bluuebunny/crossref_metadata_2025 huggingface dataset:
Interannual variability in global biomass burning emissions from 1997 to 2004
Authors: van der Werf G. R. , Randerson J. T. , Giglio L. , Collatz G. J. , Kasibhatla P. S. , Arellano A. F.
Published: April 2010

Abstract. Biomass burning represents an important source of atmospheric aerosols and greenhouse gases, yet little is known about its interannual variability or the underlying mechanisms regulating this variability at continental to global scales. Here we investigated fire emissions during the 8 year period from 1997 to 2004 using satellite data and the CASA biogeochemical model. Burned area from 2001–2004 was derived using newly available active fire and 500 m. burned area datasets from MODIS following the approach described by Giglio et al. (2006). ATSR and VIRS satellite data were used to extend the burned area time series back in time through 1997. In our analysis we estimated fuel loads, including organic soil layer and peatland fuels, and the net flux from terrestrial ecosystems as the balance between net primary production (NPP), heterotrophic respiration (Rh), and biomass burning, using time varying inputs of precipitation (PPT), temperature, solar radiation, and satellite-derived fractional absorbed photosynthetically active radiation (fAPAR). For the 1997–2004 period, we found that on average approximately 58 Pg C year−1 was fixed by plants as NPP, and approximately 95% of this was returned back to the atmosphere via Rh. Another 4%, or 2.5 Pg C year−1 was emitted by biomass burning; the remainder consisted of losses from fuel wood collection and subsequent burning. At a global scale, burned area and total fire emissions were largely decoupled from year to year. Total carbon emissions tracked burning in forested areas (including deforestation fires in the tropics), whereas burned area was largely controlled by savanna fires that responded to different environmental and human factors. Biomass burning emissions showed large interannual variability with a range of more than 1 Pg C year−1, with a maximum in 1998 (3.2 Pg C year−1) and a minimum in 2000 (2.0 Pg C year−1).
Interannual variation patterns of total ozone and lower stratospheric temperature in observations and model simulations
Authors: Steinbrecht W. , Haßler B. , Brühl C. , Dameris M. , Giorgetta M. A. , Grewe V. , Manzini E. , Matthes S. , Schnadt C. , Steil B. , Winkler P.
Published: April 2010

Abstract. We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2000, by TOMS/SBUV), of temperature reanalyses (1958 to 2000, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa (≈80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa (≈30 km). It is targeted on processes near the tropopause, and has more levels in this region. Despite some problems, both models generally reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability in total ozone and lower stratospheric temperature. In most aspects MAECHAM4-CHEM performs slightly better than E39/C. MAECHAM4-CHEM overestimates the long-term decline of total ozone, whereas underestimates the decline over Antarctica and at northern mid-latitudes. The true long-term decline in winter and spring above the Arctic may be underestimated by a lack of TOMS/SBUV observations in winter, particularly in the cold 1990s. Main contributions to the observed interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to -10 DU/decade at high northern latitudes, up to -40 DU/decade at high southern latitudes, and around -0.7 K/decade over much of the globe), from the intensity of the polar vortices (more than 40 DU, or 8 K peak to peak), the QBO (up to 20 DU, or 2 K peak to peak), and from tropospheric weather (up to 20 DU, or 2 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 15 DU, or 1 K), or to ENSO (up to 10 DU, or 1 K). These observed variations are replicated well in the simulations. Volcanic eruptions have resulted in sporadic changes (up to -30 DU, or +3 K). At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high-latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO.
The initial dispersal and radiative forcing of a Northern Hemisphere mid-latitude super volcano: a model study
Authors: Timmreck C. , Graf H.-F.
Published: April 2010

