set including sulphuric acid, particle number size distributions and meteorological data, particle growth rates, particle formation rates and source rates of condensable vapors were inferred. Growth rates were determined in two different ways, from particle size distributions as well as from a so-called timeshift analysis. Moreover, correlations between sulphuric acid and particle number concentration between 3 and 6 nm were examined and the influence of air masses of different origin was investigated. Measured maximum concentrations of sulphuric acid were in the range from 1x106 to 16x106cm-3. The gaseous sulphuric acid lifetime with respect to condensation on aerosol particles ranged from 2 to 33min in Hyytiälä and from 0.5 to 8 min in Heidelberg. Most calculated values (growth rates, formation rates, vapor source rates) were considerably higher in Central Europe (Heidelberg), due to the more polluted air and higher preexistent aerosol concentrations. Close correlations between H2SO4 and nucleation mode particles (size range: 3-6 nm) were found on most days at both sites. The percentage contribution of sulphuric acid to particle growth was below 10% at both places and to initial growth below 20%. An air mass analysis indicated that at Heidelberg new particles were formed predominantly in air advected from southwesterly directions.
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    Modelling soil dust aerosol in the Bodélé depression during the BoDEx campaign
    (München : European Geopyhsical Union, 2006) Tegen, I.; Heinold, B.; Todd, M.; Helmert, J.; Washington, R.; Dubovik, O.
    We present regional model simulations of the dust emission events during the Bodélé Dust Experiment (BoDEx) that was carried out in February and March 2005 in Chad. A box model version of the dust emission model is used to test different input parameters for the emission model, and to compare the dust emissions computed with observed wind speeds to those calculated with wind speeds from the regional model simulation. While field observations indicate that dust production occurs via self-abrasion of saltating diatomite flakes in the Bodélé, the emission model based on the assumption of dust production by saltation and using observed surface wind speeds as input parameters reproduces observed dust optical thicknesses well. Although the peak wind speeds in the regional model underestimate the highest wind speeds occurring on 10–12 March 2005, the spatio-temporal evolution of the dust cloud can be reasonably well reproduced by this model. Dust aerosol interacts with solar and thermal radiation in the regional model; it is responsible for a decrease in maximum daytime temperatures by about 5 K at the beginning the dust storm on 10 March 2005. This direct radiative effect of dust aerosol accounts for about half of the measured temperature decrease compared to conditions on 8 March. Results from a global dust model suggest that the dust from the Bodélé is an important contributor to dust crossing the African Savannah region towards the Gulf of Guinea and the equatorial Atlantic, where it can contribute up to 40% to the dust optical thickness.
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    CLABAUTAIR: A new algorithm for retrieving three-dimensional cloud structure from airborne microphysical measurements
    (München : European Geopyhsical Union, 2005) Scheirer, R.; Schmidt, S.
    A new algorithm is presented to reproduce the three-dimensional structure of clouds from airborne measurements of microphysical parameters. Data from individual flight legs are scanned for characteristic patterns, and the autocorrelation functions for several directions are used to extrapolate the observations along the flight path to a full three-dimensional distribution of the cloud field. Thereby, the mean measured profiles of microphysical parameters are imposed to the cloud field by mapping the measured probability density functions onto the model layers. The algorithm was tested by simulating flight legs through synthetic clouds (by means of Large Eddy Simulations (LES)) and applied to a stratocumulus cloud case measured during the first field experiment of the EC project INSPECTRO (INfluence of clouds on the SPECtral actinic flux in the lower TROposphere) in East Anglia, UK. The number and position of the flight tracks determine the quality of the retrieved cloud field. If they provide a representative sample of the entire field, the derived pattern closely resembles the statistical properties of the real cloud field.
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    Correlation between traffic density and particle size distribution in a street canyon and the dependence on wind direction
    (München : European Geopyhsical Union, 2006) Voigtländer, J.; Tuch, T.; Birmili, W.; Wiedensohler, A.
    Combustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements also are representative for many other street canyons in Europe. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic counts of 0.5 were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found a maximum of the correlation coefficients for nucleation mode particles in the size range between 10 and 20 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. High correlation coefficients (up to 0.8) could be observed in the lee side of the street canyon for particles in the range between 10 and 100 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons.
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    Atmospheric number size distributions of soot particles and estimation of emission factors
    (München : European Geopyhsical Union, 2006) Rose, D.; Wehner, B.; Ketzel, M.; Engler, C.; Voigtländer, J.; Tuch, T.; Wiedensohler, A.
    Number fractions of externally mixed particles of four different sizes (30, 50, 80, and 150 nm in diameter) were measured using a Volatility Tandem DMA. The system was operated in a street canyon (Eisenbahnstrasse, EI) and at an urban background site (Institute for Tropospheric Research, IfT), both in the city of Leipzig, Germany as well as at a rural site (Melpitz (ME), a village near Leipzig). Intensive campaigns of 3–5 weeks each took place in summer 2003 as well as in winter 2003/04. The data set thus obtained provides mean number fractions of externally mixed soot particles of atmospheric aerosols in differently polluted areas and different seasons (e.g. at 80 nm on working days, 60% (EI), 22% (IfT), and 6% (ME) in summer and 26% (IfT), and 13% (ME) in winter). Furthermore, a new method is used to calculate the size distribution of these externally mixed soot particles from parallel number size distribution measurements. A decrease of the externally mixed soot fraction with decreasing urbanity and a diurnal variation linked to the daily traffic changes demonstrate, that the traffic emissions have a significant impact on the soot fraction in urban areas. This influence becomes less in rural areas, due to atmospheric mixing and transformation processes. For estimating the source strength of soot particles emitted by vehicles (veh), soot particle emission factors were calculated using the Operational Street Pollution Model (OSPM). The emission factor for an average vehicle was found to be (1.5±0.4)·1014 #(km·veh). The separation of the emission factor into passenger cars ((5.8±2)·1013} #(km·veh)) and trucks ((2.5±0.9)·1015 #(km·veh)) yielded in a 40-times higher emission factor for trucks compared to passenger cars.
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    Particle 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.
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    Hygroscopic 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.