Items

Advanced search

Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

Airborne desert dust influences radiative transfer, atmospheric chemistry and dynamics, as well as nutrient transport and deposition. It directly and indirectly affects climate on regional and global scales. Two versions of a parameterization scheme to compute desert dust emissions are incorporated into the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). One uses a globally uniform soil particle size distribution, whereas the other explicitly accounts for different soil textures worldwide. We have tested these two versions and investigated the sensitivity to input parameters, using remote sensing data from the Aerosol Robotic Network (AERONET) and dust concentrations and deposition measurements from the AeroCom dust benchmark database (and others). The two versions are shown to produce similar atmospheric dust loads in the N-African region, while they deviate in the Asian, Middle Eastern and S-American regions. The dust outflow from Africa over the Atlantic Ocean is accurately simulated by both schemes, in magnitude, location and seasonality. Approximately 70% of the modelled annual deposition data and 70–75% of the modelled monthly aerosol optical depth (AOD) in the Atlantic Ocean stations lay in the range 0.5 to 2 times the observations for all simulations. The two versions have similar performance, even though the total annual source differs by ~50%, which underscores the importance of transport and deposition processes (being the same for both versions). Even though the explicit soil particle size distribution is considered more realistic, the simpler scheme appears to perform better in several locations. This paper discusses the differences between the two versions of the dust emission scheme, focusing on their limitations and strengths in describing the global dust cycle and suggests possible future improvements.
Crop harvest in Denmark and Central Europe contributes to the local load of airborne Alternaria spore concentrations in Copenhagen

This study examines the hypothesis that Danish agricultural areas are the main source of airborne Alternaria spores in Copenhagen, Denmark. We suggest that the contribution to the overall load is mainly local or regional, but with intermittent long distance transport (LDT) from more remote agricultural areas. This hypothesis is supported by investigating a 10 yr bi-hourly record of Alternaria spores in the air from Copenhagen. This record shows 232 clinically relevant episodes (daily average spore concentration above 100 m−3) with a distinct daily profile. The data analysis also revealed potential LDT episodes almost every year. A source map and analysis of atmospheric transport suggest that LDT always originates from the main agricultural areas in Central Europe. A dedicated emission study in cereal crops under harvest during 2010 also supports our hypothesis. The emission study showed that although the fields had been treated against fungal infections, harvesting still produced large amounts of airborne fungal spores. It is likely that such harvesting periods can cause clinically relevant levels of fungal spores in the atmosphere. Our findings suggest that crop harvest in Central Europe causes episodes of high airborne Alternaria spore concentrations in Copenhagen as well as other urban areas in this region. It is likely that such episodes could be simulated using atmospheric transport models.
Overview of the LADCO winter nitrate study: hourly ammonia, nitric acid and PM2.5 composition at an urban and rural site pair during PM2.5 episodes in the US Great Lakes region

An overview of the LADCO (Lake Michigan Air Directors Consortium) Winter Nitrate Study (WNS) is presented. Sampling was conducted at ground level at an urban-rural pair of sites during January–March 2009 in eastern Wisconsin, toward the western edge of the US Great Lakes region. Areas surrounding these sites experience multiday episodes of wintertime PM2.5 pollution characterized by high fractions of ammonium nitrate in PM, low wind speeds, and air mass stagnation. Hourly surface monitoring of inorganic gases and aerosols supplemented long-term 24-h aerosol chemistry monitoring at these locations. The urban site (Milwaukee, WI) experienced 13 PM2.5 episodes, defined as periods where the seven-hour moving average PM2.5 concentration exceeded 27 μg m−3 for at least four consecutive hours. The rural site experienced seven episodes by the same metric, and all rural episodes coincided with urban episodes. Episodes were characterized by low pressure systems, shallow/stable boundary layer, light winds, and increased temperature and relative humidity relative to climatological mean conditions. They often occurred in the presence of regional snow cover at temperatures near freezing, when snow melt and sublimation could generate fog and strengthen the boundary layer inversion. Substantial contribution to nitrate production from nighttime chemistry of ozone and NO2 to N2O5 and nitric acid is likely and requires further investigation. Pollutant-specific urban excess during episode and non-episode conditions is presented. The largest remaining uncertainties in the conceptual model of the wintertime episodes are the variability from episode-to-episode in ammonia emissions, the balance of daytime and nighttime nitrate production, the relationship between ammonia controls, NOx controls and ammonium nitrate reductions, and the extent to which snow and fog are causal (either through meteorological or chemical processes) rather than just correlated with episodes because of similar synoptic meteorology.
Observational constraints on entrainment and the entrainment interface layer in stratocumulus

