bluuebunny/crossref_metadata_2025 huggingface dataset:
Comparison of satellite limb-sounding humidity climatologies of the uppermost tropical troposphere
Authors: Ekström M. , Eriksson P. , Read W. G. , Milz M. , Murtagh D. P.
Published: April 2010

Abstract. Humidity climatologies of the tropical uppermost troposphere from satellite limb emission measurements have been compared. Four instruments are considered; UARS-MLS, Odin-SMR, and Aura-MLS operating in the microwave region, and MIPAS in the infrared region. A reference for the comparison is obtained by MOZAIC in-situ measurements. The upper tropospheric humidity products were compared on basis of their empirical probability density functions and seasonally averaged horizontal fields at two altitude layers, 12 and 15 km. The probability density functions of the microwave datasets were found to be in very good agreement with each other, and were also consistent with MOZAIC. The average seasonal humidities differ with less than 10%RHi between the instruments, indicating that stated measurement accuracies of 20–30% are conservative estimates. The systematic uncertainty in Odin-SMR data due to cloud correction was also independently estimated to be 10%RHi. MIPAS humidity profiles were found to suffer from cloud contamination, with only 30% of the measurements reaching into the upper troposphere, but under clear-sky conditions there is a good agreement between MIPAS, Odin-SMR and Aura-MLS. Odin-SMR and the two MLS datasets can be treated as independent, being based on different underlying spectroscopy and technology. The good agreement between the microwave limb-sounders, and MOZAIC, is therefore an important step towards understanding the upper tropospheric humidity. The found accuracy of 10%RHi is approaching the level required to validate climate modelling of the upper troposphere humidity. The comparison of microwave and infrared also stresses that microwave limb-sounding is necessary for a complete view of the upper troposphere.
Validation of HNO3, ClONO2, and N2O5 from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)
Authors: Wolff M. A. , Kerzenmacher T. , Strong K. , Walker K. A. , Toohey M. , Dupuy E. , Bernath P. F. , Boone C. D. , Brohede S. , Catoire V. , von Clarmann T. , Coffey M. , Daffer W. H. , De Mazière M. , Duchatelet P. , Glatthor N. , Griffith D. W. T. , Hannigan J. , Hase F. , Höpfner M. , Huret N. , Jones N. , Jucks K. , Kagawa A. , Kasai Y. , Kramer I. , Küllmann H. , Kuttippurath J. , Mahieu E. , Manney G. , McElroy C. T. , McLinden C. , Mébarki Y. , Mikuteit S. , Murtagh D. , Piccolo C. , Raspollini P. , Ridolfi M. , Ruhnke R. , Santee M. , Senten C. , Smale D. , Tétard C. , Urban J. , Wood S.
Published: April 2010

Abstract. The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv ±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.
A model tool for assessing real-time mixing of mineral and anthropogenic pollutants in East Asia: a case study of April 2005
Authors: Lasserre F. , Cautenet G. , Bouet C. , Dong X. , Kim Y. J. , Sugimoto N. , Matsui I. , Shimizu A.
Published: April 2010

Abstract. In order to assess the complex mixing of atmospheric anthropogenic and natural pollutants over the East Asian region, we present a modelling tool which takes into account the main aerosols which are to be found simultaneously over China, Korea and Japan during springtime. Using the mesoscale RAMS (Regional Atmospheric Modeling System) tool, we present a simulation of natural (desert) dust events along with some of the most critical anthropogenic pollutants over East Asia, sulphur elements (SO2 and SO2-4) and Black Carbon (BC). As regards a one-week case study of dust events which occurred during late April 2005 over an area extending from the Gobi deserts to the Japan surroundings, we satisfactorily model the behaviours of the different aerosol plumes. We focus on possible dust mixing with the anthropogenic pollutants from megacities. For both natural and anthropogenic pollution, the model results are in fairly good agreement with the horizontal and vertical distributions of concentrations as measured by in situ LIDAR, and as observed in remote data, PM10 data and literature. In particular, we show that a simplified chemistry approach of this complex issue is sufficient to model this event, with a real-time step of 3 h. The model reproduces the main patterns and orders of magnitude for Aerosol Optical Thickness (AOT) and species contributions (via the Angström Exponent) when compared with the AErosol RObotic NETwork (AERONET) data.
Personal UV exposure in high albedo alpine sites
Authors: Siani A. M. , Casale G. R. , Diémoz H. , Agnesod G. , Kimlin M. G. , Lang C. A. , Colosimo A.
Published: April 2010