Abstract. The chemistry climate model MAECHAM4/ CHEM with interactive and prognostic volcanic aerosol and ozone was used to study the initial dispersal and radiative forcing of a possible Northern Hemisphere mid-latitude super eruption. Tropospheric climate anomalies are not analysed since sea surface temperatures are kept fixed. Our experiments show that the global dispersal of a super eruption located at Yellowstone, Wy. is strongly dependent on the season of the eruption. In Northern Hemisphere summer the volcanic cloud is transported westward and preferentially southward, while in Northern Hemisphere winter the cloud is transported eastward and more northward compared to the summer case. Aerosol induced heating leads to a more global spreading with a pronounced cross equatorial transport. For a summer eruption aerosol is transported much further to the Southern Hemisphere than for a winter eruption. In contrast to Pinatubo case studies, strong cooling tendencies appear with maximum peak values of less than −1.6 K/day three months after the eruption in the upper tropical stratosphere. This strong cooling effect weakens with decreasing aerosol density over time and initially prevents the aerosol laden air from further active rising. All-sky net radiative flux changes of less than −32 W/m2 at the surface are about a factor of 6 larger than for the Pinatubo eruption. Large positive flux anomalies of more than 16 W/m2 are found in the first months in the tropics and sub tropics. These strong forcings call for a fully coupled ocean/atmosphere/chemistry model to study climate sensitivity to such a super-eruption.
Optical properties of humic-like substances (HULIS) in biomass-burning aerosols
Authors: Hoffer A. , Gelencsér A. , Guyon P. , Kiss G. , Schmid O. , Frank G. P. , Artaxo P. , Andreae M. O.
Published: April 2010

Abstract. We present here the optical properties of humic-like substances (HULIS) isolated from the fine fraction of biomass-burning aerosol collected in the Amazon basin during the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia – SMOke aerosols, Clouds, rainfall and Climate) experiment in September 2002. From the isolated HULIS, aerosol particles were generated and their scattering and absorption coefficients measured. The size distribution and mass of the particles were also recorded. The value of the index of refraction was derived from "closure" calculations based on particle size, scattering and absorption measurements. On average, the complex index of refraction at 532 nm of HULIS collected during day and nighttime was 1.65–0.0019i and 1.69–0.0016i, respectively. In addition, the imaginary part of the complex index of refraction was calculated using the measured absorption coefficient of the bulk HULIS. The mass absorption coefficient of the HULIS at 532 nm was found to be quite low (0.031 and 0.029 m2 g−1 for the day and night samples, respectively). However, due to the high absorption Ångström exponent (6–7) of HULIS, the specific absorption increases substantially towards shorter wavelengths (~2–3 m2 g−1 at 300 nm), causing a relatively high (up to 50%) contribution to the light absorption of our Amazonian aerosol at 300 nm. For the relative contribution of HULIS to light absorption in the entire solar spectrum, lower values (6.4–8.6%) are obtained, but those are still not negligible.
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species
Authors: Atkinson R. , Baulch D. L. , Cox R. A. , Crowley J. N. , Hampson R. F. , Hynes R. G. , Jenkin M. E. , Rossi M. J. , Troe J. ,   IUPAC Subcommittee
Published: April 2010

Abstract. This article, the second in the series, presents kinetic and photochemical data evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of Organic species, which were last published in 1999, and were updated on the IUPAC website in late 2002, and subsequently during the preparation of this article. The article consists of a summary table of the recommended rate coefficients, containing the recommended kinetic parameters for the evaluated reactions, and eight appendices containing the data sheets, which provide information upon which the recommendations are made.
Search for evidence of trend slow-down in the long-term TOMS/SBUV total ozone data record: the importance of instrument drift uncertainty
Authors: Stolarski R. S. , Frith S. M.
Published: April 2010

Abstract. We have developed a merged ozone data set (MOD) for the period October 1978 through June 2006 combining total ozone measurements (Version 8 retrieval) from the TOMS (Nimbus 7, Earth Probe) and SBUV/SBUV2 (Nimbus 7, NOAA 9/11/16) series of satellite instruments. We use the MOD data set to search for evidence of ozone recovery in response to the observed leveling off of chlorine and bromine compounds in the stratosphere. A crucial step in any time series analysis is the evaluation of uncertainties. In addition to the standard statistical time series uncertainties, we evaluate the possible instrument drift uncertainty for the MOD data set. We combine these two sources of uncertainty and apply them to a cumulative sum of residuals (CUSUM) analysis for trend slow-down. For the extra-polar mean between 60° S and 60° N, the apparent slow-down in trend is found to be clearly significant if instrument uncertainties are ignored. When instrument uncertainties are added, the slow-down becomes marginally significant at the 2σ level. For the mid-latitudes of the northern hemisphere (30° to 60° N) the trend slow-down is highly significant at the 2σ level, while in the southern hemisphere the trend slow-down has yet to meet the 2σ significance criterion. The rate of change of chlorine/bromine compounds is similar in both hemispheres, and we expect the ozone response to be similar in both hemispheres as well. The asymmetry in the trend slow-down between hemispheres likely reflects the influence of dynamical variability, and thus a clearly statistically significant response of total ozone to the leveling off of chlorine and bromine in the stratosphere is not yet indicated.
Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms
Authors: Sihto S.-L. , Kulmala M. , Kerminen V.-M. , Dal Maso M. , Petäjä T. , Riipinen I. , Korhonen H. , Arnold F. , Janson R. , Boy M. , Laaksonen A. , Lehtinen K. E. J.
Published: April 2010

