bluuebunny/crossref_metadata_2025_split huggingface dataset:
Investigations of boundary layer structure, cloud characteristics and vertical mixing of aerosols at Barbados with large eddy simulations
Authors: Jähn M. , Muñoz-Esparza D. , Chouza F. , Reitebuch O. , Knoth O. , Haarig M. , Ansmann A. 
Published: January 2016

Abstract. Large eddy simulations (LESs) are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. Due to the presence of a topographically structured island surface in the domain center, the model setup has to be designed with open lateral boundaries. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, we use the cell perturbation method based on finite amplitude potential temperature perturbations. In this work, this method is for the first time tested and validated for moist boundary layer simulations with open lateral boundary conditions. Observational data obtained from the SALTRACE field campaign is used for both model initialization and a comparison with Doppler wind and Raman lidar data. Several numerical sensitivity tests are carried out to demonstrate the problems related to “gray zone modeling” when using coarser spatial grid spacings beyond the inertial subrange of three-dimensional turbulence or when the turbulent marine boundary layer flow is replaced by laminar winds. Especially cloud properties in the downwind area west of Barbados are markedly affected in these kinds of simulations. Results of an additional simulation with a strong trade-wind inversion reveal its effect on cloud layer depth and location. Saharan dust layers that reach Barbados via long-range transport over the North Atlantic are included as passive tracers in the model. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom at z ≈ 1800 m become apparent. The exact position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability (especially inversion strength) and wind shear. Comparisons of LES model output with wind lidar data show similarities in the downwind vertical wind structure. Additionally, the model results accurately reproduce the development of the daytime convective boundary layer measured by the Raman lidar.
Solubility and reactivity of HNCO in water: insights into HNCO's fate in the atmosphere
Authors: Borduas N. , Place B. , Wentworth G. R. , Abbatt J. P. D. , Murphy J. G. 
Published: January 2016

Abstract. A growing number of ambient measurements of isocyanic acid (HNCO) are being made, yet little is known about its fate in the atmosphere. To better understand HNCO's loss processes and particularly its atmospheric partitioning behaviour, we measure its effective Henry's Law coefficient KHeff with a bubbler experiment using chemical ionization mass spectrometry as the gas phase analytical technique. By conducting experiments at different pH values and temperature, a Henry's Law coefficient KH of 26 ± 2 M atm−1 is obtained, with an enthalpy of dissolution of −34 ± 2 kJ mol−1, which translates to a KHeff of 31 M atm−1 at 298 K and at pH 3. Our approach also allows for the determination of HNCO's acid dissociation constant, which we determine to be Ka = 2.1 ± 0.2  ×  10−4 M at 298 K. Furthermore, by using ion chromatography to analyze aqueous solution composition, we revisit the hydrolysis kinetics of HNCO at different pH and temperature conditions. Three pH-dependent hydrolysis mechanisms are in play and we determine the Arrhenius expressions for each rate to be k1 = (4.4 ± 0.2)  ×  107 exp(−6000 ± 240∕T) M s−1, k2 = (8.9 ± 0.9)  ×  106  exp(−6770 ± 450∕T) s−1 and k3 =  (7.2 ± 1.5)  ×  108 exp(−10 900 ± 1400∕T) s−1, where k1 is for HNCO + H++ H2O  →  NH4++ CO2, k2 is for HNCO + H2O  →  NH3 + CO2 and k3 is for NCO−+ 2 H2O  →  NH3+ HCO3−. HNCO's lifetime against hydrolysis is therefore estimated to be 10 days to 28 years at pH values, liquid water contents, and temperatures relevant to tropospheric clouds, years in oceans and months in human blood. In all, a better parameterized Henry's Law coefficient and hydrolysis rates of HNCO allow for more accurate predictions of its concentration in the atmosphere and consequently help define exposure of this toxic molecule.
Impact of vehicular emissions on the formation of fine particles in the Sao Paulo Metropolitan Area: a numerical study with the WRF-Chem model
Authors: Vara-Vela A , Andrade M. F. , Kumar P. , Ynoue R. Y. , Muñoz A. G. 
Published: January 2016