Abstract. Mountain sites experience enhanced UV radiation levels due to the concurrent effects of shorter radiation path-length, low aerosol load and high reflectivity of the snow surfaces. This study was encouraged by the possibility to collect original data of personal dose on a specific anatomical site (erythemally effective UV dose on the forehead) of two groups of volunteers (ski instructors and skiers) in the mountainous areas of Italy (the Alpine site of La Thuile-Les Suches in Valle d'Aosta region). Personal doses were assessed using polysulphone dosimetry. Exposure Ratio (ER), defined as the ratio between the personal dose and the corresponding ambient dose (i.e. erythemally weighted dose received by a horizontal surface) during the same exposure period was taken into account. In addition measuring skin colours as biological markers of individual response to UV exposure, was also carried out on the forearm and cheek of each volunteer before and after exposure. The median ER, taking into account the whole sample, is 0.60 in winter, with a range of 0.29 to 1.46, and 1.02 in spring, ranging from 0.46 to 1.72. No differences in ERs were found between skiers and instructors in spring while in winter skiers experienced lower values. Regarding skin colorimetric parameters the main result was that both skiers and instructors had on average significantly lower values of luminance after exposure i.e.~they became darker. It was found that the use of sunscreen and individual skin photo-type did not produce significant variations in ER across instructor/skier group by day and by seasons (p>0.05). It seems that sunscreen use only at the beginning of the exposure or in a few cases a couple of times during exposure (at difference with the specific instructions sheets), was not sufficient to change significantly skin colorimetric parameters across participants. In conclusion UV personal doses on the ski-fields are often significantly higher than those on horizontal surfaces and consistently more intense respect to personal doses received by sunbathers on the beach in central Italy (ER range: 0.09–0.42). Given the high levels of exposure observed in the present study, specific public health warnings with regards to the efficacy of sun-protection behaviours (proper application and re-application of sunscreen and protective measures such as hats and sun glasses) should be adopted.
Chemistry of sprite discharges through ion-neutral reactions
Authors: Hiraki Y. , Kasai Y. , Fukunishi H.
Published: April 2010

Abstract. We estimate the concentration changes, caused by streamer discharge in sprites, of ozone and related minor species as odd nitrogen (NOx) and hydrogen (HOx) families in the upper stratosphere and mesosphere. The streamer has an intense electric field and high electron density at its head, where a large number of chemically-radical ions and atoms are produced through electron impact on neutral molecules. After its propagation, densities of minor species can be perturbed through ion-neutral chemical reactions initiated by the relaxation of these radical products. We evaluate the production rates of ions and atoms using an electron kinetics model and by assuming that the electric field and electron density are in the head region. We calculate the density variations mainly for NOx, Ox, and HOx species using a one-dimensional model of the neutral and ion composition of the middle atmosphere, including the effect of the sprite streamer. Results at the nighttime condition show that the densities of NO, O3, H, and OH increase suddenly through reactions triggered by the first atomic nitrogen and oxygen product, and electrons just after streamer initiation. It is shown that NO and NO2 still remain for 1 h by a certain order of increase with their source-sink balance, predominantly around 60 km; for other species, increases in O3, OH, HO2, and H2O2 still remain in the range of 40–70 km. From this affirmative result of long-time behavior previously not presented, we emphasize that sprites would have the power to impact local chemistry at night. We also discuss the consistency with previous theoretical and observational studies, along with future suggestions.
Ternary solution of sodium chloride, succinic acid and water; surface tension and its influence on cloud droplet activation
Authors: Vanhanen J. , Hyvärinen A.-P. , Anttila T. , Raatikainen T. , Viisanen Y. , Lihavainen H.
Published: April 2010

Abstract. Surface tension of ternary solution of sodium chloride, succinic acid and water was measured as a function of both composition and temperature by using the capillary rise technique. Both sodium chloride and succinic acid are found in atmospheric aerosols, the former being main constituent of marine aerosol. Succinic acid was found to decrease the surface tension of water already at very low concentrations. Sodium chloride increased the surface tension linearly as a function of the concentration. Surface tensions of both binary solutions agreed well with the previous measurements. Succinic acid was found to lower the surface tension even if sodium chloride is present, indicating that succinic acid, as a surface active compound, tends to concentrate to the surface. An equation based on thermodynamical relations was fitted to the data and extrapolated to the whole concentration range by using estimated surface tensions for pure compounds. As a result, we obtained an estimate of surface tensions beyond solubility limits in addition to a fit to the experimental data. The parameterization can safely be used at temperatures from 10 to 30°C. These kinds of parameterizations are important for example in atmospheric nucleation models. To investigate the influence of surface tension on cloud droplet activation, the surface tension parameterization was included in an adiabatic air parcel model. Usually in cloud models the surface tension of pure water is used. Simulations were done for characteristic marine aerosol size distributions consisting of the considered ternary mixture. We found that by using the surface tension of pure water, the amount of activated particles is underestimated up to 8% if particles contain succinic acid and overestimated it up to 8% if particles contain only sodium chloride. The surface tension effect was found to increase with increasing updraft velocity.
Changes of fatty acid aerosol hygroscopicity induced by ozonolysis under humid conditions
Authors: Vesna O. , Sjogren S. , Weingartner E. , Samburova V. , Kalberer M. , Gäggeler H. W. , Ammann M.
Published: April 2010