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.
Observations of lunar tides in the mesosphere and lower thermosphere at Arctic and middle latitudes
Authors: Sandford D. J. , Muller H. G. , Mitchell N. J.
Published: April 2010

Abstract. Meteor radars have been used to measure the horizontal winds in the mesosphere and lower thermosphere over Castle Eaton (52° N) in the UK and over Esrange (68° N) in Arctic Sweden. We consider a 16-year data set covering the interval 1988–2004 for the UK and a 6-year data set covering the interval 1999–2005 for the Arctic. The signature of the 12.42-h (M2) lunar tide has been identified at both locations. The lunar tide is observed to reach amplitudes as large as 11 ms−1. The Arctic radar has an interferometer and so allows investigation of the vertical structure of the lunar tide. At both locations the tide has maximum amplitudes in winter with a second autumnal maximum. The amplitude is found to increase with height over the 80–100 km height range observed. Vertical wavelengths are very variable, ranging from about 15 km in summer to more than 60 km in winter. Comparisons with the Vial and Forbes (1994) model reveals generally good agreement, except in the case of the summer vertical wavelengths which are observed to be significantly shorter than predicted.
Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part II: Meteorological characterisation
Authors: Hellmuth O.
Published: April 2010

Abstract. 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.
The sensitivity of aerosol in Europe to two different emission inventories and temporal distribution of emissions
Authors: de Meij A. , Krol M. , Dentener F. , Vignati E. , Cuvelier C. , Thunis P.
Published: April 2010

Abstract. The sensitivity to two different emission inventories, injection altitude and temporal variations of anthropogenic emissions in aerosol modelling is studied, using the two way nested global transport chemistry model TM5 focussing on Europe in June and December 2000. The simulations of gas and aerosol concentrations and aerosol optical depth (AOD) with the EMEP and AEROCOM emission inventories are compared with EMEP gas and aerosol surface based measurements, AERONET sun photometers retrievals and MODIS satellite data. For the aerosol precursor gases SO2 and NOx in both months the model results calculated with the EMEP inventory agree better (overestimated by a factor 1.3 for both SO2 and NOx) with the EMEP measurements than the simulation with the AEROCOM inventory (overestimated by a factor 2.4 and 1.9, respectively). Besides the differences in total emissions between the two inventories, an important role is also played by the vertical distribution of SO2 and NOx emissions in understanding the differences between the EMEP and AEROCOM inventories. In December NOx and SO2 from both simulations agree within 50% with observations. In June SO4= evaluated with the EMEP emission inventory agrees slightly better with surface observations than the AEROCOM simulation, whereas in December the use of both inventories results in an underestimate of SO4 with a factor 2. Nitrate aerosol measured in summer is not reliable, however in December nitrate aerosol calculations with the EMEP and AEROCOM emissions agree with 30%, and 60%, respectively with the filter measurements. Differences are caused by the total emissions and the temporal distribution of the aerosol precursor gases NOx and NH3. Despite these differences, we show that the column integrated AOD is less sensitive to the underlying emission inventories. Calculated AOD values with both emission inventories underestimate the observed AERONET AOD values by 20–30%, whereas a case study using MODIS data shows a high spatial agreement. Our evaluation of the role of temporal distribution of anthropogenic emissions on aerosol calculations shows that the daily and weekly temporal distributions of the emissions are only important for NOx, NH3 and aerosol nitrate. However, for all aerosol species SO4=, NH4+, POM, BC, as well as for AOD, the seasonal temporal variations used in the emission inventory are important. Our study shows the value of including at least seasonal information on anthropogenic emissions, although from a comparison with a range of measurements it is often difficult to firmly identify the superiority of specific emission inventories, since other modelling uncertainties, e.g. related to transport, aerosol removal, water uptake, and model resolution, play a dominant role.
Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom
Authors: Dentener F. , Kinne S. , Bond T. , Boucher O. , Cofala J. , Generoso S. , Ginoux P. , Gong S. , Hoelzemann J. J. , Ito A. , Marelli L. , Penner J. E. , Putaud J.-P. , Textor C. , Schulz M. , van der Werf G. R. , Wilson J.
Published: April 2010

