bluuebunny/crossref_metadata_2025 huggingface dataset:
Retrieval of SO2 from thermal infrared satellite measurements: correction procedures for the effects of volcanic ash
Authors: Corradini S. , Merucci L. , Prata A. J.
Published: April 2010

Abstract. The simultaneous presence of SO2 and ash in a volcanic plume can lead to a significant error in the SO2 column abundance retrieval when multispectral Thermal InfraRed (TIR) data are used. The ash particles within the plume with effective radii from 1 to 10 μm reduce the Top Of Atmosphere (TOA) radiance in the entire TIR spectral range, including the channels used for SO2 retrieval. The net effect is a significant SO2 overestimation. In this work the interference of ash is discussed and two correction procedures for satellite SO2 volcanic plume retrieval in the TIR spectral range are developed to achieve an higher computational speed and a better accuracy. The ash correction can be applied when the sensor spectral range includes the 7.3 and/or 8.7 μm SO2 absorption bands, and the split window bands centered around 11 and 12 μm required for ash retrieval. This allows the possibility of simultaneous estimation of both volcanic SO2 and ash in the same data set. The proposed ash correction procedures have been applied to the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Spin Enhanced Visible and Infrared Imager (SEVIRI) measurements. Data collected during the 24 November 2006 Mt. Etna eruption have been used to illustrate the technique. The SO2 and ash estimation is carried out by using a best weighted least squares fit method and the Brightness Temperature Difference (BTD) procedures, respectively. The simulated TOA radiance Look-Up Table (LUT) needed for the SO2 column abundance and the ash retrievals have been computed using the MODTRAN 4 Radiative Transfer Model. The results show the importance of the ash correction on SO2 retrievals at 8.7 μm, where the corrected SO2 column abundance values are less than 50% of the uncorrected values. The ash correction on SO2 retrieval at 7.3 μm is much less important and only significant for low SO2 column abundances. Results also show that the simplified and faster correction procedure underestimates the ash correction compared with the more time consuming but more accurate correction procedure. Such underestimation is greater for instruments having better ground pixel resolution, i.e. greater for MODIS than for SEVIRI.
Methodology and calibration for continuous measurements of biogeochemical trace gas and O2 concentrations from a 300-m tall tower in central Siberia
Authors: Kozlova E. A. , Manning A. C.
Published: April 2010

Abstract. We present an integrated system for measuring atmospheric concentrations of CO2, O2, CH4, CO, and N2O in central Siberia. Our project aims to demonstrate the feasibility of establishing long-term, continuous, high precision atmospheric measurements to elucidate greenhouse gas processes from a very remote, mid-continental boreal environment. Air is sampled from five heights on a custom-built 300-m tower. Common features to all species' measurements include air intakes, an air drying system, flushing procedures, and data processing methods. Calibration standards are shared among all five measured species by extending and optimising a proven methodology for long-term O2 calibration. Our system achieves the precision and accuracy requirements specified by the European Union's "CarboEurope" and "ICOS" (Integrated Carbon Observing System) programmes in the case of CO2, O2, and CH4, while CO and N2O require some further improvements. It was found that it is not possible to achieve these high precision measurements without skilled technical assistance on-site, primarily because of 2–3 month delays in access to data and diagnostic information. We present results on the stability of reference standards in high pressure cylinders. It was also found that some previous methods do not mitigate fractionation of O2 in a sample airstream to a satisfactory level.
Multi-year comparison of stratospheric BrO vertical profiles retrieved from SCIAMACHY limb and ground-based UV-visible measurements
Authors: Hendrick F. , Rozanov A. , Johnston P. V. , Bovensmann H. , De Mazière M. , Fayt C. , Hermans C. , Kreher K. , Lotz W. , Sinnhuber B.-M. , Theys N. , Thomas A. , Burrows J. P. , Van Roozendael M.
Published: April 2010

Abstract. Vertical profiles of stratospheric bromine monoxide (BrO) retrieved daily from ENVISAT/SCIAMACHY (ENVIronmental SATellite/SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) limb scatter data and from ground-based UV-visible observations performed at Harestua (60° N, 11° E), Observatoire de Haute-Provence (44° N, 5.5° E), and Lauder (45° S, 170° E) are compared in the 15–27 km altitude range for the 2002–2006, 2005–2006, and 2002–2005 periods, respectively. At the three stations, the SCIAMACHY and ground-based UV-visible mean profiles agree reasonably well, with relative difference smaller than 23%. When comparing the BrO partial columns, the agreement obtained is good, with mean relative differences smaller than 11% and corresponding standard deviations in the 13–19% range. These comparison results are obtained, however, using different BrO cross sections in SCIAMACHY limb and ground-based UV-visible retrievals. The seasonal variation of the BrO columns at the three stations is consistently captured by both retrievals as well as large BrO column events occurring during the winter and early spring at Harestua which are associated with bromine activation.
The benefit of limb cloud imaging for infrared limb sounding of tropospheric trace gases
Authors: Adams S. , Spang R. , Preusse P. , Heinemann G.
Published: April 2010