Abstract. The objective of this work is to evaluate the impact of vehicular emissions on the formation of fine particles (PM2.5;  ≤  2.5 µm in diameter) in the Sao Paulo Metropolitan Area (SPMA) in Brazil, where ethanol is used intensively as a fuel in road vehicles. The Weather Research and Forecasting with Chemistry (WRF-Chem) model, which simulates feedbacks between meteorological variables and chemical species, is used as a photochemical modelling tool to describe the physico-chemical processes leading to the evolution of number and mass size distribution of particles through gas-to-particle conversion. A vehicular emission model based on statistical information of vehicular activity is applied to simulate vehicular emissions over the studied area. The simulation has been performed for a 1-month period (7 August–6 September 2012) to cover the availability of experimental data from the NUANCE-SPS (Narrowing the Uncertainties on Aerosol and Climate Changes in Sao Paulo State) project that aims to characterize emissions of atmospheric aerosols in the SPMA. The availability of experimental measurements of atmospheric aerosols and the application of the WRF-Chem model made it possible to represent some of the most important properties of fine particles in the SPMA such as the mass size distribution and chemical composition, besides allowing us to evaluate its formation potential through the gas-to-particle conversion processes. Results show that the emission of primary gases, mostly from vehicles, led to a production of secondary particles between 20 and 30 % in relation to the total mass concentration of PM2.5 in the downtown SPMA. Each of PM2.5 and primary natural aerosol (dust and sea salt) contributed with 40–50 % of the total PM10 (i.e. those  ≤  10 µm in diameter) concentration. Over 40 % of the formation of fine particles, by mass, was due to the emission of hydrocarbons, mainly aromatics. Furthermore, an increase in the number of small particles impaired the ultraviolet radiation and induced a decrease in ozone formation. The ground-level O3 concentration decreased by about 2 % when the aerosol-radiation feedback is taken into account.
Influence of the ambient humidity on the concentration of natural deposition-mode ice-nucleating particles
Authors: López M. L. , Ávila E. E. 
Published: January 2016

Abstract. This study reports measurements of deposition-mode ice-nucleating particle (INP) concentrations at ground level during the period July–December 2014 in Córdoba, Argentina. Ambient air was sampled into a cloud chamber where the INP concentration was measured at a temperature of −25 °C and a 15 % supersaturation over ice. Measurements were performed on days with different thermodynamic conditions, including rainy days. The effect of the relative humidity at ground level (RHamb) on the INP concentration was analyzed. The number of INPs activated varied from 1 L−1 at RHamb of 25 % to 30 L−1 at RHamb of 90 %. In general, a linear trend between the INP concentration and the RHamb was found, suggesting that this variability must be related to the effectiveness of the aerosols acting as INPs. From the backward trajectories analysis, it was found that the link between INP concentration and RHamb is independent of the origin of the air masses. The role of biological INPs and nucleation occurring in pores and cavities was discussed as a possible mechanism to explain the increase of the INP concentration during high ambient relative humidity events. This work provides valuable measurements of deposition-mode INP concentrations from the Southern Hemisphere where INP data are sparse so far.
Inverse modeling of black carbon emissions over China using ensemble data assimilation
Authors: Wang P. , Wang H. , Wang Y. Q. , Zhang X. Y. , Gong S. L. , Xue M. , Zhou C. H. , Liu H. L. , An X. Q. , Niu T. , Cheng Y. L. 
Published: January 2016