Abstract. Inventories for global aerosol and aerosol precursor emissions have been collected (based on published inventories and published simulations), assessed and prepared for the year 2000 (present-day conditions) and for the year 1750 (pre-industrial conditions). These global datasets establish a comprehensive source for emission input to global modeling, when simulating the aerosol impact on climate with state-of-the-art aerosol component modules. As these modules stratify aerosol into dust, sea-salt, sulfate, organic matter and soot, for all these aerosol types global fields on emission strength and recommendations for injection altitude and particulate size are provided. Temporal resolution varies between daily (dust and sea-salt), monthly (wild-land fires) and annual (all other emissions). These datasets benchmark aerosol emissions according to the knowledge in the year 2004. They are intended to serve as systematic constraints in sensitivity studies of the AeroCom initiative, which seeks to quantify (actual) uncertainties in aerosol global modeling.
Boundary layer structure and decoupling from synoptic scale flow during NAMBLEX
Authors: Norton E. G. , Vaughan G. , Methven J. , Coe H. , Brooks B. , Gallagher M. , Longley I.
Published: April 2010

Abstract. This paper presents an overview of the meteorology and planetary boundary layer structure observed during the NAMBLEX field campaign to aid interpretation of the chemical and aerosol measurements. The campaign has been separated into five periods corresponding to the prevailing synoptic condition. Comparisons between meteorological measurements (UHF wind profiler, Doppler sodar, sonic aneometers mounted on a tower at varying heights and a standard anemometer) and the ECMWF analysis at 10m and 1100 m identified days when the internal boundary layer was decoupled from the synoptic flow aloft. Generally the agreement was remarkably good apart from during period one and on a few days during period four when the diurnal swing in wind direction implies a sea/land breeze circulation near the surface. During these periods the origin of air sampled at Mace Head would not be accurately represented by back trajectories following the winds resolved in ECMWF analyses. The wind profiler observations give a detailed record of boundary layer structure including an indication of its depth, average wind speed and direction. Turbulence statistics have been used to assess the height to which the developing internal boundary layer, caused by the increased surface drag at the coast, reaches the sampling location under a wide range of marine conditions. Sampling conducted below 10 m will be impacted by emission sources at the shoreline in all wind directions and tidal conditions, whereas sampling above 15 m is unlikely to be affected in any of the wind directions and tidal heights sampled during the experiment.
Modelling soil dust aerosol in the Bodélé depression during the BoDEx campaign
Authors: Tegen I. , Heinold B. , Todd M. , Helmert J. , Washington R. , Dubovik O.
Published: April 2010

Abstract. 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.
Direct measurement of particle formation and growth from the oxidation of biogenic emissions
Authors: VanReken T. M. , Greenberg J. P. , Harley P. C. , Guenther A. B. , Smith J. N.
Published: April 2010

Abstract. A new facility has been developed to investigate the formation of new particles from the oxidation of volatile organic compounds emitted from vegetation. The facility consists of a biogenic emissions enclosure, an aerosol growth chamber, and the associated instrumentation. Using the facility, new particle formation events have been induced through the reaction of ozone with three different precursor gas mixtures: an α-pinene test mixture and the emissions of a Holm oak (Quercus ilex) specimen and a loblolly pine (Pinus taeda) specimen. The results demonstrate the variability between species in their potential to form new aerosol products. The emissions of Q. ilex specimen resulted in fewer particles than did α-pinene, although the concentration of monoterpenes was roughly equal in both experiments before the addition of ozone. Conversely, the oxidation of P. taeda specimen emissions led to the formation of more particles than either of the other two gas mixtures, despite a lower initial terpenoid concentration. These variations can be attributed to differences in the speciation of the vegetative emissions with respect to the α-pinene mixture and to each other. Specifically, the presence of β-pinene and other slower-reacting monoterpenes probably inhibited particle formation in the Q. ilex experiment, while the presence of sesquiterpenes, including β-caryophyllene, in the emissions of the P. taeda specimen were the likely cause of the more intense particle formation events observed during that experiment.
Distribution of meteoric smoke – sensitivity to microphysical properties and atmospheric conditions
Authors: Megner L. , Rapp M. , Gumbel J.
Published: April 2010