Abstract. Advances in detector technology enable a new generation of infrared limb sounders to measure 2-D images of the atmosphere. A proposed limb cloud imager (LCI) mode will detect clouds with a spatial resolution unprecedented for limb sounding. For the inference of temperature and trace gas distributions, detector pixels of the LCI have to be combined into super-pixels which provide the required signal-to-noise and information content for the retrievals. This study examines the extent to which tropospheric coverage can be improved in comparison to limb sounding using a fixed field of view with the size of the super-pixels, as in conventional limb sounders. The study is based on cloud topographies derived from (a) IR brightness temperatures (BT) of geostationary weather satellites in conjunction with ECMWF temperature profiles and (b) ice and liquid water content data of the Consortium for Small-scale Modeling-Europe (COSMO-EU) of the German Weather Service. Limb cloud images are simulated by matching the cloud topography with the limb sounding line of sight (LOS). The analysis of the BT data shows that the reduction of the spatial sampling along the track has hardly any effect on the gain in information. The comparison between BT and COSMO-EU data identifies the strength of both data sets, which are the representation of the horizontal cloud extent for the BT data and the reproduction of the cloud amount for the COSMO-EU data. The results of the analysis of both data sets show the great advantage of the cloud imager. However, because both cloud data sets do not present the complete fine structure of the real cloud fields in the atmosphere it is assumed that the results tend to underestimate the increase in information. In conclusion, real measurements by such an instrument may result in an even higher benefit for tropospheric limb retrievals.
New perspectives on gravity wave remote sensing by spaceborne infrared limb imaging
Authors: Preusse P. , Schroeder S. , Hoffmann L. , Ern M. , Friedl-Vallon F. , Ungermann J. , Oelhaf H. , Fischer H. , Riese M.
Published: April 2010

Abstract. Gravity wave (GW) remote sensing from space now has reached a stage of maturity that some first confinements for GW modeling can be deduced. This is in particular due to global distributions of absolute values of GW momentum flux from infrared limb sounders and due to 2-D maps of the horizontal wave field provided by nadir viewing instruments. The logical step forward is an infrared limb imager (ILI) which combines the good vertical resolution of limb sounding with horizontal mapping capabilities and provides 3-D images of the GW temperature structures. In this paper we investigate 1) how an ILI advances measurements of GW momentum flux, 2) which additional benefits are achieved by limb imaging of GWs, and 3) how an ILI compares to other GW momentum flux measurements, in-situ, ground-based, and from space. In particular, the large advance made by gaining regular 3-D sampling is demonstrated.
Design and construction of a simple Knudsen Effusion Mass Spectrometer (KEMS) system for vapour pressure measurements of low volatility organics
Authors: Booth A. M. , Markus T. , McFiggans G. , Percival C. J. , Mcgillen M. R. , Topping D. O.
Published: April 2010

Abstract. A design of and initial results from a Knudsen Effusion Mass Spectrometer (KEMS) are presented. The design was adapted from high temperature alloy studies with a view to using it to measure vapour pressures for low volatility organics. The system uses a temperature controlled cell with an effusive orifice. This produces a molecular beam which is sampled by a quadropole mass spectrometer with electron impact ionization calibrated to a known vapour pressure. We have determined P(298 K) and ΔHsub of the first 5 saturated straight chain dicarboxylic acids: 2.15±1.19×10-2 Pa and 75±19 KJ mol−1 respectively for oxalic acid, 5.73±1.14×10-4 Pa and 91±4 KJ mol−1 for Malonic acid, 1.13±0.47×10-4 Pa and 93±6 KJ mol−1 for Succinic acid, 4.21±1.66×10-4 Pa and 123±22 KJ mol−1 for Glutaric acid and 6.09±3.85×10-6 Pa and 125±40 KJ mol−1 for Adipic acid.
A Relaxed Eddy Accumulation (REA)-GC/MS system for the determination of halocarbon fluxes
Authors: Hornsby K. E. , Flynn M. J. , Dorsey J. R. , Gallagher M. W. , Chance R. , Jones C. E. , Carpenter L. J.
Published: April 2010

Abstract. Very short lived halocarbons (VSLH) play an important role in the transport of halogen atoms to the troposphere and lower stratosphere. Here we describe the development of a relaxed eddy accumulation system using gas chromatography coupled to a mass spectrometer (REA-GC/MS) to determine surface fluxes of VSLH with a time resolution of about 0.5 h. Laboratory tests showed that use of a common inlet for upward, downward and deadband flow paths resulted in mixing of upward and downward moving air masses, therefore we recommend the use of separate inlets. The modified system underwent field trials at Mace Head on the west coast of Ireland, where there are dense kelp beds known to emit a range of halocarbons. Over a 16 h period in mid-September 2007, the mean fluxes obtained were 16.1±1.8, 4.0±0.54 and 1.2±0.2 nmol m−2 day−1 for CH2Br2 CH2ICl and CH2IBr, respectively.
Comparison of NLC particle sizes derived from SCIAMACHY/Envisat observations with ground-based LIDAR measurements at ALOMAR (69° N)
Authors: von Savigny C. , Robert C. E. , Baumgarten G. , Bovensmann H. , Burrows J. P.
Published: April 2010

