bluuebunny/crossref_metadata_2025 huggingface dataset:
Modelling transport and deposition of caesium and iodine from the Chernobyl accident using the DREAM model
Authors: Brandt J. , Christensen J. H. , Frohn L. M.
Published: April 2010

Abstract. A tracer model, DREAM (the Danish Rimpuff and Eulerian Accidental release Model), has been developed for modelling transport, dispersion and deposition (wet and dry) of radioactive material from accidental releases, as the Chernobyl accident. The model is a combination of a Lagrangian model, that includes the near source dispersion, and an Eulerian model describing the long-range transport. The performance of the transport model has previously been tested within the European Tracer Experiment, ETEX, which included transport and dispersion of an inert, non-depositing tracer from a controlled release. The focus of this paper is the model performance with respect to the total deposition of  137Cs, 134Cs and 131I from the Chernobyl accident, using different relatively simple and comprehensive parameterizations for dry- and wet deposition. The performance, compared to measurements, of using different combinations of two different wet deposition parameterizations and three different parameterizations of dry deposition has been evaluated, using different statistical tests. The best model performance, compared to measurements, is obtained when parameterizing the total deposition combined of a simple method for dry deposition and a subgrid-scale averaging scheme for wet deposition based on relative humidities. The same major conclusion is obtained for all the three different radioactive isotopes and using two different deposition measurement databases. Large differences are seen in the results obtained by using the two different parameterizations of wet deposition based on precipitation rates and relative humidities, respectively. The parameterization based on subgrid-scale averaging is, in all cases, performing better than the parameterization based on precipitation rates. This indicates that the in-cloud scavenging process is more important than the below cloud scavenging process for the submicron particles and that the precipitation rates are relatively uncertain in the meteorological model compared to the relative humidity. Relatively small differences are, however, seen in the statistical tests between the three different parameterizations of dry deposition.
Constraining tropospheric mixing timescales using airborne observations and numerical models
Authors: Good P. , Giannakopoulos C. , O’Connor F. M. , Arnold S. R. , de Reus M. , Schlager H.
Published: April 2010

Abstract. A technique is demonstrated for estimating atmospheric mixing time-scales from in-situ data, using a Lagrangian model initialised from an Eulerian chemical transport model (CTM). This method is applied to airborne tropospheric CO observations taken during seven flights of the Mediterranean Intensive Oxidant Study (MINOS) campaign, of August 2001. The time-scales derived, correspond to mixing applied at the spatial scale of the CTM grid. They are relevant to the family of hybrid Lagrangian-Eulerian models, which impose Eulerian grid mixing to an underlying Lagrangian model. The method uses the fact that in Lagrangian tracer transport modelling, the mixing spatial and temporal scales are decoupled: the spatial scale is determined by the resolution of the initial tracer field, and the time scale by the trajectory length. The chaotic nature of lower-atmospheric advection results in the continuous generation of smaller spatial scales, a process terminated in the real atmosphere by mixing. Thus, a mix-down lifetime can be estimated by varying trajectory length so that the model reproduces the observed amount of small-scale tracer structure. Selecting a trajectory length is equivalent to choosing a mixing timescale. For the cases studied, the results are very insensitive to CO photochemical change calculated along the trajectories. That is, it was found that if CO was treated as a passive tracer, this did not affect the mix-down timescales derived, since the slow CO photochemistry does not have much influence at small spatial scales. The results presented correspond to full photochemical calculations. The method is most appropriate for relatively homogeneous regions, i.e. it is not too important to account for changes in aircraft altitude or the positioning of stratospheric intrusions, so that small scale structure is easily distinguished. The chosen flights showed a range of mix-down time upper limits: a very short timescale of 1 day for 8 August, due possibly to recent convection or model error, 3 days for 3 August, probably due to recent convective and boundary layer mixing, and 6-9 days for 16, 17, 22a, 22c and 24 August. These numbers refer to a mixing spatial scale of 2.8°, defined here by the resolution of the Eulerian grid from which tracer fields were interpolated to initialise the Lagrangian model. For the flight of 3 August, the observed concentrations result from a complex set of transport histories, and the models are used to interpret the observed structure, while illustrating where more caution is required with this method of estimating mix-down lifetimes.
Halogen Occultation Experiment (HALOE) and balloon-borne in situ measurements of methane in stratosphere and their relation to the quasi-biennial oscillation (QBO)
Authors: Patra P. K. , Lal S. , Venkataramani S. , Chand D.
Published: April 2010