Abstract. Meteoroids entering the Earth's atmosphere experience strong deceleration and ablate, whereupon the resulting material is believed to re-condense to nanometre-size "smoke particles". These particles are thought to be of great importance for many middle atmosphere phenomena, such as noctilucent clouds, polar mesospheric summer echoes, metal layers, and heterogeneous chemistry. The properties and distribution of meteoric smoke depend on poorly known or highly variable factors such as the amount, composition and velocity of incoming meteoric material, the efficiency of coagulation, and the state and circulation of the atmosphere. This work uses a one-dimensional microphysical model to investigate the sensitivities of meteoric smoke properties to these poorly known or highly variable factors. The resulting uncertainty or variability of meteoric smoke quantities such as number density, mass density, and size distribution are determined. It is found that the two most important factors are the efficiency of the coagulation and background vertical wind. The seasonal variation of the vertical wind in the mesosphere implies strong global and temporal variations in the meteoric smoke distribution. This contrasts the simplistic picture of a homogeneous global meteoric smoke layer, which is currently assumed in many studies of middle atmospheric phenomena. In particular, our results suggest a very low number of nanometre-sized smoke particles at the summer mesopause where they are thought to serve as condensation nuclei for noctilucent clouds.
MALTE – model to predict new aerosol formation in the lower troposphere
Authors: Boy M. , Hellmuth O. , Korhonen H. , Nilsson E. D. , ReVelle D. , Turnipseed A. , Arnold F. , Kulmala M.
Published: April 2010

Abstract. 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.
Separation of emitted and photochemical formaldehyde in Mexico City using a statistical analysis and a new pair of gas-phase tracers
Authors: Garcia A. R. , Volkamer R. , Molina L. T. , Molina M. J. , Samuelson J. , Mellqvist J. , Galle B. , Herndon S. C. , Kolb C. E.
Published: April 2010

Abstract. Photochemical pollution control strategies require an understanding of photochemical oxidation precursors, making it important to distinguish between primary and secondary sources of HCHO. Estimates for the relative strengths of primary and secondary sources of formaldehyde (HCHO) were obtained using a statistical regression analysis with time series data of carbon monoxide (CO) and glyoxal (CHOCHO) measured in the Mexico City Metropolitan Area (MCMA) during the spring of 2003. Differences between Easter week and more typical weeks are evaluated. The use of CO-CHOCHO as HCHO tracers is more suitable for differentiating primary and secondary sources than CO-O3. The application of the CO-O3 tracer pair to mobile laboratory data suggests a potential in-city source of background HCHO. A significant amount of HCHO observed in the MCMA is associated with primary emissions.
Mesoscale temperature fluctuations in the stratosphere
Authors: Gary B. L.
Published: April 2010

Abstract. An airborne instrument that measures altitude temperature profiles is ideally suited for the task of characterizing statistical properties of the vertical displacement of isentrope surfaces. Prior measurements of temperature fluctuations during level flight could not be used to infer isentrope altitude variations because lapse rate information was missing. The Microwave Temperature Profiler instrument, which includes lapse rate measurements at flight level as a part of temperature profiles, has been used on hundreds of flights to produce altitude versus ground track cross-sections of potential temperature. These cross-sections show isentrope altitude variations with a horizontal resolution of ~3 km for a >6 km altitude region. An airborne isentrope-altitude cross-section (IAC) can be compared with a counterpart IAC generated from synoptic scale data, based on radiosondes and satellite instruments, in order to assess differences between the altitudes of isentrope surfaces sampled at mesoscale versus synoptic scale. It has been found that the synoptic scale isentropes fail to capture a significant component of vertical displacement of isentrope surfaces, especially in the vicinity of jet streams. Under the assumptions that air parcels flow along isentrope surfaces, and change temperature adiabatically while undergoing altitude displacements, it is possible to compute mesoscale temperature fluctuations that are not present in synoptic scale back trajectory parcel temperature histories. It has been found that the magnitude of the mesoscale component of temperature fluctuations varies with altitude, season, latitude and underlying topography. A model for these dependences is presented, which shows, for example, that mesoscale temperature fluctuations increase with altitude in a systematic way, are greatest over mountainous terrain, and are greater at polar latitudes during winter.
The composition of nucleation and Aitken modes particles during coastal nucleation events: evidence for marine secondary organic contribution
Authors: Vaattovaara P. , Huttunen P. E. , Yoon Y. J. , Joutsensaari J. , Lehtinen K. E. J. , O'Dowd C. D. , Laaksonen A.
Published: April 2010