Abstract. SCIAMACHY, the Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY has provided measurements of limb-scattered solar radiation in the 220 nm to 2380 nm wavelength range since summer of 2002. Measurements in the UV spectral range are well suited for the retrieval of particle sizes of noctilucent clouds (NLCs) and have been used to compile the largest existing satellite data base of NLC particle sizes. This paper presents a comparison of SCIAMACHY NLC size retrievals with the extensive NLC particle size data set based on ground-based LIDAR measurements at the Arctic LIDAR Observatory for Middle Atmosphere Research (ALOMAR, 69° N, 16° E) for the Northern Hemisphere NLC seasons 2003 to 2007. Most of the presented SCIAMACHY NLC particle size retrievals are based on cylindrical particles and a Gaussian particle size distribution with a fixed width of 24 nm. If the differences in spatial as well as vertical resolution between SCIAMACHY and the ALOMAR LIDAR are taken into account, very good agreement is found. The mean particle size derived from SCIAMACHY limb observations for the ALOMAR overpasses in 2003 to 2007 is 56.2 nm with a standard deviation of 12.5 nm, and the LIDAR observations yield a value of 54.2 nm with a standard deviation of 17.4 nm.
Ground-based FTIR water vapour profile analyses
Authors: Schneider M. , Hase F.
Published: April 2010

Abstract. Due to a large vertical gradient and strong variability of water vapour, algorithms that are effectively applied for ground-based remote sensing of many different atmospheric trace gases can be insufficient for the retrieval of tropospheric water vapour profiles. We review the most important features of the retrieval and of the radiative transfer modelling required for accurate monitoring of tropospheric water vapour profiles by ground-based FTIR (Fourier Transform Infrared) experiments. These are: a fit of a variety of different water vapour lines with different strength, a logarithmic scale inversion, a speed dependent Voigt line shape model, and a joint temperature profile retrieval. Furthermore, the introduction of an interspecies constraint allows for a monitoring of HDO/H2O ratio profiles.
Relationship between the NO2 photolysis frequency and the solar global irradiance
Authors: Trebs I. , Bohn B. , Ammann C. , Rummel U. , Blumthaler M. , Königstedt R. , Meixner F. X. , Fan S. , Andreae M. O.
Published: April 2010

Abstract. Representative values of the atmospheric NO2 photolysis frequency j(NO2) are required for the adequate calculation and interpretation of NO and NO2 concentrations and exchange fluxes near the surface. Direct measurements of j(NO2) at ground level are often not available in field studies. In most cases, modeling approaches involving complex radiative transfer calculations are used to estimate j(NO2) and other photolysis frequencies for air chemistry studies. However, important input parameters for accurate modeling are often missing, most importantly with regard to the radiative effects of clouds. On the other hand, solar global irradiance ("global radiation", G) is nowadays measured as a standard parameter in most field experiments and in many meteorological observation networks around the world. Previous studies mainly reported linear relationships between j(NO2) and G. We have measured j(NO2) using spectro- or filter radiometers and G using pyranometers side-by-side at several field sites. Our results cover a solar zenith angle range of 0–90°, and are based on nine field campaigns in temperate, subtropical and tropical environments during the period 1994–2008. We show that a second-order polynomial function (intercept = 0): j(NO2)=(1+α)× (B1×G+B2×G2), with α defined as the site-dependent UV-A surface albedo and the polynomial coefficients: B1=(1.47± 0.03)×10-5 W−1 m2 s−1 and B2=(-4.84±0.31)×10-9 W−2 m4 s−1 can be used to estimate ground-level j(NO2) directly from G, independent of solar zenith angle under all atmospheric conditions. The absolute j(NO2) residual of the empirical function is ±6×10-4 s−1(2σ). The relationship is valid for sites below 800 m a.s.l. and with low surface albedo (α<0.2). It is not valid in high mountains, above snow or ice and sandy or dry soil surfaces.
Real-time profiling of organic trace gases in the planetary boundary layer by PTR-MS using a tethered balloon
Authors: Schnitzhofer R. , Wisthaler A. , Hansel A.
Published: April 2010

Abstract. A method for real-time profiling of volatile organic compounds (VOCs) was developed combining the advantages of a tethered balloon as a research platform and of proton transfer reaction mass spectrometry (PTR-MS) as an analytical technique for fast and highly sensitive VOC measurements. A 200 m Teflon tube was used to draw sampling air from a tethered aerodynamic balloon to the PTR-MS instrument. Positive and negative artefacts (i.e. formation and loss of VOCs in the tube) were characterised in the laboratory and in the field by a set of 11 atmospherically relevant VOCs including both pure and oxygenated hydrocarbons. The only two compounds that increased or decreased when sampled through the tube were acetone (+7%) and xylene (-6%). The method was successfully deployed during a winter field campaign to determine the small scale spatial and temporal patterns of air pollutants under winter inversion conditions.
Influence of particle charging on TEOM measurements in the presence of an electrostatic precipitator
Authors: Meyer N. K. , Lauber A. , Nussbaumer T. , Burtscher H.
Published: April 2010

Abstract. The efficiency of an electrostatic precipitator (ESP) for reducing wood combustion emissions was investigated. Real-time measurements were conducted by directly reading the change in frequency of the tapered element in a Thermo Scientific 1400a TEOM. These measurements have been shown to be influenced by the charge on the aerosols reaching the tapered element such that the TEOM overestimates mass concentration. This electrostatic effect was crosschecked with particle mass concentration and particle number concentration measurements where no influence was observed. Placing a radioactive neutraliser prior to the TEOM leads to agreement between observed ESP efficiencies as measured by both the TEOM, mass filters and a CPC.
Determining the sea-air flux of dimethylsulfide by eddy correlation using mass spectrometry
Authors: Blomquist B. W. , Huebert B. J. , Fairall C. W. , Faloona I. C.
Published: April 2010