Abstract. Unsaturated fatty acids are important constituents of the organic fraction of atmospheric aerosols originating from biogenic or combustion sources. Oxidative processing of these may change their interaction with water and thus affect their effect on climate. The ozonolysis of oleic and arachidonic acid aerosol particles was studied under humid conditions in a flow reactor at ozone exposures close to atmospheric levels, at concentrations between 0.5 and 2 ppm. While oleic acid is a widely used proxy for such studies, arachidonic acid represents polyunsaturated fatty acids, which may decompose into hygroscopic products. The hygroscopic (diameter) growth factor at 93% relative humidity (RH) of the oxidized arachidonic particles increased up to 1.09 with increasing RH during the ozonolysis. In contrast, the growth factor of oleic acid was very low (1.03 at 93% RH) and was almost invariant to the ozonolysis conditions, so that oleic acid is not a good model to observe oxidation induced changes of hygroscopicity under atmospheric conditions. We show for arachidonic acid particles that the hygroscopic changes induced by humidity during ozonolysis are accompanied by about a doubling of the ratio of carboxylic acid protons to aliphatic protons. We suggest that, under humid conditions, the reaction of water with the Criegee intermediates might open a pathway for the formation of smaller acids that lead to more significant changes in hygroscopicity. Thus the effect of water to provide a competing pathway during ozonolysis observed in this study should be motivation to include water, which is ubiquitously present in and around atmospheric particles, in future studies related to aerosol particle aging.
Comparison of UV irradiance measurements at Summit, Greenland; Barrow, Alaska; and South Pole, Antarctica
Authors: Bernhard G. , Booth C. R. , Ehramjian J. C.
Published: April 2010

Abstract. An SUV-150B spectroradiometer for measuring solar ultraviolet (UV) irradiance was installed at Summit, Greenland, in August 2004. Here we compare the initial data from this new location with similar measurements from Barrow, Alaska, and South Pole. Measurements of irradiance at 345 nm performed at equivalent solar zenith angles (SZAs) are almost identical at Summit and South Pole. The good agreement can be explained with the similar location of the two sites on high-altitude ice caps with high surface albedo. Clouds attenuate irradiance at 345 nm at both sites by less than 6% on average, but can reduce irradiance at Barrow by more than 75%. Clear-sky measurements at Barrow are smaller than at Summit by 14% in spring and 36% in summer, mostly due to differences in surface albedo and altitude. Comparisons with model calculations indicate that aerosols can reduce clear-sky irradiance at Summit by 4–6%; aerosol influence is largest in April. Differences in total ozone at the three sites have a large influence on the UV Index. At South Pole, the UV Index is on average 20–80% larger during the ozone hole period than between January and March. At Summit, total ozone peaks in April and UV Indices in spring are on average 10–25% smaller than in the summer. Maximum UV Indices ever observed at Summit, Barrow, and South Pole are 6.7, 5.0, and 4.0, respectively. The larger value at Summit is due to the site's lower latitude. For comparable SZAs, average UV Indices measured during October and November at South Pole are 1.9–2.4 times larger than measurements during March and April at Summit. Average UV Indices at Summit are over 50% greater than at Barrow because of the larger cloud influence at Barrow.
Ship plume dispersion rates in convective boundary layers for chemistry models
Authors: Chosson F. , Paoli R. , Cuenot B.
Published: April 2010

Abstract. Detailed ship plume simulations in various convective boundary layer situations have been performed using a Lagrangian Dispersion Model driven by a Large Eddy Simulation Model. The simulations focus on the early stage (1–2 h) of plume dispersion regime and take into account the effects of plume rise on dispersion. Results are presented in an attempt to provide to atmospheric chemistry modellers a realistic description of characteristic dispersion impact on exhaust ship plume chemistry. Plume dispersion simulations are used to derive analytical dilution rate functions. Even though results exhibit striking effects of plume rise parameter on dispersion patterns, it is shown that initial buoyancy fluxes at ship stack have a minor effect on plume dilution rate. After initial high dispersion regimes a simple characteristic dilution time scale can be used to parameterize the subgrid plume dilution effect in large-scale chemistry models. The results show that this parameter is directly related to the typical turn-over time scale of the convective boundary layer.
The aerosol distribution in Europe derived with the Community Multiscale Air Quality (CMAQ) model: comparison to near surface in situ and sunphotometer measurements
Authors: Matthias V.
Published: April 2010