Abstract. Emissions inventories of black carbon (BC), which are traditionally constructed using a bottom-up approach based on activity data and emissions factors, are considered to contain a large level of uncertainty. In this paper, an ensemble optimal interpolation (EnOI) data assimilation technique is used to investigate the possibility of optimally recovering the spatially resolved emissions bias of BC. An inverse modeling system for emissions is established for an atmospheric chemistry aerosol model and two key problems related to ensemble data assimilation in the top-down emissions estimation are discussed: (1) how to obtain reasonable ensembles of prior emissions and (2) establishing a scheme to localize the background-error matrix. An experiment involving 1-year-long simulation cycle with EnOI inversion of BC emissions is performed for 2008. The bias of the BC emissions intensity in China at each grid point is corrected by this inverse system. The inverse emission over China in January is 240.1 Gg, and annual emission is about 2539.3 Gg, which is about 1.8 times of bottom-up emission inventory. The results show that, even though only monthly mean BC measurements are employed to inverse the emissions, the accuracy of the daily model simulation improves. Using top-down emissions, the average root mean square error of simulated daily BC is decreased by nearly 30 %. These results are valuable and promising for a better understanding of aerosol emissions and distributions, as well as aerosol forecasting.
Sensitivity of thermal infrared nadir instruments to the chemical and microphysical properties of UTLS secondary sulfate aerosols
Authors: Sellitto P. , Legras B. 
Published: January 2016

Abstract. Monitoring upper-tropospheric–lower-stratospheric (UTLS) secondary sulfate aerosols and their chemical and microphysical properties from satellite nadir observations is crucial to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Here we present a study aimed at the evaluation of the sensitivity of thermal infrared (TIR) satellite nadir observations to the chemical composition and the size distribution of idealised UTLS sulfate aerosol layers. The extinction properties of sulfuric acid/water droplets, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. IASI (Infrared Atmospheric Sounding Interferometer) pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on the brightness temperature spectra observed by this satellite instrument. We found a marked and typical spectral signature of these aerosol layers between 700 and 1200 cm−1, due to the absorption bands of the sulfate and bisulfate ions and the undissociated sulfuric acid, with the main absorption peaks at 1170 and 905 cm−1. The dependence of the aerosol spectral signature to the sulfuric acid mixing ratio, and effective number concentration and radius, as well as the role of interfering parameters like the ozone, sulfur dioxide, carbon dioxide and ash absorption, and temperature and water vapour profile uncertainties, are analysed and critically discussed. The information content (degrees of freedom and retrieval uncertainties) of synthetic satellite observations is estimated for different instrumental configurations. High spectral resolution (IASI-like pseudo-observations) and broadband spectral features (Moderate Resolution Imaging Spectroradiometer (MODIS) and Spinning Enhanced Visible and InfraRed Imager (SEVIRI)-like pseudo-observations) approaches are proposed and discussed.
UTLS water vapour from SCIAMACHY limb measurementsV3.01 (2002–2012)
Authors: Weigel K. , Rozanov A. , Azam F. , Bramstedt K. , Damadeo R. , Eichmann K.-U. , Gebhardt C. , Hurst D. , Kraemer M. , Lossow S. , Read W. , Spelten N. , Stiller G. P. , Walker K. A. , Weber M. , Bovensmann H. , Burrows J. P. 
Published: January 2016

Abstract. The SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) aboard the Envisat satellite provided measurements from August 2002 until April 2012. SCIAMACHY measured the scattered or direct sunlight using different observation geometries. The limb viewing geometry allows the retrieval of water vapour at about 10–25 km height from the near-infrared spectral range (1353–1410 nm). These data cover the upper troposphere and lower stratosphere (UTLS), a region in the atmosphere which is of special interest for a variety of dynamical and chemical processes as well as for the radiative forcing. Here, the latest data version of water vapour (V3.01) from SCIAMACHY limb measurements is presented and validated by comparisons with data sets from other satellite and in situ measurements. Considering retrieval tests and the results of these comparisons, the V3.01 data are reliable from about 11 to 23 km and the best results are found in the middle of the profiles between about 14 and 20 km. Above 20 km in the extra tropics V3.01 is drier than all other data sets. Additionally, for altitudes above about 19 km, the vertical resolution of the retrieved profile is not sufficient to resolve signals with a short vertical structure like the tape recorder. Below 14 km, SCIAMACHY water vapour V3.01 is wetter than most collocated data sets, but the high variability of water vapour in the troposphere complicates the comparison. For 14–20 km height, the expected errors from the retrieval and simulations and the mean differences to collocated data sets are usually smaller than 10 % when the resolution of the SCIAMACHY data is taken into account. In general, the temporal changes agree well with collocated data sets except for the Northern Hemisphere extratropical stratosphere, where larger differences are observed. This indicates a possible drift in V3.01 most probably caused by the incomplete treatment of volcanic aerosols in the retrieval. In all other regions a good temporal stability is shown. In the tropical stratosphere an increase in water vapour is found between 2002 and 2012, which is in agreement with other satellite data sets for overlapping time periods.
An automated gas chromatography time-of-flight mass spectrometry instrument for the quantitative analysis of halocarbons in air
Authors: Obersteiner F. , Bönisch H. , Engel A. 
Published: January 2016