Abstract. Mass spectrometric measurement of DMS by atmospheric pressure ionization with an isotopically labeled standard (APIMS-ILS) is a sensitive method with sufficient bandpass for direct flux measurements by eddy correlation. Use of an isotopically labeled internal standard greatly reduces instrumental drift, improving accuracy and precision. APIMS-ILS has been used in several recent campaigns to study ocean-atmosphere gas transfer and the chemical budget of DMS in the marine boundary layer. This paper provides a comprehensive description of the method and errors associated with DMS flux measurement from ship platforms. The APIMS-ILS instrument used by most groups today has a sensitivity of 100–200 counts s−1 pptv−1, which is shown to be more than sufficient for flux measurement by eddy covariance. Mass spectral backgrounds (blanks) are determined by stripping DMS from ambient air with gold. The instrument is found to exhibit some high frequency signal loss, with a half-power frequency of ≈1 Hz, but a correction based on an empirically determined instrument response function is presented. Standard micrometeorological assumptions of steady state and horizontal uniformity are found to be appropriate for DMS flux measurement, but rapid changes in mean DMS mixing ratio may serve as a warning that measured flux does not represent the true surface flux. In addition, bias in surface flux estimates arising from the flux divergence is not generally significant in the surface layer, but under conditions of lowered inversion and high flux may become so. The effects of error in motion corrections and of vertical motion within the surface layer concentration gradient are discussed and the estimated maximum error from these effects is ≤18%.
Sources of uncertainty in eddy covariance ozone flux measurements made by dry chemiluminescence fast response analysers
Authors: Muller J. B. A. , Percival C. J. , Gallagher M. W. , Fowler D. , Coyle M. , Nemitz E.
Published: April 2010

Abstract. We present a systematic intercomparison study of eddy covariance ozone flux measurements made using two fast response dry chemiluminescence analysers. Ozone deposition was measured over a well characterised managed grassland near Edinburgh, Scotland, during August 2007. A data quality control procedure specific to these analysers is introduced. Absolute ozone fluxes were calculated based on the relative signals of the dry chemiluminescence analysers using three different methods and the results are compared for both analysers. It is shown that the error in the fitted analyser calibration parameters required for the flux calculations provides a substantial source of uncertainty in the fluxes. The choice of the calculation method itself can also constitute an uncertainty in the flux as the calculated fluxes by the three methods do not agree within error at all times. This finding highlights the need for a consistent and rigorous approach for comparable datasets, such as e.g. in flux networks. Ozone fluxes calculated by one of the methods were then used to compare the two analysers in more detail. This systematic analyser comparison reveals half-hourly flux values differing by up to a factor of two at times with the difference in mean hourly flux ranging from 0 to 23% with an error in the mean daily flux of ± 12%. The comparison of analysers shows that the agreement in fluxes is excellent for some days but that there is an underlying uncertainty as a result of variable analyser performance and/or non-linear sensitivity.
A comparison of spectrophotometric and denuder based approaches for the determination of gaseous molecular iodine
Authors: Chance R. J. , Shaw M. , Telgmann L. , Baxter M. , Carpenter L. J.
Published: April 2010

Abstract. The presence of molecular iodine in the atmosphere is thought to have implications for both climate and human nutritional health, but measurement of the gas at low concentrations requires technically demanding techniques that are not widely accessible. Here, amylose coated denuder tubes and solvent traps coupled with spectrophotometric detection are evaluated and compared as relatively cheap and straightforward methods to measure gaseous molecular iodine at environmentally relevant concentrations. Denuder tubes were found to give unacceptably low and highly variable recoveries of molecular iodine from a test gas source, with values ranging from 1 to 62%. Blank concentrations were also high, being equivalent to a gas phase concentration of 5 pptv under typical operating conditions. Ethanol and hexane solvent traps gave much better performance. Optimisation of the hexane solvent trap method gave 100% recovery and an atmospheric limit of detection of 70 pptv, which is within the range of concentrations observed in the coastal marine atmosphere.
The MIPAS2D database of MIPAS/ENVISAT measurements retrieved with a multi-target 2-dimensional tomographic approach
Authors: Dinelli B. M. , Arnone E. , Brizzi G. , Carlotti M. , Castelli E. , Magnani L. , Papandrea E. , Prevedelli M. , Ridolfi M.
Published: April 2010

Abstract. We present a multi-year database of atmospheric fields of the upper troposphere, stratosphere and lower mesosphere retrieved from satellite measurements adopting a 2-dimensional tomographic approach. The full mission of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board the European Space Agency ENVISAT satellite, is analyzed with the Geofit Multi-Target Retrieval (GMTR) system to obtain the MIPAS2D database with atmospheric fields of pressure, temperature and volume mixing ratio of MIPAS main targets H2O, O3, HNO3, CH4, N2O, and NO2. The database covers both the MIPAS nominal observation mode measured at Full Resolution (FR) from July 2002 to March 2004 and the nominal observation mode of the new configuration, measured at Optimized Resolution (OR) and introduced in 2005. Further to the main targets, minor species N2O5, ClONO2, COF2, CFC-11, and CFC-12 for the FR mission only have been included in MIPAS2D to enhance its applicability in studies of stratospheric chemistry. The database is continuously updated with the analysis of the ongoing measurements that are planned to last until the end of 2013 and extended to other targets. The GMTR algorithm is operated on a fixed vertical grid coincident with the tangent altitudes of the FR nominal mode, spanning the altitude range from 6 to 68 km. In the horizontal domain, FR measurements are retrieved on both the observational grid and an equispaced 5 latitudinal-degrees grid which is made possible by the 2-dimensional retrieval algorithm. The analysis of MIPAS OR observations is operated on the same altitude-latitude fixed retrieval grid used for the FR measurements. This choice provides a database with a homogeneous altitude and latitude grid, over the whole globe, covering to date about seven years of measurements. The equispaced latitude grid provides a new and convenient layout for the much needed synergetic studies of data from various instrumental and modeling sources. MIPAS2D is available to the scientific community through the two web sites http://www.mbf.fci.unibo.it/mipas2d.html, and http://www.isac.cnr.it/~rss/mipas2d.htm
Measurement of relative humidity dependent light scattering of aerosols
Authors: Fierz-Schmidhauser R. , Zieger P. , Wehrle G. , Jefferson A. , Ogren J. A. , Baltensperger U. , Weingartner E.
Published: April 2010