Abstract. The aerosol distribution in Europe was simulated with the Community Multiscale Air Quality (CMAQ) model system version 4.5 for the years 2000 and 2001. The results were compared with daily averages of PM10 measurements taken in the framework of EMEP and with aerosol optical depth (AOD) values measured within AERONET. The modelled total aerosol mass is typically about 30–60% lower than the corresponding measurements. However a comparison of the chemical composition of the aerosol revealed a considerably better agreement between the modelled and the measured aerosol components for ammonium, nitrate and sulfate, which are on average only 15–20% underestimated. Sligthly worse agreement was determined for sea salt, that was only avaliable at two sites. The largest discrepancies result from the aerosol mass which was not chemically specified by the measurements. The agreement between measurements and model is better in winter than in summer. The modelled organic aerosol mass is higher in summer than in winter but it is significantly underestimated by the model. This could be one of the main reasons for the discrepancies between measurements and model results. The other is that primary coarse particles are underestimated in the emissions. The probability distribution function of the PM10 measurements follows a log-normal distribution at most sites. The model is only able to reproduce this distribution function at non-coastal low altitude stations. The AOD derived from the model results is 20–70% lower than the values observed within AERONET. This is mainly attributed to the missing aerosol mass in the model. The day-to-day variability of the AOD and the log-normal distribution functions are quite well reproduced by the model. The seasonality on the other hand is underestimated by the model results because better agreement is achieved in winter.
Tropospheric ozone sources and wave activity over Mexico City and Houston during MILAGRO/Intercontinental Transport Experiment (INTEX-B) Ozonesonde Network Study, 2006 (IONS-06)
Authors: Thompson A. M. , Yorks J. E. , Miller S. K. , Witte J. C. , Dougherty K. M. , Morris G. A. , Baumgardner D. , Ladino L. , Rappenglück B.
Published: April 2010

Abstract. During the INTEX-B (Intercontinental Chemical Transport Experiment)/ MILAGRO (Megacities Initiative: Local and Global Research Observations) experiments in March 2006 and the associated IONS-06 (INTEX Ozonesonde Network Study; http://croc.gsfc.nasa.gov/intexb/ions06.html), regular ozonesonde launches were made over 15 North American sites. The soundings were strategically positioned to study inter-regional flows and meteorological interactions with a mixture of tropospheric O3 sources: local pollution; O3 associated with convection and lightning; stratosphere-troposphere exchange. The variability of tropospheric O3 over the Mexico City Basin (MCB; 19° N, 99° W) and Houston (30° N, 95° W) is reported here. MCB and Houston profiles displayed a double tropopause in most soundings and a subtropical tropopause layer with frequent wave disturbances, identified through O3 laminae as gravity-wave induced. Ozonesondes launched over both cities in August and September 2006 (IONS-06, Phase 3) displayed a thicker tropospheric column O3 (~7 DU or 15–20%) than in March 2006; nearly all of the increase was in the free troposphere. In spring and summer, O3 laminar structure manifested mixed influences from the stratosphere, convective redistribution of O3 and precursors, and O3 from lightning NO. Stratospheric O3 origins were present in 39% (MCB) and 60% (Houston) of the summer sondes. Comparison of summer 2006 O3 structure with summer 2004 sondes (IONS-04) over Houston showed 7% less tropospheric O3 in 2006. This may reflect a sampling contrast, August to mid-September 2006 instead of July-mid August 2004.
CO emission and export from Asia: an analysis combining complementary satellite measurements (MOPITT, SCIAMACHY and ACE-FTS) with global modeling
Authors: Turquety S. , Clerbaux C. , Law K. , Coheur P.-F. , Cozic A. , Szopa S. , Hauglustaine D. A. , Hadji-Lazaro J. , Gloudemans A. M. S. , Schrijver H. , Boone C. D. , Bernath P. F. , Edwards D. P.
Published: April 2010

Abstract. This study presents the complementary picture of the pollution outflow provided by several satellite observations of carbon monoxide (CO), based on different observation techniques. This is illustrated by an analysis of the Asian outflow during the spring of 2005, through comparisons with simulations by the LMDz-INCA global chemistry transport model. The CO observations from the MOPITT and SCIAMACHY nadir sounders, which provide vertically integrated information with excellent horizontal sampling, and from the ACE-FTS solar occultation instrument, which has limited spatial coverage but allows the retrieval of vertical profiles, are used. Combining observations from MOPITT (mainly sensitive to the free troposphere) and SCIAMACHY (sensitive to the full column) allows a qualitative evaluation of the boundary layer CO. The model tends to underestimate this residual compared to the observations, suggesting underestimated emissions, especially in eastern Asia. However, a better understanding of the consistency and possible biases between the MOPITT and SCIAMACHY CO is necessary for a quantitative evaluation. Underestimated emissions, and possibly too low lofting and underestimated chemical production in the model, lead to an underestimate of the export to the free troposphere, as highlighted by comparisons with MOPITT and ACE-FTS. Both instruments observe large trans-Pacific transport extending from ~20° N to ~60° N, with high upper tropospheric CO observed by ACE-FTS above the eastern Pacific (with values of up to 300 ppbv around 50° N at 500 hPa and up to ~200 ppbv around 30° N at 300 hPa). The low vertical and horizontal resolutions of the global model do not allow the simulation of the strong enhancements in the observed plumes. However, the transport patterns are well captured, and are mainly attributed to export from eastern Asia, with increasing contributions from South Asia and Indonesia towards the tropics. Additional measurements of C2H2, C2H6 and HCN by ACE-FTS provide further information on the plume history. C2H2 and C2H6 enhancements are well correlated with the CO plumes, indicating common sources and rapid trans-Pacific transport. HCN observations show that the biomass burning contributes mainly at latitudes lower than ~40° N. This study provides a first step towards a full combination of complementary observations, but also highlights the need for a better evaluation of consistency between the datasets in order to allow precise quantitative analyses.
Long-term field performance of a tunable diode laser absorption spectrometer for analysis of carbon isotopes of CO2 in forest air
Authors: Schaeffer S. M. , Miller J. B. , Vaughn B. H. , White J. W. C. , Bowling D. R.
Published: April 2010

