Items

Advanced search

Source attributions of pollution to the Western Arctic during the NASA ARCTAS field campaign

We use the NASA GEOS-5 transport model with tagged tracers to investigate the contributions of different regional sources of CO and black carbon (BC) to their concentrations in the Western Arctic (i.e., 50–90° N and 190–320° E) in spring and summer 2008. The model is evaluated by comparing the results with airborne measurements of CO and BC from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaigns to demonstrate the strengths and limitations of our simulations. We also examine the reliability of tagged CO tracers in characterizing air mass origins using the measured fossil fuel tracer of dichloromethane and the biomass burning tracer of acetonitrile. Our tagged CO simulations suggest that most of the enhanced CO concentrations (above background level from CH4 production) observed during April originate from Asian anthropogenic emissions. Boreal biomass burning emissions and Asian anthropogenic emissions are of similar importance in July domain wise, although the biomass burning CO fraction is much larger in the area of the ARCTAS field experiments. The fraction of CO from Asian anthropogenic emissions is larger in spring than in summer. European sources make up no more than 10% of CO levels in the campaign domain during either period. Comparisons of CO concentrations along the flight tracks with regional averages from GEOS-5 show that the along-track measurements are representative of the concentrations within the large domain of the Western Arctic in April but not in July.
How much CO was emitted by the 2010 fires around Moscow?

The fires around Moscow in July and August 2010 emitted a large amount of pollutants to the atmosphere. Here we estimate the carbon monoxide (CO) source strength of the Moscow fires in July and August by using the TM5-4DVAR system in combination with CO column observations of the Infrared Atmospheric Sounding Interferometer (IASI). It is shown that the IASI observations provide a strong constraint on the total emissions needed in the model. Irrespective of the prior emissions used, the optimised CO fire emission estimates from mid-July to mid-August 2010 amount to approximately 24 Tg CO. This estimate depends only weakly (< 15%) on the assumed diurnal variations and injection height of the emissions. However, the estimated emissions might depend on unaccounted model uncertainties such as vertical transport. Our emission estimate of 22–27 Tg CO during roughly one month of intense burning is less than suggested by another recent study, but substantially larger than predicted by the bottom-up inventories. This latter discrepancy suggests that bottom-up emission estimates for extreme peat burning events require improvements.
Mixing state of individual submicron carbon-containing particles during spring and fall seasons in urban Guangzhou, China: a case study

Growing evidence suggests that the size-resolved mixing state of carbon-containing particles is very critical in determining their optical properties, atmospheric lifetime, and impact on the environment. However, still little is known about the mixing state of particles in the urban area of the Pearl River Delta (PRD) region, China. To investigate the mixing state of submicron carbon-containing particles, measurements were carried out during spring and fall periods of 2010 using a single-particle aerosol mass spectrometer (SPAMS). Approximately 700 000 particles for each period were detected. This is the first report on the size-resolved mixing state of carbon-containing particles by direct observations in the PRD region. Cluster analysis of single-particle mass spectra was applied to identify carbon-containing particle classes. These classes represented ~80% and ~90% of all the detected particles for spring and fall periods, respectively. Carbon-containing particle classes mainly consisted of biomass/biofuel burning particles (Biomass), organic carbon (OC), fresh elemental carbon (EC-fresh), internally mixed OC and EC (ECOC), internally mixed EC with sulfate (EC-Sulfate), vanadium-containing ECOC (V-ECOC), and amines-containing particles (Amine). In spring, the top three ranked carbon-containing particle classes were ECOC (26.1%), Biomass (23.6%) and OC (10%), respectively. However, the fraction of Biomass particles increased remarkably and predominated (61.0%), while the fraction of ECOC (3.0%) and V-ECOC (0.1%) significantly decreased in fall. To highlight the influence of monsoon on the properties of carbon-containing particles in urban Guangzhou, their size distributions, mixing state, and aerosol acidity were compared between spring and fall seasons. In addition, a case study was also performed to investigate how the formation of fog and haze influenced the mixing state of carbon-containing particles. These results could improve our understanding of the mixing state of carbon-containing particles, and may also be helpful in modeling the climate forcing of aerosol in the PRD region.
Aerosol size-resolved trace metal composition in remote northern tropical Atlantic marine environment: case study Cape Verde islands