Abstract. Relative humidity (RH) influences the water content of aerosol particles and therefore has an important impact on the particles' ability to scatter visible light. The RH dependence of the particle light scattering coefficient (σsp is therefore an important measure for climate forcing calculations. We built a humidification system for a nephelometer which allows the measurement of σsp at a defined RH in the range of 40–90%. This RH conditioner consists of a humidifier followed by a dryer, which enables us to measure the hysteresis behavior of deliquescent aerosol particles. In this paper we present the set-up of a new humidified nephelometer, a detailed characterization with well defined laboratory generated aerosols, and a first application in the field by comparing our instrument to another humidified nephelometer. Monodisperse ammonium sulfate and sodium chloride particles were measured at four different dry particle sizes. Agreement between measurement and prediction based on Mie theory was found for both σsp and f(RH)=σsp(RH)/σsp(dry) within the range of uncertainty. The two humidified nephelometers measuring at a rural site in the Black Forest (Germany) often detected different f(RH), probably caused by the aerosol hysteresis behavior: when the aerosol was metastable, therefore was scattering more light, only one instrument detected the higher f(RH).
A low power automated MAX-DOAS instrument for the Arctic and other remote unmanned locations
Authors: Carlson D. , Donohoue D. , Platt U. , Simpson W. R.
Published: April 2010

Abstract. Multiple Axis Differential Optical Absorption Spectrometer (MAX-DOAS) systems are inherently very simple instruments, which have been shown to provide extremely useful information about a wide variety of environmental parameters. In order to exploit the potential of the technique we have developed a new field-deployable, passive MAX-DOAS system that is automated and uses little power (<3 W). This new instrument utilizes a fully enclosed scan head that protects all moving parts and optics from harsh environments. Instrument diagnostics, such as tilt monitoring and frost accumulation detection and removal, are integrated into the main data acquisition program, which then acts to remedy problems that were discovered. This full automation and data quality checking make this instrument ideal for long-term deployment at remote, unmanned locations around the world, such as in polar regions or in the monitoring of trace gas emissions from volcanoes. This instrument was recently integrated into an ice-tethered autonomous buoy and tested in Elson Lagoon, near Barrow, Alaska to monitor halogen chemistry in the Arctic. During this investigation, differential slant column densities (dSCDs) of BrO up to 6×1014 molecules/cm2 were observed. Typical spectral fit residual RMS optical densities were less than 6×10−4 for solar zenith angles (SZA) <80° and a 6-min integration time. Here we describe the design concepts and performance of this new MAX-DOAS instrument through detailed analyses of spectral quality, power usage, possible instrument response biases, and typical instrument operations.
Determination of oceanic ozone deposition by ship-borne eddy covariance flux measurements
Authors: Bariteau L. , Helmig D. , Fairall C. W. , Hare J. E. , Hueber J. , Lang E. K.
Published: April 2010

Abstract. A fast response ozone analyzer based on the ozone-nitric oxide chemiluminescence method was integrated into the NOAA-ESRL flux system to achieve the first ship-borne, direct ozone flux measurements over the open ocean. Air was collected from an inlet at 18 m height over the ocean surface mounted to the bow-jackstaff and via a 30 m-long sampling line to the ozone instrument on the ship deck. A "puff" system was used for accurate and regular determination of the sample transport time (lag) between the inlet and the chemical analyzer. A Nafion-membrane dryer facilitated removal of fast water vapor fluctuations, which eliminated the need for quenching and density correction of the ozone signal. The sampling-analyzer system was found to have a ~0.25–0.40 s response time at a sensitivity of ~2800 counts s−1 per ppbv of ozone. Quality control and data filtering procedures for eliminating data that did not meet measurement requirements were critically evaluated. The new ozone flux system was deployed aboard the NOAA Ship Ronald H. Brown, and evaluated using results obtained during several research cruises off the coasts of the North and South America continents, yielding ozone deposition velocities (mean ± standard error) ranging from 0.009±0.001 cm s−1 to 0.24±0.020 cm s−1.
On the improvement of NO2 satellite retrievals – aerosol impact on the airmass factors
Authors: Leitão J. , Richter A. , Vrekoussis M. , Kokhanovsky A. , Zhang Q. J. , Beekmann M. , Burrows J. P.
Published: April 2010