Abstract. Newly-formed nanometer-sized particles have been observed at coastal and marine environments world wide. Organic species have so far not been detected in those newly-formed nucleation mode particles. In this study, we applied the ultrafine organic tandem differential mobility analyzer method to study the possible existence of an organic fraction in recently formed coastal nucleation mode particles (d<20 nm) at the Mace Head research station. Furthermore, effects of those nucleation events on potential cloud condensation nuclei were studied. The coastal events were typical for the Mace Head region and they occurred at low tide conditions during efficient solar radiation and enhanced biological activity in spring 2002. Additionally, a pulse height analyzer ultrafine condensation particle counter technique was used to study the composition of newly-formed particles formed in low tide conditions during a lower biological activity in October 2002. The overall results of the ultrafine organic tandem differential mobility analyzer and the pulse height analyzer ultrafine condensation particle counter measurements indicate that those coastally/marinely formed nucleation mode particles include a remarkable fraction of secondary organic products, beside iodine oxides, which are likely to be responsible for the nucleation. During clean marine air mass conditions, the origin of those secondary organic oxidation compounds can be related to marine coast and open ocean biota and thus a major fraction of the organics may originate from biosynthetic production of alkenes such as isoprene and their oxidation driven by iodine radicals, hydroxyl radicals, acid catalysis, and ozone during efficient solar radiation. During modified marine conditions, also anthropogenic secondary organic compounds may contribute to the nucleation mode organic mass, in addition to biogenic secondary organic compounds. Thus, the ultrafine organic tandem differential mobility analyzer results suggest that the secondary organic compounds may, in addition to being significant contributors to the nucleation mode processes, accelerate the growth of freshly nucleated particles and increase their survival probability to cloud condensation nuclei and even larger radiatively active particle sizes. The results give new insights to the marine/coastal particle formation, growth, and properties. The marine biota driven secondary organic contributions to marine/coastal particle formation and composition can be anticipated in other species specific biologically active oceans and fresh-waters areas around the world and thus, they may be significant also to the global radiative bugdet, atmosphere-biosphere feedbacks, and climate change.
Technical Note: An implementation of the dry removal processes DRY DEPosition and SEDImentation in the Modular Earth Submodel System (MESSy)
Authors: Kerkweg A. , Buchholz J. , Ganzeveld L. , Pozzer A. , Tost H. , Jöckel P.
Published: April 2010

Abstract. We present the submodels DRYDEP and SEDI for the Modular Earth Submodel System (MESSy). Dry deposition of gases and aerosols is calculated within DRYDEP, whereas SEDI deals with aerosol particle sedimentation. Dry deposition velocities depend on the near-surface turbulence and the physical and chemical properties of the surface cover (e.g. the roughness length, soil pH or leaf stomatal exchange). The dry deposition algorithm used in DRYDEP is based on the big leaf approach and is described in detail within this Technical Note. The sedimentation submodel SEDI contains two sedimentation schemes: a simple upwind zeroth order scheme and a first order approach.
Impact of H2SO4/H2O coating and ice crystal size on radiative properties of sub-visible cirrus
Authors: Räisänen P. , Bogdan A. , Sassen K. , Kulmala M. , Molina M. J.
Published: April 2010

Abstract. Recent laboratory experiments showed that at conditions resembling those near the tropopause region, small ice particles can be coated by a liquid H2SO4/H2O over-layer formed after the freezing of diluted sulfuric acid/water aerosol drops. Here, idealized radiative transfer tests are conducted to evaluate the impact that such an over-layer would have on the radiative effects produced by sub-visible cirrus clouds (SVCs). Spherical particle shape is assumed to keep the problem tractable. The calculations show that the over-layer increases both the shortwave (SW) and longwave (LW) cloud radiative effects (CRE), but the impact is small: ~0.02 W m−2, or even less, for the total (LW+SW) CRE at the top of the atmosphere. For the smallest ice particles, for which the over-layer is thickest, the fractional change in CRE can, however, reach ~20% for the SW CRE and over 50% for the LW CRE. The dependence of LW and SW CRE on particle size is also studied in the paper. Calculations for spherical and spheroidal uncoated ice particles show that even for high, optically thin cirrus, the total CRE can be negative, if the diameter of the particles is smaller than about 3–4 μm. Apart from the SVCs, this result could be relevant for contrail cirrus clouds, which are believed to consist of large numbers of very small ice particles.
The 1986–1989 ENSO cycle in a chemical climate model
Authors: Brönnimann S. , Schraner M. , Müller B. , Fischer A. , Brunner D. , Rozanov E. , Egorova T.
Published: April 2010