Size-resolved trace metal concentrations of 15 elements in aerosol particles at the Cape Verde Atmospheric Observatory (CVAO) under remote background conditions were investigated through analysis of aerosol samples collected during intensive field studies from January 2007 to November 2011 using total reflection x-ray fluorescence (TXRF). The identification of the main air mass origin that influence remote marine aerosol in the northern tropical Atlantic has been investigated. In total, 317 samples were collected. The dataset was analyzed according to the main air mass inflow at the station. We found that remote conditions make up about 45% of the meteorological conditions in a year at CVAO and thus the northern tropical Atlantic. Surprisingly, air masses from North America are often responsible for higher trace metal concentrations in this region. Elements such as Zn, Pb, Cu, Cr, Ni, and V were mostly found in the submicron size fractions, while elements with dominant crustal or oceanic origin such as Fe, Ti, Mn, Sr, and Rb were found in the coarse fractions (>1 μm). The highest metal concentrations, especially for Zn (3.23 ng m−3), Cu (0.81 ng m−3), Sr (2.63 ng m−3), and Cr (0.53 ng m−3), were observed in air masses originating from North America and the concentrations were within the same concentration range to those reported previously in the literature for remote marine aerosols. Fe (12.26 ng m−3), Ti (0.91 ng m−3), and Mn (0.35 ng m−3) showed higher concentrations when air mass came from Europe and the Canary Islands. Pb concentration was low (<0.20 ng m−3) and did not vary significantly with air mass direction. The low Pb concentration is indicative of the complete phase-out of leaded gasoline even in African countries. Crustal enrichment factor values decreased from fine to coarse-mode particles with low values (<4) observed for Fe, Mn, and Rb, and high values (>20) for Zn, Cu, Ni, Cr, Pb, and Se. The observed enrichment of the elements was attributed to crustal, marine, anthropogenic, and biogenic sources, as well as long-range transport and resuspension. Zn, Cu and Pb were indicators of anthropogenic activities, while Ti and Sr were indicators of crustal and marine origin, respectively. Oceanic and biogenic emissions might have contributed to most of the Se observed. This work provides the first long-term size-resolved trace metals study for remote tropical northern Atlantic marine aerosols and the dataset could serve as good initiation of yearly flux estimates.
Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

Primary marine aerosols (PMAs) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw) range between −1°C and 15°C. A sharp decrease in PMA emissions for a Tw increase from −1°C to 4°C was followed by a lower rate of change in PMA emissions for Tw up to about 6°C. Near constant number concentrations for water temperatures between 6°C to 10°C and higher were recorded. Even though the total particle number concentration changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (Dp< 0.125μm measured during winter conditions were similar (deviation of up to 3%), or lower (up to 70%) than the ones measured during summer conditions (for the same water temperature range). For Dp > 0.125μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1°C to 10°C during winter measurements showed a decrease in the peak of relative particle number concentration at about a Dp of 0.180μm, while an increase was observed for particles with Dp > 1μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range 7–11°C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (for example sea ice production in winter and increased glacial meltwater inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.
Systematic investigation of bromine monoxide in volcanic plumes from space by using the GOME-2 instrument

During recent years, volcanic emissions turned out to be a natural source of bromine compounds in the atmosphere. While the initial formation process of bromine monoxide (BrO) has been successfully studied in local ground-based measurements at quiescent degassing volcanoes worldwide, literature on the chemical evolution of BrO on large spatial and temporal scales is sparse. The first space-based observation of a volcanic BrO plume following the Kasatochi eruption in 2008 demonstrated the capability of satellite instruments to monitor such events on a global scale. In this study, we systematically examined GOME-2 observations from January 2007 until June 2011 for significantly enhanced BrO slant column densities (SCDs) in the vicinity of volcanic plumes. In total, 772 plumes from at least 37 volcanoes have been found by using sulphur dioxide (SO2) as a tracer for a volcanic plume. All captured SO2 plumes were subsequently analysed for a simultaneous enhancement of BrO and the data were checked for a possible spatial correlation between the two species. Additionally, the mean BrO/SO2 ratios for all volcanic plumes have been calculated by the application of a bivariate linear fit. A total number of 64 volcanic plumes from at least 11 different volcanoes showed clear evidence for BrO of volcanic origin, revealing large differences in the BrO/SO2 ratios (ranging from some 10−5 to several 10−4) and the spatial distribution of both species. A close correlation between SO2 and BrO occurred only for some of the observed eruptions or just in certain parts of the examined plumes. For other cases, only a rough spatial relationship was found. We discuss possible explanations for the occurrence of the different spatial SO2 and BrO distributions in aged volcanic plumes.
Continuous monitoring of summer surface water vapor isotopic composition above the Greenland Ice Sheet

We present here surface water vapor isotopic measurements conducted from June to August 2010 at the NEEM (North Greenland Eemian Drilling Project) camp, NW Greenland (77.45° N, 51.05° W, 2484 m a.s.l.). Measurements were conducted at 9 different heights from 0.1 m to 13.5 m above the snow surface using two different types of cavity-enhanced near-infrared absorption spectroscopy analyzers. For each instrument specific protocols were developed for calibration and drift corrections. The inter-comparison of corrected results from different instruments reveals excellent reproducibility, stability, and precision with a standard deviations of ~ 0.23&permil; for δ18O and ~ 1.4&permil; for δD. Diurnal and intraseasonal variations show strong relationships between changes in local surface humidity and water vapor isotopic composition, and with local and synoptic weather conditions. This variability probably results from the interplay between local moisture fluxes, linked with firn–air exchanges, boundary layer dynamics, and large-scale moisture advection. Particularly remarkable are several episodes characterized by high (> 40&permil;) surface water vapor deuterium excess. Air mass back-trajectory calculations from atmospheric analyses and water tagging in the LMDZiso (Laboratory of Meteorology Dynamics Zoom-isotopic) atmospheric model reveal that these events are associated with predominant Arctic air mass origin. The analysis suggests that high deuterium excess levels are a result of strong kinetic fractionation during evaporation at the sea-ice margin.
Overview of aerosol properties associated with air masses sampled by the ATR-42 during the EUCAARI campaign (2008)

Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Météo-France aircraft ATR-42 performed 22 research flights over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped to study the aerosol physical, chemical, hygroscopic and optical properties, as well as cloud microphysics. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin, allowing for a qualitative evaluation of emission influence on the respective air parcel. This study shows that the extensive aerosol parameters (aerosol mass and number concentrations) show vertical decreasing gradients and in some air masses maximum mass concentrations (mainly organics) in an intermediate layer (1–3 km). The observed mass concentrations (in the boundary layer (BL): between 10 and 30 μg m−3; lower free troposphere (LFT): 0.8 and 14 μg m−3) are high especially in comparison with the 2015 European norms for PM2.5 (25 μg m−3) and with previous airborne studies performed over England (Morgan et al., 2009; McMeeking et al., 2012). Particle number size distributions show a larger fraction of particles in the accumulation size range in the LFT compared to BL. The chemical composition of submicron aerosol particles is dominated by organics in the BL, while ammonium sulphate dominates the submicron aerosols in the LFT, especially in the aerosol particles originated from north-eastern Europe (~ 80%), also experiencing nucleation events along the transport. As a consequence, first the particle CCN acting ability, shown by the CCN/CN ratio, and second the average values of the scattering cross sections of optically active particles (i.e. scattering coefficient divided by the optical active particle concentration) are increased in the LFT compared to BL.
Simulation of trace gases and aerosols over the Indian domain: evaluation of the WRF-Chem Model

The "online" meteorological and chemical transport Weather Research and Forecasting/Chemistry (WRF-Chem) model has been implemented over the Indian subcontinent for three consecutive summers in 2008, 2009 and 2010 to study the aerosol properties over the domain. The initial and boundary conditions are obtained from NCAR reanalysis data. The emission rates of sulfur dioxide, black carbon, organic carbon and PM2.5, which are developed over India at a grid resolution of 0.25° × 0.25° have been used in the present study. The remaining emissions are obtained from global inventories (RETRO and EDGAR). The model simulated the meteorological parameters, trace gases and particulate matter. Predicted mixing ratios of trace gases (Ozone, carbon monoxide and sulfur dioxide) are compared with ground based observations over Kanpur. Simulated aerosol optical depth are compared with those observed at nine Aerosol Robotic Network stations (AERONET). The simulations show that the aerosol optical depth of the less polluted regions is better simulated compared to that of the locations where the aerosol loading is very high. The vertical profiles of extinction coefficient observed at Kanpur Micropulse Lidar Network (MPLNET) station is in agreement with the simulated values for altitudes greater than 1.5 km and qualitatively simulate the elevated layers of aerosols. The simulated mass concentration of black carbon shows very good correlation with observations, due to the better local emission inventory used. The vertical profiles of black carbon at various locations have also been compared with observations from aircraft campaign held during pre-monsoon period of 2008 and 2009 resulting in good agreement. This study shows that WRF-Chem model captures many important features of the observations and therefore can be used for understanding and predicting regional atmospheric composition over Indian subcontinent.
Evaluating and constraining ice cloud parameterizations in CAM5 using aircraft measurements from the SPARTICUS campaign

This study uses aircraft measurements of relative humidity and ice crystal size distribution collected during the SPARTICUS (Small PARTicles In CirrUS) field campaign to evaluate and constrain ice cloud parameterizations in the Community Atmosphere Model version 5. About 200 h of data were collected during the campaign between January and June 2010, providing the longest aircraft measurements available so far for cirrus clouds in the midlatitudes. The probability density function (PDF) of ice crystal number concentration (Ni) derived from the high-frequency (1 Hz) measurements features a strong dependence on ambient temperature. As temperature decreases from −35 °C to −62 °C, the peak in the PDF shifts from 10–20 L−1 to 200–1000 L−1, while Ni shows a factor of 6–7 increase. Model simulations are performed with two different ice nucleation schemes for pure ice-phase clouds. One of the schemes can reproduce a clear increase of Ni with decreasing temperature by using either an observation-based ice nuclei spectrum or a classical-theory-based spectrum with a relatively low (5–10%) maximum freezing ratio for dust aerosols. The simulation with the other scheme, which assumes a high maximum freezing ratio (100%), shows much weaker temperature dependence of Ni. Simulations are also performed to test empirical parameters related to water vapor deposition and the autoconversion of ice crystals to snow. Results show that a value between 0.05 and 0.1 for the water vapor deposition coefficient, and 250 μm for the critical diameter that distinguishes ice crystals from snow, can produce good agreement between model simulation and the SPARTICUS measurements in terms of Ni and effective radius. The climate impact of perturbing these parameters is also discussed.