Abstract. The accurate determination of nitrogen dioxide (NO2) tropospheric vertical columns from satellite measurements depends strongly on the airmass factor (AMF) used. A sensitivity study was performed with the radiative transfer model SCIATRAN to better understand the impact of aerosols on the calculation of NO2 AMFs. This influence was studied by varying the NO2 and aerosol vertical distributions, as well as physical and optical properties of the particles. In terms of aerosol definitions, the key factors for these calculations were identified as the relation between trace gas and aerosol vertical profiles, the optical depth of the aerosol layer, and single scattering albedo. In addition, surface albedo also has a large impact on the calculations. Overall it was found that particles mixed with the trace gas increases the measurements' sensitivity, but only when the aerosol is not very absorbing. The largest change, a factor of ~2 relative to the situation without aerosols, was found when a low layer of aerosol (600 m) was combined with a homogenous NO2 layer of 1.0 km. A layer of aerosol above the NO2 usually reduces the sensitivity of the satellite measurement. This situation is found mostly for runs with discrete elevated aerosol layers (representative for long-range transport) that can generate a decrease of the AMF values of up to 70%. The use of measured aerosol profiles and modelled NO2 resulted, generally, in much smaller changes of AMF relative to the pure Rayleigh case. Exceptions are some events of elevated layers with high aerosol optical depth that lead to a strong decrease of the AMF values. These results highlight the importance of aerosols in the retrieval of tropospheric NO2 columns from space and indicate the need for detailed information on aerosol properties and vertical distribution.
Water vapor δ2H and δ18O measurements using off-axis integrated cavity output spectroscopy
Authors: Sturm P. , Knohl A.
Published: April 2010

Abstract. We present a detailed assessment of a commercially available water vapor isotope analyzer (WVIA, Los Gatos Research, Inc.) for simultaneous in-situ measurements of δ2H and δ18O in water vapor. This method, based on off-axis integrated cavity output spectroscopy, is an alternative to the conventional water trap/isotope ratio mass spectrometry (IRMS) techniques. We evaluate the analyzer in terms of precision, memory effects, concentration dependence, temperature sensitivity and long-term stability. A calibration system based on a droplet generator is used to characterize the performance and to calibrate the analyzer. Our results show that the precision at an averaging time of 15 s is 0.16‰ for δ2H and 0.08‰ for δ18O. The isotope ratios are strongly dependent on the water mixing ratio of the air. Taking into account this concentration dependence as well as the temperature sensitivity of the instrument we obtained a long-term stability of the water isotope measurements of 0.38‰ for δ2H and 0.25‰ for δ18O. The accuracy of the WVIA was further assessed by comparative measurements using IRMS and a dew point generator indicating a linear response in isotopic composition and H2O concentrations. The WVIA combined with a calibration system provides accurate high resolution water vapor isotope measurements and opens new possibilities for hydrological and ecological applications.
Field inter-comparison of eleven atmospheric ammonia measurement techniques
Authors: von Bobrutzki K. , Braban C. F. , Famulari D. , Jones S. K. , Blackall T. , Smith T. E. L. , Blom M. , Coe H. , Gallagher M. , Ghalaieny M. , McGillen M. R. , Percival C. J. , Whitehead J. D. , Ellis R. , Murphy J. , Mohacsi A. , Pogany A. , Junninen H. , Rantanen S. , Sutton M. A. , Nemitz E.
Published: April 2010

Abstract. Eleven instruments for the measurement of ambient concentrations of atmospheric ammonia gas (NH3), based on eight different measurement methods were inter-compared above an intensively managed agricultural field in late summer 2008 in Southern Scotland. To test the instruments over a wide range of concentrations, the field was fertilised with urea midway through the experiment, leading to an increase in the average concentration from 10 to 100 ppbv. The instruments deployed included three wet-chemistry systems, one with offline analysis (annular rotating batch denuder, RBD) and two with online-analysis (Annular Denuder sampling with online Analysis, AMANDA; AiRRmonia), two Quantum Cascade Laser Absorption Spectrometers (a large-cell dual system; DUAL-QCLAS, and a compact system; c-QCLAS), two photo-acoustic spectrometers (WaSul-Flux; Nitrolux-100), a Cavity Ring Down Spectrosmeter (CRDS), a Chemical Ionisation Mass Spectrometer (CIMS), an ion mobility spectrometer (IMS) and an Open-Path Fourier Transform Infra-Red (OP-FTIR) Spectrometer. The instruments were compared with each other and with the average concentration of all instruments. An overall good agreement of hourly average concentrations between the instruments (R2>0.84), was observed for NH3 concentrations at the field of up to 120 ppbv with the slopes against the average ranging from 0.67 (DUAL-QCLAS) to 1.13 (AiRRmonia) with intercepts of −0.74 ppbv (RBD) to +2.69 ppbv (CIMS). More variability was found for performance for lower concentrations (<10 ppbv). Here the main factors affecting measurement precision are (a) the inlet design, (b) the state of inlet filters (where applicable), and (c) the quality of gas-phase standards (where applicable). By reference to the fast (1 Hz) instruments deployed during the study, it was possible to characterize the response times of the slower instruments.
The horizontal resolution of MIPAS
Authors: von Clarmann T. , De Clercq C. , Ridolfi M. , Höpfner M. , Lambert J.-C.
Published: April 2010