Abstract. Measurements of methane have been made from various observational platforms in the atmosphere. In this article, we have compared four high precision balloon-borne measurements from Hyderabad (17.5°N), India in the period of 1987 and 1998 with a part of HALOE/UARS global observations available since 1991. All the balloon measurements correspond to boreal spring (March and April) but belong to different years. A comparison shows fairly good agreement with each other. The gradient in CH4 profiles in the troposphere is controlled by the variation in vertical transport. The strongest effect of dynamical influence on methane vertical profiles is shown to be resulting from the dynamical quasi-biennial oscillation in the stratosphere, and that has been consistently derived from both the measurement techniques and chemistry-transport model simulations. It is observed that the QBO signal in CH4 anomaly exhibits interhemispheric asymmetry caused by the tropics to midlatitude circulation in the stratosphere. A mechanism is suggested to explain how and to what extent the methane vertical profiles over Hyderabad and higher latitudes could be modulated by the prevailing QBO winds in the tropics. We have also discussed how the same mechanism would affect ozone distribution in the stratosphere quite differently.
Improving the seasonal cycle and interannual variations of biomass burning aerosol sources
Authors: Generoso S. , Bréon F.-M. , Balkanski Y. , Boucher O. , Schulz M.
Published: April 2010

Abstract. This paper suggests a method for improving current inventories of aerosol emissions from biomass burning. The method is based on the hypothesis that, although the total estimates within large regions are correct, the exact spatial and temporal description can be improved. It makes use of open fire detection from the ATSR instrument that is available since 1996. The emissions inventories are re-distributed in space and time according to the occurrence of open fires. Although the method is based on the night-time hot-spot product of the ATSR, other satellite biomass burning proxies (AVHRR, TRMM, GLOBSCAR and GBA2000) show similar distributions. The impact of the method on the emission inventories is assessed using an aerosol transport model, the results of which are compared to sunphotometer and satellite data. The seasonal cycle of aerosol load in the atmosphere is significantly improved in several regions, in particular South America and Australia. Besides, the use of ATSR fire detection may be used to account for interannual events, as is demonstrated on the large Indonesian fires of 1997, a consequence of the 1997-1998 El Niño. Despite these improvements, there are still some large discrepancies between the simulated and observed aerosol optical thicknesses resulting from biomass burning emissions.
Charging of ice-vapor interfaces: applications to thunderstorms
Authors: Nelson J. , Baker M.
Published: April 2010

Abstract. The build-up of intrinsic Bjerrum and ionic defects at ice-vapor interfaces electrically charges ice surfaces and thus gives rise to many phenomena including thermoelectricity, ferroelectric ice films, sparks from objects in blizzards, electromagnetic emissions accompanying cracking in avalanches, glaciers, and sea ice, and charge transfer during ice-ice collisions in thunderstorms. Fletcher's theory of the ice surface in equilibrium proposed that the Bjerrum defects have a higher rate of creation at the surface than in the bulk, which produces a high concentration of surface D defects that then attract a high concentration of OH- ions at the surface. Here, we add to this theory the effect of a moving interface caused by growth or sublimation. This effect can increase the amount of ionic surface charges more than 10-fold for growth rates near 1 mm s-1 and can extend the spatial separation of interior charges in qualitative agreement with many observations. In addition, ice-ice collisions should generate sufficient pressure to melt ice at the contact region and we argue that the ice particle with the initially sharper point at contact loses more mass of melt than the other particle. A simple analytic model of this process with parameters that are consistent with observations leads to predicted collisional charge exchange that semiquantitatively explains the negative charging region of thunderstorms. The model also has implications for snowflake formation, ferroelectric ice, polarization of ice in snowpacks, and chemical reactions in ice surfaces
A three-dimensional model study of long-term mid-high latitude lower stratosphere ozone changes
Authors: Chipperfield M. P.
Published: April 2010