Abstract. We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument (GC-TOFMS) for the quantitative analysis of halocarbons in air samples. The setup comprises three fundamental enhancements compared to our earlier work (Hoker et al., 2015): (1) full automation, (2) a mass resolving power R = m/Δm of the TOFMS (Tofwerk AG, Switzerland) increased up to 4000 and (3) a fully accessible data format of the mass spectrometric data. Automation in combination with the accessible data allowed an in-depth characterization of the instrument. Mass accuracy was found to be approximately 5 ppm in mean after automatic recalibration of the mass axis in each measurement. A TOFMS configuration giving R = 3500 was chosen to provide an R-to-sensitivity ratio suitable for our purpose. Calculated detection limits are as low as a few femtograms by means of the accurate mass information. The precision for substance quantification was 0.15 % at the best for an individual measurement and in general mainly determined by the signal-to-noise ratio of the chromatographic peak. Detector non-linearity was found to be insignificant up to a mixing ratio of roughly 150 ppt at 0.5 L sampled volume. At higher concentrations, non-linearities of a few percent were observed (precision level: 0.2 %) but could be attributed to a potential source within the detection system. A straightforward correction for those non-linearities was applied in data processing, again by exploiting the accurate mass information. Based on the overall characterization results, the GC-TOFMS instrument was found to be very well suited for the task of quantitative halocarbon trace gas observation and a big step forward compared to scanning, quadrupole MS with low mass resolving power and a TOFMS technique reported to be non-linear and restricted by a small dynamical range.
Carbon monoxide total columns from SCIAMACHY 2.3  µm atmospheric reflectance measurements: towards a full-mission data product (2003–2012)
Authors: Borsdorff T. , Tol P. , Williams J. E. , de Laat J. , aan de Brugh J. , Nédélec P. , Aben I. , Landgraf J. 
Published: January 2016

Abstract. We present a full-mission data product of carbon monoxide (CO) vertical column densities using the 2310–2338 nm SCIAMACHY reflectance measurements over clear-sky land scenes for the period January 2003–April 2012. The retrieval employs the SICOR algorithm, which will be used for operational data processing of the Sentinel-5 Precursor mission. The retrieval approach infers simultaneously carbon monoxide, methane and water vapour column densities together with a Lambertian surface albedo from individual SCIAMACHY measurements employing a non-scattering radiative transfer model. To account for the radiometric instrument degradation including the formation of an ice-layer on the 2.3 µm detector array, we consider clear-sky measurements over the Sahara as a natural calibration target. For these specific measurements, we spectrally calibrate the SCIAMACHY measurements and determine a spectral radiometric offset and the width of the instrument spectral response function as a function of time for the entire operational phase of the mission. We show that the smoothing error of individual clear-sky CO retrievals is less than ±1 ppb and thus this error contribution does not need to be accounted for in the validation considering the much higher retrieval noise. The CO data product is validated against measurements of ground-based Fourier transform infrared spectrometers at 27 stations of the NDACC-IRWG and TCCON network and MOZAIC/IAGOS aircraft measurements at 26 airports worldwide. Overall, we find a good agreement with TCCON measurements with a mean bias b  = −1.2 ppb and a station-to-station bias with σ   = 7.2 ppb. The negative sign of the bias means a low bias of SCIAMACHY CO with respect to TCCON. For the NDACC-IRWG network, we obtain a larger mean station bias of b  = −9.2 ppb with σ  = 8.1 ppb and for the MOZAIC/IAGOS measurements we find b  = −6.4 ppb with σ  = 5.6 ppb. The SCIAMACHY data set is subject to a small but significant bias trend of 1.47 ± 0.25 ppb yr−1. After trend correction, the bias with respect to MOZAIC/IAGOS observation is 2.5 ppb, with respect to TCCON measurements it is −4.6 ppb and with respect to NDACC-IRWG measurements −8.4 ppb. Hence, a discrepancy of 3.8 ppb remains between the global biases with NDACC-IRWG and TCCON, which is confirmed by directly comparing NDACC-IRWG and TCCON measurements. Generally, the scatter of the individual SCIAMACHY CO retrievals is high and dominated by large measurement noise. Hence, for practical usage of the data set, averaging of individual retrievals is required. As an example, we show that monthly mean SCIAMACHY CO retrievals, averaged separately over Northern and Southern Africa, reflect the spatial and temporal variability of biomass burning events in agreement with the global chemical transport model TM5.
Comparison of GOME-2/Metop-A ozone profiles with GOMOS, OSIRIS and MLS measurements
Authors: Kauppi A. , Tuinder O. N. E. , Tukiainen S. , Sofieva V. , Tamminen J. 
Published: January 2016