Abstract. Limb remote sensing from space provides atmospheric composition measurements at high vertical resolution while the information is smeared in the horizontal domain. The horizontal components of two-dimensional (altitude and along-track coordinate) averaging kernels of a limb retrieval constrained to horizontal homogeneity can be used to estimate the horizontal resolution of limb retrievals. This is useful for comparisons of measured data with modeled data, to construct horizontal observation operators in data assimilation applications or when measurements of different horizontal resolution are intercompared. We present these averaging kernels for retrievals of temperature, H2O, O3, CH4, N2O, HNO3 and NO2 from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) high-resolution limb emission spectra. The horizontal smearing of a MIPAS retrieval in terms of full width at half maximum of the rows of the horizontal averaging kernel matrix varies typically between about 200 and 350 km for most species, altitudes and atmospheric conditions. The range where 95% of the information originates from varies from about 260 to 440 km for these cases. This information spread is smaller than the MIPAS horizontal sampling, i.e. MIPAS data are horizontally undersampled, and the effective horizontal resolution is driven by the sampling rather than the smearing. The point where the majority of the information originates from is displaced from the tangent point towards the satellite by typically less than 10 km for trace gas profiles and about 50 to 100 km for temperature, with a few exceptions for uppermost altitudes. The geolocation of a MIPAS profile is defined as the tangent point of the middle line of sight in a MIPAS limb scan. The majority of the information displacement with respect to this nominal geolocation of the measurement is caused by the satellite movement and the geometrical displacement of the actual tangent point as a function of the elevation angle. In none of the cases investigated, propagation of the horizontal smoothing on the vertical profile shape has been observed.
Experimental characterization of the COndensation PArticle counting System for high altitude aircraft-borne application
Authors: Weigel R. , Hermann M. , Curtius J. , Voigt C. , Walter S. , Böttger T. , Lepukhov B. , Belyaev G. , Borrmann S.
Published: April 2010

Abstract. This study aims at a detailed characterization of an ultra-fine aerosol particle counting system for operation on board the Russian high altitude research aircraft M-55 "Geophysica" (maximum ceiling of 21 km). The COndensation PArticle counting Systems (COPAS) consists of an aerosol inlet and two dual-channel continuous flow Condensation Particle Counters (CPCs). The aerosol inlet, adapted for COPAS measurements on board the M-55 "Geophysica", is described concerning aspiration, transmission, and transport losses. The counting efficiencies of the CPCs using the chlorofluorocarbon FC-43 as the working fluid are studied experimentally at two pressure conditions, 300 hPa and 70 hPa. Three COPAS channels are operated with different temperature differences between the saturator and the condenser block yielding smallest detectable particle sizes (dp50 – as 50% detection "cut off" diameters) of 6 nm, 11 nm, and 15 nm, respectively, at ambient pressure of 70 hPa. The fourth COPAS channel is operated with an aerosol heating line (250°C) for a determination of the non-volatile number of particles. The heating line is experimentally proven to volatilize pure H2SO4-H2O particles for a particle diameter (dp) range of 11 nm<dp<200 nm. Additionally this study includes investigation to exclude auto-nucleation of the working fluid inside the CPCs. An instrumental inter-comparison (cross-correlation) has been performed for several measurement flights and mission flights in the Arctic and the Tropics are discussed. Finally, COPAS measurements are used for an aircraft plume crossing analysis.
Multi-year comparison of stratospheric BrO vertical profiles retrieved from SCIAMACHY limb and ground-based UV-visible measurements
Authors: Hendrick F. , Rozanov A. , Johnston P. V. , Bovensmann H. , De Mazière M. , Fayt C. , Hermans C. , Kreher K. , Lotz W. , Sinnhuber B.-M. , Theys N. , Thomas A. , Burrows J. P. , Van Roozendael M.
Published: April 2010

Abstract. Vertical profiles of stratospheric bromine monoxide (BrO) daily retrieved from ENVISAT/SCIAMACHY (ENVIronmental SATellite/SCanning Imaging Absorption spectrometer for Atmospheric CHartographY) limb scatter data and from ground-based UV-visible observations performed at Harestua (60° N, 11° E), Observatoire de Haute-Provence (44° N, 5.5° E), and Lauder (45° S, 170° E) are compared in the 15–27 km altitude range for the period from 2002 until 2006. At the three stations, the SCIAMACHY and ground-based UV-visible profiles agree reasonably well, with relative difference smaller than 23% on average. When comparing the BrO partial columns, the agreement obtained is good, with mean relative differences smaller than 11% and corresponding standard deviations in the 13–19% range. The seasonal variation of the BrO columns at the three stations is consistently captured by both retrievals as well as large BrO column events occurring during the winter and early spring at Harestua which are associated with chlorine activation.
Development of an H-TDMA for long-term unattended measurement of the hygroscopic properties of atmospheric aerosol particles
Authors: Nilsson E. , Swietlicki E. , Sjogren S. , Löndahl J. , Nyman M. , Svenningsson B.
Published: April 2010

Abstract. A new hygroscopic tandem differential mobility analyzer (H-TDMA) has been constructed at Lund University within the frameworks of the EU FP6 Infrastructure Project EUSAAR (http://www.eusaar.org/). The aim of this coordinated H-TDMA development is to design and evaluate a new generation of H-TDMAs that are capable of conducting long term measurements of the hygroscopic growth and state of mixing of sub-micrometer atmospheric aerosol particles at the EUSAAR aerosol super-sites across Europe. The H-TDMA constructed for this project has been validated with respect to hygroscopic growth factor, stability of relative humidity (RH), temperature stability and its ability to operate unattended for longer periods of time. When measuring growth factors of ammonium sulphate, the new H-TDMA system was found to measure within a growth factor deviation of ±0.05 compared to previously recorded data by Tang et al. (1994). The long term RH of the system has been found stable at 90.0% with a standard deviation of ±0.23% and an average temperature variability of the second DMA less than ±0.1 K. Daily automated ammonium sulphate measurements have validated the ambient measurements. The instrument is operated at the EMEP/EUSAAR background station Vavihill in the southern part of Sweden.
A single gas chromatograph for accurate atmospheric mixing ratio measurements of CO2, CH4, N2O, SF6 and CO
Authors: van der Laan S. , Neubert R. E. M. , Meijer H. A. J.
Published: April 2010