Abstract. We have used a 3D off-line chemical transport model (CTM) to study the causes of the observed changes in ozone in the mid-high latitude lower stratosphere from 1979-1998. The model was forced by European Centre for Medium Range Weather Forecasts (ECMWF) analyses and contains a detailed chemistry scheme. A series of model runs were performed at a horizontal resolution of 7.5°x7.5° and covered the domain from about 12 km to 30 km. The basic model performs well in reproducing the decadal evolution of the springtime depletion of ozone in the northern hemisphere (NH) and southern hemisphere (SH) high latitudes in the 1980s and early 1990s. After about 1994 the modelled interannual variability does not match the observations as well, which is probably due in part to changes in the operational ECMWF analyses - which places limits on using this dataset to diagnose dynamical trends. For mid-latitudes (35°-60°) the basic model reproduces the observed column ozone decreases from 1980 until the early 1990s. Model experiments show that the halogen trends appear to dominate this modelled decrease and of this around 30-50% is due to high-latitude processing on polar stratospheric clouds (PSCs). Dynamically induced ozone variations in the model correlate with observations over the timescale of a few years. Large discrepancies between the modelled and observed variations in the mid 1980s and mid 1990s can be largely resolved by assuming that the 11-year solar cycle (not explicitly included in the 3D model) causes a 2% (min-max) change in mid-latitude column ozone.
Inorganic bromine in the marine boundary layer: a critical review
Authors: Sander R. , Keene W. C. , Pszenny A. A. P. , Arimoto R. , Ayers G. P. , Baboukas E. , Cainey J. M. , Crutzen P. J. , Duce R. A. , Hönninger G. , Huebert B. J. , Maenhaut W. , Mihalopoulos N. , Turekian V. C. , Van Dingenen R.
Published: April 2010

Abstract. The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is substantially depleted in bromine (often exceeding 50%) relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that the supermicrometer depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. Mechanisms for the submicrometer enrichments are not well understood. Currently available techniques cannot reliably quantify many Br containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans outside the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. The diurnal cycle of gas-phase Br and the corresponding particulate Br deficits are correlated. Higher values of Br in the gas phase during daytime are consistent with expectations based on photochemistry. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.
Hygroscopic properties of different aerosol types over the Atlantic and Indian Oceans
Authors: Maßling A. , Wiedensohler A. , Busch B. , Neusüß C. , Quinn P. , Bates T. , Covert D.
Published: April 2010

Abstract. 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.
Small scale density variations of electrons and charged particles in the vicinity of polar mesosphere summer echoes
Authors: Rapp M. , Lübken F.-J. , Blix T. A.
Published: April 2010

Abstract. We present small scale variations of electron number densities and particle charge number densities measured in situ in the presence of polar mesosphere summer echoes. It turns out that the small scale fluctuations of electrons and negatively charged particles show a strong anticorrelation down to the smallest scales observed. Comparing these small scale structures with the simultaneously measured radar signal to noise profile, we find that the radar profile is well described by the power spectral density of both electrons and charged particles at the radar half wavelength (=the Bragg scale). Finally, we consider the shape of the power spectra of the observed plasma fluctuations and find that both charged particles and electrons show spectra that can be explained in terms of either neutral air turbulence acting on the distribution of a low diffusivity tracer or the fossil remnants of a formerly active turbulent region. All these results are consistent with the theoretical ideas by Rapp and Lübken (2003) suggesting that PMSE can be explained by a combination of active and fossil neutral air turbulence acting on the large and heavy charged aerosol particles which are subsequently mirrored in the electron number density distribution that becomes visible to a VHF radar when small scale fluctuations are present.
Comparison of total ozone from the satellite instruments GOME and TOMS with measurements from the Dobson network 1996–2000
Authors: Bramstedt K. , Gleason J. , Loyola D. , Thomas W. , Bracher A. , Weber M. , Burrows J. P.
Published: April 2010

Abstract. Over the last 3 decades, satellite data have been used to monitor long-term global changes in stratospheric ozone. The TOMS series (1978-present) and GOME (1995-present) are two very important instruments in this context. In this paper, TOMS total ozone and three approaches to derive total ozone from GOME measurements are validated with ground-based Dobson network data. Beyond the operational products of both instruments, e.g. TOMS version 7 and GOME Data Processor version 2.7, total ozone is calculated by integrating FURM ozone profiles and by applying the TOMS algorithm to the GOME spectra. All algorithms show in general good agreement with ground-based measurements. The operational GOME total ozone shows seasonal variations, most likely introduced by difficulties in the derivation of airmass factors, which convert measured slant columns into vertical columns. The TOMS algorithm estimates on average 2% higher total ozone in the southern hemisphere than in the northern for both instruments as compared to the ground-based data, indicating that the source of the observed hemispheric differences is in the TOMS algorithm. Both instruments show aging effects in 2000, leading to enhanced variability in the ozone column differences with respect to Dobson data. In addition, the integrated GOME ozone profiles and the TOMS algorithm applied to GOME data show larger mean deviations in 2000.
Application of the Spectral Structure Parameterization technique: retrieval of total water vapor columns from GOME
Authors: Lang R. , Williams J. E. , van der Zande W. J. , Maurellis A. N.
Published: April 2010