Abstract. Tunable diode laser absorption spectrometry (TDLAS) is gaining in popularity for measuring the mole fraction [CO2] and stable isotopic composition (δ13C) of carbon dioxide (CO2) in air in studies of biosphere-atmosphere gas exchange. Here we present a detailed examination of the performance of a commercially-available TDLAS located in a high-altitude subalpine coniferous forest (the Niwot Ridge AmeriFlux site), providing the first multi-year analysis of TDLAS instrument performance for measuring CO2 isotopes in the field. Air was sampled from five to nine vertical locations in and above the forest canopy every ten minutes for 2.4 years. A variety of methods were used to assess instrument performance. Measurement of two compressed air cylinders that were in place over the entire study establish the long-term field precision of 0.2 μmol mol−1 for [CO2] and 0.35‰ for δ13C, but after fixing several problems the isotope precision improved to 0.2‰ (over the last several months). The TDLAS provided detail on variability of δ13C of atmospheric CO2 that was not represented in weekly flask samples, as well as information regarding the influence of large-scale (regional) seasonal cycle and local forest processes on [CO2] and δ13C of CO2. There were also clear growing season and winter differences in the relative contributions of photosynthesis and respiration on the [CO2] and δ13C of forest air.
Mode resolved density of atmospheric aerosol particles
Authors: Kannosto J. , Virtanen A. , Lemmetty M. , Mäkelä J. M. , Keskinen J. , Junninen H. , Hussein T. , Aalto P. , Kulmala M.
Published: April 2010

Abstract. In this study, we investigate the mode resolved density of ultrafine atmospheric particles measured in boreal forest environment. The method used here enables us to find the distinct density information for each mode in atmospheric fine particle population: the density values for nucleation, Aitken, and accumulation mode particles are presented. The experimental data was gained during 2 May 2005–19 May 2005 at the boreal forest measurement station "SMEAR II" in Hyytiälä, Southern Finland. The density values for accumulation mode varied from 1.1 to 2 g/cm3 (average 1.5 g/cm3) and for Aitken mode from 0.4 to 2 g/cm3 (average 0.97 g/cm3). As an overall trend during the two weeks campaign, the density value of Aitken mode was seen to gradually increase. With the present method, the time dependent behaviour of the particle density can be investigated in the time scale of 10 min. This allows us to follow the density evolution of the nucleation mode particles during the particle growth process following the nucleation burst. The density of nucleation mode particles decreased during the growth process. The density values for 15 nm particles were 1.2–1.5 g/cm3 and for grown 30 nm particles 0.5–1 g/cm3. These values are consistent with the present knowledge that the condensing species are semi-volatile organics, emitted from the boreal forest.
Increased UV radiation due to polar ozone chemical depletion and vortex occurrences at Southern Sub-polar Latitudes in the period [1997–2005]
Authors: Pazmiño A. F. , Godin-Beekmann S. , Luccini E. A. , Piacentini R. D. , Quel E. J. , Hauchecorne A.
Published: April 2010

Abstract. The variability of total ozone and UV radiation from Total Ozone Mapping Spectrometer (TOMS) measurements is analyzed as a function of polar vortex occurrences over the southern subpolar regions during the 1997–2005 period. The analysis of vortex occurrences showed high interannual variability in the 40° S–60° S latitude band with a longitudinal asymmetry showing the largest frequencies over the 90° W–90° E region. The impact of vortex occurrences on UV radiation and ozone in clear sky conditions was determined from the comparison between the measurements inside the vortex and a climatology obtained from data outside the vortex over the studied period. Clear sky conditions were determined from TOMS reflectivity data. For measurements outside the vortex, clear sky conditions were selected for reflectivity values lower than 7.5%, while for measurements inside the vortex, a relaxed threshold was determined from statistically similar UV values as a function of reflectivity. UV changes and ozone differences from the climatology were analyzed in the 40° S–50° S and 50° S–60° S latitude bands during the spring period (September to November). The largest UV increases and ozone decreases, reaching ~200% and ~65%, respectively, were found in the 50° S–60° S latitude band in September and October. The heterogeneous ozone loss during vortex occurrences was estimated using a chemical transport model. The largest impact of vortex occurrences was found in October with mean UV increase, total ozone decrease and accumulated ozone loss in the 350–650 K range of, respectively, 47%, 30% and 57%. The region close to South America is the most affected by the Antarctic ozone depletion due to the combined effect of large number of vortex occurrences, lower cloud cover and large ozone decrease. This region would be the most vulnerable in case of cloud cover decrease, due to more frequent occurrence of ozone poor air masses during austral spring.
Photolysis frequency measurement techniques: results of a comparison within the ACCENT project
Authors: Bohn B. , Corlett G. K. , Gillmann M. , Sanghavi S. , Stange G. , Tensing E. , Vrekoussis M. , Bloss W. J. , Clapp L. J. , Kortner M. , Dorn H.-P. , Monks P. S. , Platt U. , Plass-Dülmer C. , Mihalopoulos N. , Heard D. E. , Clemitshaw K. C. , Meixner F. X. , Prevot A. S. H. , Schmitt R.
Published: April 2010