Abstract. We present an adapted gas chromatograph capable of measuring simultaneously and semi-continuously the atmospheric mixing ratios of the greenhouse gases CO2, CH4, N2O and SF6 and the trace gas CO with high precision and long-term stability. The novelty of our design is that all species are measured with only one device, making it a very cost-efficient system. No time lags are introduced between the measured mixing ratios. The system is designed to operate fully autonomously which makes it ideal for measurements at remote and unmanned stations. Only a small amount of sample air is needed, which makes this system also highly suitable for flask air measurements. In principle, only two reference cylinders are needed for daily operation and only one calibration per year against international WMO standards is sufficient to obtain high measurement precision and accuracy. The system described in this paper is in use since May 2006 at our atmospheric measurement site Lutjewad near Groningen, The Netherlands at 6°21' E, 53°24' N, 1 m a.s.l. Results show the long-term stability of the system. Observed measurement precisions at our remote research station Lutjewad were: ±0.04 ppm for CO2, ±0.8 ppb for CH4, ±0.8 ppb for CO, ±0.3 ppb for N2O, and ±0.1 ppt for SF6. The ambient mixing ratios of all measured species as observed at station Lutjewad for the period of May 2007 to August 2008 are presented as well.
Uncertainty analysis of computational methods for deriving sensible heat flux values from scintillometer measurements
Authors: Solignac P. A. , Brut A. , Selves J.-L. , Béteille J.-P. , Gastellu-Etchegorry J.-P. , Keravec P. , Béziat P. , Ceschia E.
Published: April 2010

Abstract. The use of scintillometers to determine sensible heat fluxes is now common in studies of land-atmosphere interactions. The main interest in these instruments is due to their ability to quantify energy distributions at the landscape scale, as they can calculate sensible heat flux values over long distances, in contrast to Eddy Correlation systems. However, scintillometer data do not provide a direct measure of sensible heat flux, but require additional data, such as the Bowen ratio (β), to provide flux values. The Bowen ratio can either be measured using Eddy Correlation systems or derived from the energy balance closure. In this work, specific requirements for estimating energy fluxes using a scintillometer were analyzed, as well as the accuracy of two flux calculation methods. We first focused on the classical method (used in standard software). We analysed the impact of the Bowen ratio according to both time averaging and ratio values; for instance, an averaged Bowen ratio (β) of less than 1 proved to be a significant source of measurement uncertainty. An alternative method, called the "β-closure method", for which the Bowen ratio measurement is not necessary, was also tested. In this case, it was observed that even for low β values, flux uncertainties were reduced and scintillometer data were well correlated with the Eddy Correlation results.
A new thermal gradient ice nucleation diffusion chamber instrument: design, development and first results using Saharan mineral dust
Authors: Kulkarni G. , Dobbie S. , McQuaid J.
Published: April 2010

Abstract. A new Thermal Gradient ice nucleation Diffusion Chamber (TGDC) capable of investigating ice nucleation efficiency of atmospherically important aerosols, termed Ice Nuclei (IN), has been designed, constructed and validated. The TGDC can produce a range of supersaturations with respect to ice (SSi) over the temperature range of −10 to −34°C for sufficiently long time needed to observe the ice nucleation by the aerosol particles. The novel aspect of this new TGDC is that the chamber is run in static mode with aerosol particles supported on a Teflon substrate, which can be raised and lowered in a controlled way through the SSi profile within the chamber, and nucleation events are directly observed using digital photography. The TGDC consists of two ice coated plates to which a thermal gradient is applied to produce the range of SSi. The design of the TGDC gives the ability to understand time-related ice nucleation event information and to perform experiments at different temperatures and SSi conditions for different IN without changing the thermal gradient within the TGDC. The temperature and SSi conditions of the experimental system are validated by observing (NH4)2SO4 deliquescence and the results are in good agreement with the literature data. First results are presented of the onset ice nucleation for mineral dust sampled from the Saharan Desert, including images of nucleation and statistical distributions of onset ice nucleation SSi as a function of temperature. This paper illustrates how useful this new TGDC is for process level studies of ice nucleation and more experimental investigations are needed to better quantify the role of ice formation in the atmosphere.
A method for real-time profiling of organic trace gases in the planetary boundary layer
Authors: Schnitzhofer R. , Wisthaler A. , Hansel A.
Published: April 2010

Abstract. A method for real time profiling of volatile organic compounds (VOCs) was developed combining the advantages of a tethered balloon as a research platform and of proton transfer reaction mass spectrometry (PTR-MS) as an analytical technique for fast and highly sensitive VOC measurements. A 200 m Teflon tube was used to draw sampling air from a tethered aerodynamic balloon to the PTR-MS instrument. Potential positive and negative VOC artifacts of the inlet line were characterized in the laboratory and in the field and were found to be insignificant for most compounds. The method was successfully deployed during a winter field campaign to determine the small scale spatial and temporal pattern of air pollutants under winter inversion conditions.