Abstract. This paper presents a comparison of vertical ozone profiles retrieved by the Ozone ProfilE Retrieval Algorithm (OPERA) (versions 1.14–1.24) from the Global Ozone Monitoring Experiment-2 (GOME-2) measurements on board the Meteorological operational Metop-A satellite with spaceborne high-vertical-resolution ozone profiles by Global Ozone Monitoring by Occultation of Stars (GOMOS), Optical Spectrograph and Infrared Imager System (OSIRIS) and Microwave Limb Sounder (MLS). The comparison, with global coverage, focuses on the stratosphere and the lower mesosphere and covers the period from March 2008 until the end of 2011. The comparison shows an agreement of GOME-2 ozone profiles with those of GOMOS, OSIRIS and MLS within ±15 % in the altitude range from 15 km up to  ∼ 35–40 km depending on latitude. The GOME-2 bias with respect to the reference instruments depends on season, with the strongest dependence observed at high latitudes. The GOME-2 ozone profiles retrieved from non-degradation corrected radiances have a tendency to a systematic negative bias with respect to the reference data above  ∼ 30 km. We have studied the influence of solar zenith angle and the effect of instrumental degradation correction. In addition, we have studied GOME-2 performance in Arctic ozone depletion case and demonstrated that GOME-2 data provide valuable information about ozone profiles.
Characterization of downwelling radiance measured from a ground-based microwave radiometer using numerical weather prediction model data
Authors: Ahn M.-H. , Won H. Y. , Han D. , Kim Y.-H. , Ha J.-C. 
Published: January 2016

Abstract. The ground-based microwave sounding radiometers installed at nine weather stations of Korea Meteorological Administration alongside with the wind profilers have been operating for more than 4 years. Here we apply a process to assess the characteristics of the observation data by comparing the measured brightness temperature (Tb) with reference data. For the current study, the reference data are prepared by the radiative transfer simulation with the temperature and humidity profiles from the numerical weather prediction model instead of the conventional radiosonde data. Based on the 3 years of data, from 2010 to 2012, we were able to characterize the effects of the absolute calibration on the quality of the measured Tb. We also showed that when clouds are present the comparison with the model has a high variability due to presence of cloud liquid water therefore making cloudy data not suitable for assessment of the radiometer's performance. Finally we showed that differences between modeled and measured brightness temperatures are unlikely due to a shift in the selection of the center frequency but more likely due to spectroscopy issues in the wings of the 60 GHz absorption band. With a proper consideration of data affected by these two effects, it is shown that there is an excellent agreement between the measured and simulated Tb. The regression coefficients are better than 0.97 along with the bias value of better than 1.0 K except for the 52.28 GHz channel which shows a rather large bias and variability of −2.6 and 1.8 K, respectively.