Abstract. An intercomparison of different radiometric techniques measuring atmospheric photolysis frequencies j(NO2), j(HCHO) and j(O1D) was carried out in a two-week field campaign in June 2005 at Jülich, Germany. Three double-monochromator based spectroradiometers (DM-SR), three single-monochromator based spectroradiometers with diode-array detectors (SM-SR) and seventeen filter radiometers (FR) (ten j(NO2)-FR, seven j(O1D)-FR) took part in this comparison. For j(NO2), all spectroradiometer results agreed within ±3%. For j(HCHO), agreement was slightly poorer between −8% and +4% of the DM-SR reference result. For the SM-SR deviations were explained by poorer spectral resolutions and lower accuracies caused by decreased sensitivities of the photodiode arrays in a wavelength range below 350 nm. For j(O1D), the results were more complex within +8% and −4% with increasing deviations towards larger solar zenith angles for the SM-SR. The direction and the magnitude of the deviations were dependent on the technique of background determination. All j(NO2)-FR showed good linearity with single calibration factors being sufficient to convert from output voltages to j(NO2). Measurements were feasible until sunset and comparison with previous calibrations showed good long-term stability. For the j(O1D)-FR, conversion from output voltages to j(O1D) needed calibration factors and correction functions considering the influences of total ozone column and elevation of the sun. All instruments showed good linearity at photolysis frequencies exceeding about 10% of maximum values. At larger solar zenith angles, the agreement was non-uniform with deviations explainable by insufficient correction functions. Comparison with previous calibrations for some j(O1D)-FR indicated drifts of calibration factors.
Typical distribution of the solar erythemal UV radiation over Slovakia
Authors: Pribullová A. , Chmelík M.
Published: April 2010

Abstract. Maps of solar erythemal ultraviolet (EUV) irradiance daily doses were created for every month with a horizontal resolution of 500 m at the geographical domain 47.15 N–49.86 N×16.94 E–22.81 E covering the territory of Slovakia. The cloud modification factor for the EUV radiation (cmfUV) was modeled utilizing the relation between the cloud modification factor of global and EUV radiation. The maps of the cmfUV factor were created by utilizing measurements of global irradiance performed at nine observatories during the period 1995–2004 and modeling of the cmfUV dependence on altitude. Maps of the EUV irradiance daily dose corresponded to clear-sky conditions and EUV irradiance daily dose affected by average cloudiness were constructed for mean monthly total ozone, its upper and lower monthly limits, for two probability levels of snow cover occurrence as criteria for the snow effect incorporation in the model and for one day representing typical values for every month. The map-set can be regarded as an atlas of solar EUV radiation over Slovakia.
Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets
Authors: Murray B. J.
Published: April 2010

Abstract. Homogeneous nucleation of ice within aqueous solution droplets and their subsequent crystallisation is thought to play a significant role in upper tropospheric ice cloud formation. It is normally assumed that homogeneous nucleation will take place at a threshold supersaturation, irrespective of the identity of the solute, and that rapid growth of ice particles will follow immediately after nucleation. However, it is shown here through laboratory experiments that droplets may not readily freeze in the very cold tropical tropopause layer (TTL, typical temperatures of 186–200 K). In these experiments ice crystal growth in citric acid solution droplets did not occur when ice nucleated below 197±6 K. Citric acid, 2-hydroxypropane-1,2,3-tricarboxyllic acid, is a molecule with similar functionality to oxygenated organic compounds which are ubiquitous in atmospheric aerosol. It is therefore thought to be a sensible proxy for atmospheric organic material. Evidence is presented that suggests citric acid solution droplets become ultra-viscous and form glassy solids under atmospherically relevant conditions. Diffusion of liquid water molecules to ice nuclei is expected to be very slow in ultra-viscous solution droplets and nucleation is negligible in glassy droplets; this most likely provides an explanation for the experimentally observed inhibition of ice crystallisation. The implications of ultra-viscous and glassy solution droplets for ice cloud formation and supersaturations in the TTL are discussed.
Application of the Aventech AIMMS20AQ airborne probe for turbulence measurements during the Convective Storm Initiation Project
Authors: Beswick K. M. , Gallagher M. W. , Webb A. R. , Norton E. G. , Perry F.
Published: April 2010