Abstract. A pronounced ENSO cycle occurred from 1986 to 1989, accompanied by distinct dynamical and chemical anomalies in the global troposphere and stratosphere. Reproducing these effects with current climate models not only provides a model test but also contributes to our still limited understanding of ENSO's effect on stratosphere-troposphere coupling. We performed several sets of ensemble simulations with a chemical climate model (SOCOL) forced with global sea surface temperatures. Results were compared with observations and with large-ensemble simulations performed with an atmospheric general circulation model (MRF9). We focus our analysis on the extratropical stratosphere and its coupling with the troposphere. In this context, the circulation over the North Atlantic sector is particularly important. Relative to the La Niña winter 1989, observations for the El Niño winter 1987 show a negative North Atlantic Oscillation index with corresponding changes in temperature and precipitation patterns, a weak polar vortex, a warm Arctic middle stratosphere, negative and positive total ozone anomalies in the tropics and at middle to high latitudes, respectively, as well as anomalous upward and poleward Eliassen-Palm (EP) flux in the midlatitude lower stratosphere. Most of the tropospheric features are well reproduced in the ensemble means in both models, though the amplitudes are underestimated. In the stratosphere, the SOCOL simulations compare well with observations with respect to zonal wind, temperature, EP flux, meridional mass streamfunction, and ozone, but magnitudes are underestimated in the middle stratosphere. With respect to the mechanisms relating ENSO to stratospheric circulation, the results suggest that both, upward and poleward components of anomalous EP flux are important for obtaining the stratospheric signal and that an increase in strength of the Brewer-Dobson circulation is part of that signal.
Ground-based remote sensing of HDO/H2O ratio profiles: introduction and validation of an innovative retrieval approach
Authors: Schneider M. , Hase F. , Blumenstock T.
Published: April 2010

Abstract. We propose an innovative approach for analysing ground-based FTIR spectra which allows us to detect variabilities of lower and middle/upper tropospheric HDO/H2O ratios. We show that the proposed method is superior to common approaches. We estimate that lower tropospheric HDO/H2O ratios can be detected with a noise to signal ratio of 15% and middle/upper tropospheric ratios with a noise to signal ratio of 50%. The method requires the inversion to be performed on a logarithmic scale and to introduce an inter-species constraint. While common methods calculate the isotope ratio posterior to an independent, optimal estimation of the HDO and H2O profile, the proposed approach is an optimal estimator for the ratio itself. We apply the innovative approach to spectra measured continuously during 15 months and present, for the first time, an annual cycle of tropospheric HDO/H2O ratio profiles as detected by ground-based measurements. Outliers in the detected middle/upper tropospheric ratios are interpreted by backward trajectories.
Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia
Authors: Rissler J. , Vestin A. , Swietlicki E. , Fisch G. , Zhou J. , Artaxo P. , Andreae M. O.
Published: April 2010

Abstract. Aerosol particle number size distributions and hygroscopic properties were measured at a pasture site in the southwestern Amazon region (Rondonia). The measurements were performed 11 September-14 November 2002 as part of LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia - SMOke aerosols, Clouds, rainfall and Climate), and cover the later part of the dry season (with heavy biomass burning), a transition period, and the onset of the wet period. Particle number size distributions were measured with a DMPS (Differential Mobility Particle Sizer, 3-850nm) and an APS (Aerodynamic Particle Sizer), extending the distributions up to 3.3 µm in diameter. An H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) measured the hygroscopic diameter growth factors (Gf) at 90% relative humidity (RH), for particles with dry diameters (dp) between 20-440 nm, and at several occasions RH scans (30-90% RH) were performed for 165nm particles. These data provide the most extensive characterization of Amazonian biomass burning aerosol, with respect to particle number size distributions and hygroscopic properties, presented until now. The evolution of the convective boundary layer over the course of the day causes a distinct diel variation in the aerosol physical properties, which was used to get information about the properties of the aerosol at higher altitudes. The number size distributions averaged over the three defined time periods showed three modes; a nucleation mode with geometrical median diameters (GMD) of ~12 nm, an Aitken mode (GMD=61-92 nm) and an accumulation mode (GMD=128-190 nm). The two larger modes were shifted towards larger GMD with increasing influence from biomass burning. The hygroscopic growth at 90% RH revealed a somewhat external mixture with two groups of particles; here denoted nearly hydrophobic (Gf~1.09 for 100 nm particles) and moderately hygroscopic (Gf~1.26). While the hygroscopic growth factors were surprisingly similar over the periods, the number fraction of particles belonging to each hygroscopic group varied more, with the dry period aerosol being more dominated by nearly hydrophobic particles. As a result the total particle water uptake rose going into the cleaner period. The fraction of moderately hygroscopic particles was consistently larger for particles in the accumulation mode compared to the Aitken mode for all periods. Scanning the H-TDMA over RH (30-90% RH) showed no deliquescence behavior. A parameterization of both Gf(RH) and Gf(dp), is given.
Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber
Authors: Wagner R. , Benz S. , Möhler O. , Saathoff H. , Schurath U.
Published: April 2010