Abstract. We use a recently proposed spectral sampling technique for measurements of atmospheric transmissions called the Spectral Structure Parameterization (SSP) in order to retrieve total water vapor columns (WVC) from reflectivity spectra measured by the Global Ozone Monitoring Experiment (GOME). SSP provides a good compromise between efficiency and speed when performing retrievals on highly structured spectra of narrow-band absorbers like water vapor. We show that SSP can be implemented in a radiative transfer scheme which treats both direct-path absorption and absorption by singly-scattered light directly. For the retrieval we exploit a ro-vibrational overtone band of water vapor located in the visible around 590 nm. We compare our results to independent values given by the data assimilation model of ECMWF. In addition, results are compared to those obtained from the more accurate, but more computationally expensive, Optical Absorption Coefficient Spectroscopy (OACS).
Rarity of upper-tropospheric low O3 mixing ratio events during MOZAIC flights
Authors: Asman W. A. H. , Lawrence M. G. , Brenninkmeijer C. A. M. , Crutzen P. J. , Cuijpers J. W. M. , Nédélec P.
Published: April 2010

Abstract. Only a few previous observations of very low O3 mixing ratios in the upper troposphere are available. The aim of this study was to examine the rich MOZAIC data set for more. Flights with at least 25 4 s averaged mixing ratios less than 8 ppbv at pressures lower than 500 hPa measured using commercial aircraft within the MOZAIC project have been analysed. There are eleven flights that fulfil these conditions (excluding artefacts as discussed below), representing about 0.001% of all measurements during the analysed period August 1994-December 1997. The low O3 events occurred over Southeast Asia, Africa, Brazil and the sea area 200 km east of Florida (US) and were all likely to be associated with transport of air masses from tropical sea areas. These low mixing ratio events occur in the upper troposphere during periods with generally low mixing ratios. They are not only found over sea, but also over land at pressure levels as low as 179 hPa. It could well be that some of the low O3 mixing ratio events measured during two or more flights belong to the same bigger low O3 mixing ratio area.
Hohenpeissenberg Photochemical Experiment (HOPE 2000): Measurements and photostationary state calculations of OH and peroxy radicals
Authors: Handisides G. M. , Plass-Dülmer C. , Gilge S. , Bingemer H. , Berresheim H.
Published: April 2010

Abstract. Measurements of OH, total peroxy radicals, non-methane hydrocarbons (NMHCs) and various other trace gases were made at the Meteorological Observatory Hohenpeissenberg in June 2000. The data from an intensive measurement period characterised by high solar insolation (18-21 June) are analysed. The maximum midday OH concentration ranged between 4.5x106 molecules cm-3 and 7.4x106 molecules cm-3. The maximum total ROx (ROx =OH+RO+HO2+RO2) mixing ratio increased from about 55 pptv on 18 June to nearly 70 pptv on 20 and 21 June. A total of 64 NMHCs, including isoprene and monoterpenes, were measured every 1 to 6 hours. The oxidation rate of the NMHCs by OH was calculated and reached a total of over 14x106 molecules cm-3 s-1 on two days. A simple photostationary state balance model was used to simulate the ambient OH and peroxy radical concentrations with the measured data as input. This approach was able to reproduce the main features of the diurnal profiles of both OH and peroxy radicals. The balance equations were used to test the effect of the assumptions made in this model. The results proved to be most sensitive to assumptions about the impact of unmeasured volatile organic compounds (VOC), e.g. formaldehyde (HCHO), and about the partitioning between HO2 and RO2. The measured OH concentration and peroxy radical mixing ratios were reproduced well by assuming the presence of 3 ppbv HCHO as a proxy for oxygenated hydrocarbons, and a HO2/ RO2 ratio between 1:1 and 1:2. The most important source of OH, and conversely the greatest sink for peroxy radicals, was the recycling of HO2 radicals to OH. This reaction was responsible for the recycling of more than 45x106 molecules cm-3 s-1 on two days. The most important sink for OH, and the largest source of peroxy radicals, was the oxidation of NMHCs, in particular, of isoprene and the monoterpenes.
Evidence of impact of aviation on cirrus cloud formation
Authors: Zerefos C. S. , Eleftheratos K. , Balis D. S. , Zanis P. , Tselioudis G. , Meleti C.
Published: April 2010