Abstract. The Convective Storm Initiation Project (CSIP) took place during the summers of 2004 and 2005, centred on the research radar at Chilbolton, UK. Precursors to convective precipitation were studied, using a comprehensive and broad-based range of fieldwork and modelling. The principal aim of CSIP was the detection of the primary and secondary initiation of convective cells. The Universities Facility for Atmospheric Measurements (UFAM) Cessna 182 was used to map temperature and humidity fields over a broad area within and beyond the Chilbolton radar beam. Additionally, air motion was measured using a new turbulence probe, the AIMMS20AQ. The performance of the probe is critically appraised, based on calibrations, test flights and data flights flown during CSIP intensive operating periods. In general, the probe performed well, although some aspects require more careful data interpretation which we describe in detail.
Technical Note: Review of methods for linear least-squares fitting of data and application to atmospheric chemistry problems
Authors: Cantrell C. A.
Published: April 2010

Abstract. The representation of data, whether geophysical observations, numerical model output or laboratory results, by a best fit straight line is a routine practice in the geosciences and other fields. While the literature is full of detailed analyses of procedures for fitting straight lines to values with uncertainties, a surprising number of scientists blindly use the standard least-squares method, such as found on calculators and in spreadsheet programs, that assumes no uncertainties in the x values. Here, the available procedures for estimating the best fit straight line to data, including those applicable to situations for uncertainties present in both the x and y variables, are reviewed. Representative methods that are presented in the literature for bivariate weighted fits are compared using several sample data sets, and guidance is presented as to when the somewhat more involved iterative methods are required, or when the standard least-squares procedure would be expected to be satisfactory. A spreadsheet-based template is made available that employs one method for bivariate fitting.
Long-term measurements of carbonaceous aerosols in the Eastern Mediterranean: evidence of long-range transport of biomass burning
Authors: Sciare J. , Oikonomou K. , Favez O. , Liakakou E. , Markaki Z. , Cachier H. , Mihalopoulos N.
Published: April 2010

Abstract. Long-term (5-year) measurements of Elemental Carbon (EC) and Organic Carbon (OC) in bulk aerosols are presented here for the first time in the Mediterranean Basin (Crete Island). A multi-analytical approach (including thermal, optical, and thermo-optical techniques) was applied for these EC and OC measurements. Light absorbing dust aerosols were shown to poorly contribute (+12% on a yearly average) to light absorption coefficient (babs) measurements performed by an optical method (aethalometer). Long-range transport of agricultural waste burning from European countries surrounding the Black Sea was shown for each year during two periods (March–April and July–September). The contribution of biomass burning to the concentrations of EC and OC was shown to be rather small (20 and 14%, respectively, on a yearly basis), although this contribution could be much higher on a monthly basis and showed important seasonal and interannual variability. By removing the biomass burning influence, our data revealed an important seasonal variation of OC, with an increase by almost a factor of two for the spring months of May and June, whereas BC was found to be quite stable throughout the year. Preliminary measurements of Water Soluble Organic Carbon (WSOC) have shown that the monthly mean WSOC/OC ratio remains stable throughout the year (0.45±0.12), suggesting that the partitioning between water soluble and water insoluble organic matter is not significantly affected by biomass burning and secondary organic aerosol (SOA) formation. A chemical mass closure performed in the fine mode (Aerodynamic Diameter, A.D.<1.5μm) showed that the mass contribution of organic matter (POM) was found to be essentially invariable during the year (monthly average of 26±5%).
ENSO surface shortwave radiation forcing over the tropical Pacific
Authors: Pavlakis K. G. , Hatzianastassiou N. , Matsoukas C. , Fotiadi A. , Vardavas I.
Published: April 2010

Abstract. We have studied the spatial and temporal variation of the downward shortwave radiation (DSR) at the surface of the Earth during ENSO events for a 21-year period over the tropical and subtropical Pacific Ocean (40° S–40° N, 90° E–75° W). The fluxes were computed using a deterministic model for atmospheric radiation transfer, along with satellite data from the ISCCP-D2 database, reanalysis data from NCEP/NCAR for the key atmospheric and surface input parameters, and aerosol parameters from GADS (acronyms explained in main text). A clear anti-correlation was found between the downward shortwave radiation anomaly (DSR-A) time-series, in the region 7° S–5° N 160° E–160° W located west of the Niño-3.4 region, and the Niño-3.4 index time-series. In this region where the highest in absolute value DSR anomalies are observed, the mean DSR anomaly values range from −45 Wm−2 during El Niño episodes to +40 Wm−2 during La Niña events. Within the Niño-3.4 region no significant DSR anomalies are observed during the cold ENSO phase in contrast to the warm ENSO phase. A high correlation was also found over the western Pacific (10° S–5° N, 120–140° E), where the mean DSR anomaly values range from +20 Wm−2 to −20 Wm−2 during El Niño and La Niña episodes, respectively. There is also convincing evidence that the time series of the mean downward shortwave radiation anomaly in the off-equatorial western Pacific region 7–15° N 150–170° E, precedes the Niño-3.4 index time-series by about 7 months and the pattern of this anomaly is indicative of ENSO operating through the mechanism of the western Pacific oscillator. Thus, the downward shortwave radiation anomaly is a complementary index to the SST anomaly for the study of ENSO events and can be used to assess whether or not El Niño or La Niña conditions prevail.
A method for evaluating spatially-resolved NOx emissions using Kalman filter inversion, direct sensitivities, and space-based NO2 observations
Authors: Napelenok S. L. , Pinder R. W. , Gilliland A. B. , Martin R. V.
Published: April 2010