Abstract. Series of infrared extinction spectra of ice crystals were recorded in the 6000–800 cm−1 wavenumber regime during expansion cooling experiments in the large aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe. Either supercooled sulphuric acid solution droplets or dry mineral dust particles were added as seed aerosols to initiate ice formation after having established ice supersaturated conditions inside the chamber. The various ice nucleation runs were conducted at temperatures between 237 and 195 K, leading to median sizes of the nucleated ice particles of 1–15 µm. The measured infrared spectra were fitted with reference spectra from T-matrix calculations to retrieve the number concentration as well as the number size distribution of the generated ice clouds. The precise evaluation of the time-dependent ice particle number concentrations, i.e., the rates of new ice particle formation, is of particular importance to quantitatively analyse the ice nucleation experiments in terms of nucleation rates and ice activation spectra. The ice particles were modelled as finite circular cylinders with aspect ratios ranging from 0.5 to 3.0. Benefiting from the comprehensive diagnostic tools for the characterisation of ice clouds which are available at the AIDA facility, the infrared retrieval results with regard to the ice particle number concentration could be compared to independent measurements with various optical particle counters. This provided a unique chance to quantitatively assess potential errors or solution ambiguities in the retrieval procedure which mainly originate from the difficulty to find an appropriate shape representation for the aspherical particle habits of the ice crystals. Based on these inter-comparisons, we demonstrate that there is no standard retrieval approach which can be routinely applied to all different experimental scenarios. In particular, the concept to account for the asphericity of the ice crystals, the a priori constraints which might be imposed on the unknown number size distribution of the ice crystals (like employing an analytical distribution function), and the wavenumber range which is included in the fitting algorithm should be carefully adjusted to each single retrieval problem.
McSCIA: application of the Equivalence Theorem in a Monte Carlo radiative transfer model for spherical shell atmospheres
Authors: Spada F. , Krol M. C. , Stammes P.
Published: April 2010

Abstract. A new multiple-scattering Monte Carlo 3-D radiative transfer model named McSCIA (Monte Carlo for SCIAmachy) is presented. The backward technique is used to efficiently simulate narrow field of view instruments. The McSCIA algorithm has been formulated as a function of the Earth's radius, and can thus perform simulations for both plane-parallel and spherical atmospheres. The latter geometry is essential for the interpretation of limb satellite measurements, as performed by SCIAMACHY on board of ESA's Envisat. The model can simulate UV-vis-NIR radiation. First the ray-tracing algorithm is presented in detail, and then successfully validated against literature references, both in plane-parallel and in spherical geometry. A simple 1-D model is used to explain two different ways of treating absorption. One method uses the single scattering albedo while the other uses the equivalence theorem. The equivalence theorem is based on a separation of absorption and scattering. It is shown that both methods give, in a statistical way, identical results for a wide variety of scenarios. Both absorption methods are included in McSCIA, and it is shown that also for a 3-D case both formulations give identical results. McSCIA limb profiles for atmospheres with and without absorption compare well with the one of the state of the art Monte Carlo radiative transfer model MCC++. A simplification of the photon statistics may lead to very fast calculations of absorption features in the atmosphere. However, these simplifications potentially introduce biases in the results. McSCIA does not use simplifications and is therefore a relatively slow implementation of the equivalence theorem.