Abstract. This work examines changes in cirrus cloud cover (CCC) in possible association with aviation activities at congested air corridors. The analysis is based on the latest version of the International Satellite Cloud Climatology Project D2 data set and covers the period 1984-1998. Over the studied areas, the effect of large-scale modes of natural climate variability such as ENSO, QBO and NAO as well as the possible influence of the tropopause variability, were first removed from the cloud data set in order to calculate long-term changes of observed cirrus cloudiness. The results show increasing trends in (CCC) between 1984 and 1998 over the high air traffic corridors of North America, North Atlantic and Europe. Of these upward trends, only in the summertime over the North Atlantic and only in the wintertime over North America are statistically significant (exceeding +2.0% per decade). Over adjacent locations with low air traffic, the calculated trends are statistically insignificant and in most cases negative both during winter and summer in the regions studied. These negative trends, over low air traffic regions, are consistent with the observed large scale negative trends seen in (CCC) over most of the northern middle latitudes and over the tropics. Moreover, further investigation of vertical velocities over high and low air traffic regions provide evidence that the trends of opposite signs in (CCC) over these regions, do not seem to be caused by different trends in dynamics. It is also shown that the longitudinal distribution of decadal changes in (CCC) along the latitude belt centered at the North Atlantic air corridor, parallels the spatial distribution of fuel consumption from highflying air traffic, providing an independent test of possible impact of aviation on contrail cirrus formation. The correlation between the fuel consumption and the longitudinal variability of (CCC) is significant (+0.7) over the middle latitudes but not over the tropics. This could be explained by the fact that over the tropics the variability of (CCC) is dominated by dynamics while at middle latitudes microphysics explain most of its variability. Results from this study are compared with other studies and for different periods of records and it appears that there exists general agreement as to the evidence of a possible aviation effect on high cloud positive trends over regions with congested air traffic.
Simulating gas-aerosol-cirrus interactions: Process-oriented microphysical model and applications
Authors: Kärcher B.
Published: April 2010

Abstract. This work describes a process-oriented, microphysical-chemical model to simulate the formation and evolution of aerosols and ice crystals under the conditions prevailing in the upper troposphere and lower stratosphere. The model can be run as a box model or along atmospheric trajectories, and considers mixing, gas phase chemistry of aerosol precursors, binary homogeneous aerosol nucleation, homogeneous and heterogeneous ice nucleation, coagulation, condensation and dissolution, gas retention during particle freezing, gas trapping in growing ice crystals, and reverse processes. Chemical equations are solved iteratively using a second order implicit integration method. Gas-particle interactions and coagulation are treated over various size structures, with fully mass conserving and non-iterative numerical solution schemes. Particle types include quinternary aqueous solutions composed of H2SO4, HNO3, HCl, and HBr with and without insoluble components, insoluble aerosol particles, and spherical or columnar ice crystals deriving from each aerosol type separately. Three case studies are discussed in detail to demonstrate the potential of the model to simulate real atmospheric processes and to highlight current research topics concerning aerosol and cirrus formation near the tropopause. Emphasis is placed on how the formation of cirrus clouds and the scavenging of nitric acid in cirrus depends on small-scale temperature fluctuations and the presence of efficient ice nuclei in the tropopause region, corroborating and partly extending the findings of previous studies.
The North Atlantic Oscillation controls air pollution transport to the Arctic
Authors: Eckhardt S. , Stohl A. , Beirle S. , Spichtinger N. , James P. , Forster C. , Junker C. , Wagner T. , Platt U. , Jennings S. G.
Published: April 2010

Abstract. This paper studies the interannual variability of pollution pathways from northern hemisphere (NH) continents into the Arctic. Using a 15-year model simulation of the dispersion of passive tracers representative of anthropogenic emissions from NH continents, we show that the North Atlantic Oscillation (NAO) exerts a strong control on the pollution transport into the Arctic, particularly in winter and spring. For tracer lifetimes of 5 (30) days, surface concentrations in the Arctic winter are enhanced by about 70% (30%) during high phases of the NAO (in the following referred to as NAO+) compared to its low phases (NAO-). This is mainly due to great differences in the pathways of European pollution during NAO+ and NAO- phases, respectively, but reinforced by North American pollution, which is also enhanced in the Arctic during NAO+ phases. In contrast, Asian pollution in the Arctic does not significantly depend on the NAO phase. The model results are confirmed using remotely-sensed NO2 vertical atmospheric columns obtained from seven years of satellite measurements, which show enhanced northward NO2 transport and reduced NO2 outflow into the North Atlantic from Central Europe during NAO+ phases. Surface measurements of carbon monoxide (CO) and black carbon at high-latitude stations further corroborate the overall picture of enhanced Arctic pollution levels during NAO+ phases
Experimental investigation of homogeneous freezing of sulphuric acid particles in the aerosol chamber AIDA
Authors: Möhler O. , Stetzer O. , Schaefers S. , Linke C. , Schnaiter M. , Tiede R. , Saathoff H. , Krämer M. , Mangold A. , Budz P. , Zink P. , Schreiner J. , Mauersberger K. , Haag W. , Kärcher B. , Schurath U.
Published: April 2010