Abstract. An inverse modeling method was developed and tested for identifying possible biases in emission inventories using satellite observations. The relationships between emission inputs and modeled ambient concentrations were estimated using sensitivities calculated with the decoupled direct method in three dimensions (DDM-3D) implemented within the framework of the Community Multiscale Air Quality (CMAQ) regional model. As a case study to test the approach, the method was applied to regional ground-level NOx emissions in the southeastern United States as constrained by observations of NO2 column densities derived from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) satellite instrument. A controlled "pseudodata" scenario with a known solution was used to establish that the methodology can achieve the correct solution, and the approach was then applied to a summer 2004 period where the satellite data are available. The results indicate that emissions biases differ in urban and rural areas of the southeast. The method suggested slight downward (less than 10%) adjustment to urban emissions, while rural region results were found to be highly sensitive to NOx processes in the upper troposphere. As such, the bias in the rural areas is likely not solely due to biases in the ground-level emissions. It was found that CMAQ was unable to predict the significant level of NO2 in the upper troposphere that was observed during the NASA Intercontinental Chemical Transport Experiment (INTEX) measurement campaign. The best correlation between satellite observations and modeled NO2 column densities, as well as comparison to ground-level observations of NO2, was obtained by performing the inverse while accounting for the significant presence of NO2 in the upper troposphere not captured by the regional model.
The interpretation of spikes and trends in concentration of nitrate in polar ice cores, based on evidence from snow and atmospheric measurements
Authors: Wolff E. W. , Jones A. E. , Bauguitte S. J.-B. , Salmon R. A.
Published: April 2010

Abstract. Nitrate is frequently measured in ice cores, but its interpretation remains immature. Using daily snow surface concentrations of nitrate at Halley (Antarctica) for 2004–2005, we show that sharp spikes (>factor 2) in nitrate concentration can occur from day to day. Some of these spikes will be preserved in ice cores. Many of them are associated with sharp increases in the concentration of sea salt in the snow. There is also a close association between the concentrations of aerosol nitrate and sea salt aerosol. This evidence is consistent with many of the spikes in deposited nitrate being due to the conversion or trapping of gas-phase nitrate, i.e. to enhanced deposition rather than enhanced atmospheric concentrations of NOy. Previously, sharp spikes in nitrate concentration (with concentration increases of up to a factor 4 seen in probably just one snowfall) have been assigned to sharp production events such as solar proton events (SPEs). We find that it is unlikely that SPEs can produce spikes of the kind seen. Taken together with our evidence that such spikes can be produced depositionally, we find that it is not possible to track past SPEs without carrying out a new multi-site and multi-analyte programme. Seasonal and interannual trends in nitrate concentration in cores from any single site cannot be interpreted in terms of production changes until the recycling of nitrate from central Antarctica to coastal Antarctica is better quantified. It might be possible to assess the interannual input of NOy to the Antarctic lower troposphere by using a network of cores to estimate variability in the total annual deposition across the continent (which we estimate to be 9±2×107kg/a – as NO3−), but it will first have to be established that the outflow across the coast can be ignored.
The influence of chemical composition and mixing state of Los Angeles urban aerosol on CCN number and cloud properties
Authors: Cubison M. J. , Ervens B. , Feingold G. , Docherty K. S. , Ulbrich I. M. , Shields L. , Prather K. , Hering S. , Jimenez J. L.
Published: April 2010

Abstract. The relationship between cloud condensation nuclei (CCN) number and the physical and chemical properties of the atmospheric aerosol distribution is explored for a polluted urban data set from the Study of Organic Aerosols at Riverside I (SOAR-1) campaign conducted at Riverside, California, USA during summer 2005. The mixing state and, to a lesser degree, the average chemical composition are shown to be important parameters in determining the activation properties of those particles around the critical activation diameters for atmospherically-realistic supersaturation values. Closure between predictions and measurements of CCN number at several supersaturations is attempted by modeling a number of aerosol chemical composition and mixing state cases of increasing complexity. It is shown that a realistic treatment of the state of mixing of the urban aerosol distribution is critical in order to eliminate model bias. Fresh emissions such as elemental carbon and small organic particles must be treated as non-activating and explicitly accounted for in the model. The relative number concentration of these particles compared to inorganics and oxygenated organic compounds of limited hygroscopicity plays an important role in determining the CCN number. Furthermore, expanding the different composition/mixing state cases to predictions of cloud droplet number concentration in a cloud parcel model highlights the dependence of cloud optical properties on the state of mixing and hygroscopic properties of the different aerosol modes, but shows that the relative differences between the different cases are reduced compared to those from the CCN model.