Abstract. The homogeneous freezing of supercooled H2SO4/H2O solution droplets was investigated in the aerosol chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) of Forschungszentrum Karlsruhe. 24 freezing experiments were performed at temperatures between 189 and 235 K with aerosol particles in the diameter range 0.05 to 1 µm. Individual experiments started at homogeneous temperatures and ice saturation ratios between 0.9 and 0.95. Cloud cooling rates up to -2.8 K min-1 were simulated dynamically in the chamber by expansion cooling using a mechanical pump. Depending on the cooling rate and starting temperature, freezing threshold relative humidities were exceeded after expansion time periods between about 1 and 10 min. The onset of ice formation was measured with three independent methods showing good agreement among each other. Ice saturation ratios measured at the onset of ice formation increased from about 1.4 at 231 K  to about 1.75 at 189 K. The experimental data set including thermodynamic parameters as well as physical and chemical aerosol analysis provides a good basis for microphysical model applications.
Particle formation at a continental background site: comparison of model results with observations
Authors: Uhrner U. , Birmili W. , Stratmann F. , Wilck M. , Ackermann I. J. , Berresheim H.
Published: April 2010

Abstract. 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.
Factors controlling Arctic denitrification in cold winters of the 1990s
Authors: Mann G.W. , Davies S. , Carslaw K. S. , Chipperfield M. P.
Published: April 2010

Abstract. Denitrification of the Arctic winter stratosphere has been calculated using a 3-D microphysical model for the winters 1994/95, 1995/96, 1996/97 and 1999/2000. Denitrification is assumed to occur through the sedimentation of low number concentrations of large nitric acid trihydrate (NAT) particles (as inferred by e.g. Fahey et al., 2001). We examine whether the meteorological conditions that allowed particles to grow to the very large sizes observed in 1999/2000 also occurred in the other cold winters. The results show that winter 1999/2000 had conditions that were optimum for denitrification by large NAT particles, which are a deep concentric NAT area and vortex. Under these conditions, NAT particles can circulate in the NAT-supersaturated air for several days, reaching several micrometres in radius and leading to a high downward flux of nitric acid. The other winters had shorter periods with optimum conditions for denitrification. However, we find that NAT particles could have grown to large sizes in all of these winters and could have caused significant denitrification. We define the quantity "closed-flow area'' (the fraction of the NAT area in which air parcel trajectories can form closed loops) and show that it is a very useful indicator of possible denitrification. We find that even with a constant NAT nucleation rate throughout the NAT area, the average NAT number concentration and size can vary by up to a factor of 10 in response to this meteorological quantity. These changes in particle properties account for a high degree of variability in denitrification between the different winters. This large meteorologically induced variability in denitrification rate needs to be compared with that which could arise from a variable nucleation rate of NAT particles, which remains an uncertain quantity in models. Sensitivity studies show that although denitrification was likely approaching asymptotic minimum values throughout much of the 1999/2000 vortex, decreases in the volume-averaged nucleation rate would have substantially reduced the denitrification.
Atmospheric impact of the 1783–1784 Laki eruption: Part I Chemistry modelling
Authors: Stevenson D. S. , Johnson C. E. , Highwood E. J. , Gauci V. , Collins W. J. , Derwent R. G.
Published: April 2010

Abstract. Results from the first chemistry-transport model study of the impact of the 1783–1784 Laki fissure eruption (Iceland: 64°N, 17°W) upon atmospheric composition are presented. The eruption released an estimated 61 Tg(S) as SO2 into the troposphere and lower stratosphere. The model has a high resolution tropopause region, and detailed sulphur chemistry. The simulated SO2 plume spreads over much of the Northern Hemisphere, polewards of ~40°N. About 70% of the SO2 gas is directly deposited to the surface before it can be oxidised to sulphuric acid aerosol. The main SO2 oxidants, OH and H2O2, are depleted by up to 40% zonally, and the lifetime of SO2 consequently increases. Zonally averaged tropospheric SO2 concentrations over the first three months of the eruption exceed 20 ppbv, and sulphuric acid aerosol reaches ~2 ppbv. These compare to modelled pre-industrial/present-day values of 0.1/0.5 ppbv SO2 and 0.1/1.0 ppbv sulphate. A total sulphuric acid aerosol yield of 17–22 Tg(S) is produced. The mean aerosol lifetime is 6–10 days, and the peak aerosol loading of the atmosphere is 1.4–1.7 Tg(S) (equivalent to 5.9–7.1 Tg of hydrated sulphuric acid aerosol). These compare to modelled pre-industrial/present-day sulphate burdens of 0.28/0.81 Tg(S), and lifetimes of 6/5 days, respectively. Due to the relatively short atmospheric residence times of both SO2 and sulphate, the aerosol loading approximately mirrors the temporal evolution of emissions associated with the eruption. The model produces a reason-able simulation of the acid deposition found in Greenland ice cores. These results appear to be relatively insensitive to the vertical profile of emissions assumed, although if more of the emissions reached higher levels (>12 km), this would give longer lifetimes and larger aerosol yields. Introducing the emissions in episodes generates similar results to using monthly mean emissions, because the atmospheric lifetimes are similar to the repose periods between episodes. Most previous estimates of the global aerosol loading associated with Laki did not use atmospheric models; this study suggests that these earlier estimates have been generally too large in magnitude, and too long-lived. Environmental effects following the Laki eruption may have been dominated by the widespread deposition of SO2 gas rather than sulphuric acid aerosol.
On the formation of radiation fogs under heavily polluted conditions
Authors: Kokkola H. , Romakkaniemi S. , Laaksonen A.
Published: April 2010

Abstract. We have studied the effect of gaseous pollutants on fog droplet growth in heavily polluted air using a model that describes time-dependent sulfate production in the liquid phase and thermodynamical equilibrium between the droplets and the gas phase. Our research indicates that the oxidation of SO2 to sulfate has a significant effect on fog droplet growth especially when hygroscopic trace gases, for example HNO3 and NH3 are present. The increased sulfate production by dissolution of hygroscopic gases results from increased pH (caused by absorption of ammonia) and from the increased size of the fog/smog droplets. Our results indicate that unactivated fogs may become optically very thick when the droplet concentrations are on the order of several thousand per cubic centimeter of air.
Mass closure on the chemical species in size-segregated atmospheric aerosol collected in an urban area of the Po Valley, Italy
Authors: Matta E. , Facchini M. C. , Decesari S. , Mircea M. , Cavalli F. , Fuzzi S. , Putaud J.-P. , Dell’Acqua A.
Published: April 2010

Abstract. A complete size segregated chemical characterisation was carried out for aerosol samples collected in the urban area of Bologna over a period of one year, using five-stage low pressure Berner impactors. An original dual-substrate technique was adopted to obtain samples suitable for a complete chemical characterisation. Total mass, inorganic, and organic components were analysed as a function of size, and a detailed characterisation of the water soluble organic compounds was also performed by means of a previously developed methodology, based on HPLC separation of organic compounds according to their acid character and functional group analysis by Proton Nuclear Magnetic Resonance. Chemical mass closure of the collected samples was reached to within a few percent on average in the submicron aerosol range, while a higher unknown fraction in the coarse aerosol range was attributed to soil-derived species not analysed in this experiment. Comparison of the functional group analysis results with model results simulating water soluble organic compound production by gas-to-particle conversion of anthropogenic VOCs showed that this pathway provides a minor contribution to the organic composition of the aerosol samples in the urban area of Bologna.
OH in the coastal boundary layer of Crete during MINOS: Measurements and relationship with ozone photolysis
Authors: Berresheim H. , Plass-Dülmer C. , Elste T. , Mihalopoulos N. , Rohrer F.
Published: April 2010

Abstract. Hydroxyl radical (OH) concentrations were measured in August 2001 at Finokalia Station on the northeastern coast of Crete during the Mediterranean Intensive Oxidant Study (MINOS). OH was measured based on selected ion chemical ionization mass spectrometry (SI/CIMS) with a time resolution of 30 sec and signal integration of 5 min. The corresponding accuracy, precision, and detection limit were 20% (1σ), 11% (1σ), and 2.4 x 105 molecules cm-3 (2σ), respectively. OH levels showed a strong diurnal variability with high maxima (approximately 2 x 107 molecules cm-3) occurring around 13:30 LT (10:30 UTC) and nighttime values below the detection limit. Daily 24-hour average concentrations varied between 3.6-6.7 x 106 cm-3. For the total measurement period (6-21 August) the mean and standard deviation were 4.5 ± 1.1 x 106 cm-3. The OH data set is analyzed based on a classification into three periods: I: Aug 6-8, II: Aug 9-11, III: Aug 13-18. For each of the three periods the measured OH concentrations are described by the empirical function [OH] = a J(O1D)b, with J(O1D) being the ozone photolysis frequency and a = 1.4 x 1010 s cm-3, 1.7 x 1010 s cm-3, 2.2 x 1010 s cm-3, and b = 0.68, respectively. Taking into account the estimated precision of the OH measurements this empirical function using three values for a and one value for b explains 99% of the observed variance of OH. A detailed sensitivity analysis using a CH4-CO box model was performed to interpret this relationship, in particular the meanings of the pre-exponential factor a and the exponent b. It was found that the value of b which represents the total logarithmic dependence of [OH] on J(O1D) includes the individual contributions from the photolysis of O3, NO2, HCHO, HONO, and H2O2 which could be determined using the box model. For the conditions prevailing during the MINOS campaign the exponent b was found to be dominated by the contributions from O3- and NO2-photolysis. For the individual functional dependences between [OH] and J(O1D), [OH] and J(NO2), and J(NO2) and J(O1D) the partial logarithmic derivatives were determined to be 0.5, 0.6, and 0.3, respectively. Overall, the box model yields a value of 0.70 for the exponent b in very good agreement with the corresponding value derived from the empirical analysis of the measurements. This empirical approach in which the chemical air mass characteristics influencing the OH radical balance and thereby, the self-cleansing efficiency of the atmosphere, are represented by only two parameters which are constant over quite substantial time periods may be used in future experiments to test and compare OH measurements made in different atmospheric environments.
Ground-based intercomparison of two isoprene measurement techniques
Authors: Leibrock E. , Huey L. G. , Goldan P. D. , Kuster W. C. , Williams E. , Fehsenfeld F. C.
Published: April 2010

Abstract. An informal intercomparison of two isoprene (C5H8) measurement techniques was carried out during Fall of 1998 at a field site located approximately 3 km west of Boulder, Colorado, USA. A new chemical ionization mass spectrometric technique (CIMS) was compared to a well-established gas chromatographic technique (GC). The CIMS technique utilized benzene cation chemistry to ionize isoprene. The isoprene levels measured by the CIMS were often larger than those obtained with the GC. The results indicate that the CIMS technique suffered from an anthropogenic interference associated with air masses from the Denver, CO metropolitan area as well as an additional interference occurring in clean conditions. However, the CIMS technique is also demonstrated to be sensitive and fast. Especially after introduction of a tandem mass spectrometric technique, it is therefore a candidate for isoprene measurements in remote environments near isoprene sources.
Detailed modeling of mountain wave PSCs
Authors: Fueglistaler S. , Buss S. , Luo B. P. , Wernli H. , Flentje H. , Hostetler C. A. , Poole L. R. , Carslaw K. S. , Peter Th.
Published: April 2010

Abstract. Polar stratospheric clouds (PSCs) play a key role in polar ozone depletion. In the Arctic, PSCs can occur on the mesoscale due to orographically induced gravity waves. Here we present a detailed study of a mountain wave PSC event on 25-27 January 2000 over Scandinavia. The mountain wave PSCs were intensively observed by in-situ and remote-sensing techniques during the second phase of the SOLVE/THESEO-2000 Arctic campaign. We use these excellent data of PSC observations on 3 successive days to analyze the PSCs and to perform a detailed comparison with modeled clouds. We simulated the 3-dimensional PSC structure on all 3 days with a mesoscale numerical weather prediction (NWP) model and a microphysical box model (using best available nucleation rates for ice and nitric acid trihydrate particles). We show that the combined mesoscale/microphysical model is capable of reproducing the PSC measurements within the uncertainty of data interpretation with respect to spatial dimensions, temporal development and microphysical properties, without manipulating temperatures or using other tuning parameters. In contrast, microphysical modeling based upon coarser scale global NWP data, e.g. current ECMWF analysis data, cannot reproduce observations, in particular the occurrence of ice and nitric acid trihydrate clouds. Combined mesoscale/microphysical modeling may be used for detailed a posteriori PSC analysis and for future Arctic campaign flight and mission planning. The fact that remote sensing alone cannot further constrain model results due to uncertainities in the interpretation of measurements, underlines the need for synchronous in-situ PSC observations in campaigns.