Aircraft sampling of the stratocumulus-topped boundary layer (STBL) during the Physics of Stratocumulus Top (POST) experiment was primarily achieved using sawtooth flight patterns, during which the atmospheric layer 100 m above and below cloud top was sampled at a frequency of once every 2 min. The large data set that resulted from each of the 16 flights document the complex structure and variability of this interfacial region in a variety of conditions. In this study, we first describe some properties of the entrainment interface layer (EIL), where strong gradients in turbulent kinetic energy (TKE), potential temperature and moisture can be found. We find that defining the EIL by the first two properties tends to yield similar results, but that moisture can be a misleading tracer of the EIL. These results are consistent with studies using large-eddy simulations. We next utilize the POST data to shed light on and constrain processes relevant to entrainment, a key process in the evolution of the STBL that to-date is not well-represented even by high resolution models. We define "entrainment efficiency" as the ratio of the TKE consumed by entrainment to that generated within the STBL (primarily by cloud-top cooling). We find values for the entrainment efficiency that vary by 1.5 orders of magnitude, which is even greater than the one order magnitude that previous modeling results have suggested. Our analysis also demonstrates that the entrainment efficiency depends on the strength of the stratification of the EIL, but not on the TKE in the cloud top region. The relationships between entrainment efficiency and other STBL parameters serve as novel observational contraints for simulations of entrainment in such systems.
Accelerated dissolution of iron oxides in ice

Iron dissolution from mineral dusts and soil particles is vital as a source of bioavailable iron in various environmental media. In this work, the dissolution of iron oxide particles trapped in ice was investigated as a new pathway of iron supply. The dissolution experiments were carried out in the absence and presence of various organic complexing ligands under dark condition. In acidic pH conditions (pH 2, 3, and 4), the dissolution of iron oxides was greatly enhanced in the ice phase compared to that in water. The dissolved iron was mainly in the ferric form, which indicates that the dissolution is not a reductive process. The extent of dissolved iron was greatly affected by the kind of organic complexing ligands and the surface area of iron oxides. The iron dissolution was most pronounced with high surface area iron oxides and in the presence of strong iron binding ligands. The enhanced dissolution of iron oxides in ice is mainly ascribed to the "freeze concentration effect", which concentrates iron oxide particles, organic ligands, and protons in the liquid like ice grain boundary region and accelerates the dissolution of iron oxides. The ice-enhanced dissolution effect gradually decreased when decreasing the freezing temperature from −10 to −196 °C, which implies that the presence and formation of the liquid-like ice grain boundary region play a critical role. The proposed phenomenon of enhanced dissolution of iron oxides in ice may provide a new pathway of bioavailable iron production. The frozen atmospheric ice with iron-containing dust particles in the upper atmosphere thaws upon descending and may provide bioavailable iron upon deposition onto the ocean surface.
Supermicron modes of ammonium ions related to fog in rural atmosphere

Fog-processed aerosols were identified and analyzed in detail from a large-sized database in which size-segregated atmospheric particles and gases were simultaneously measured at eight Canadian rural sites. In ten samples collected during or following fog events, at least one supermicron mode of particulate NH4+ was observed. The supermicron modes were likely associated with fog events since they were absent on non-fog days. The supermicron mode of NH4+ in the 5–10 μm size range probably reflected the direct contribution from fog droplets. Based on detailed analysis of the chemical compositions and the extent of neutralization, the supermicron mode of NH4+ in the 1–4 μm size range was believed to be caused by fog-processing of ammonium salt aerosols. These aerosol particles consisted of incompletely neutralized sulfuric acid aerosols in NH3-poor conditions or a mixture of ammonium nitrate and ammonium sulfate aerosols in NH3-rich conditions. Interstitial aerosols and fog droplets presented during fog events likely yielded a minor direct contribution to the measured NH4+. The mass median aerodynamic diameter (MMAD) of the 1–4 μm mode of NH4+ strongly depended on ambient temperature (T) and can be grouped into two regimes. In one regime, the MMAD was between 1.1 and 1.7 μm in four samples, when fog occurred at T > 0 °C, and in two samples, at T > −3 °C. The MMAD of NH4+ in this size range was also observed in various atmospheric environments, as discussed in the literature. In the other regime, the MMAD was between 2.8 and 3.4 μm in four samples when fog occurred at T < −4 °C, a phenomenon that was first observed in this study. The MMAD was not related to chemical composition and concentration of ammonium salts. Further investigations are needed in order to fully understand the cause of the MMAD. The larger supermicron mode of ammonium salts aerosol observed at T < −4 °C has added new knowledge on the size distributions and chemical compositions of fog-processed aerosols under various ambient conditions.
Formaldehyde and nitrogen dioxide over the remote western Pacific Ocean: SCIAMACHY and GOME-2 validation using ship-based MAX-DOAS observations

In October 2009, shipborne Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed during the TransBrom campaign over the western Pacific Ocean (≈ 40° N to 20° S). Vertical tropospheric trace gas columns and profiles of nitrogen dioxide (NO2) and formaldehyde (HCHO) as well as stratospheric NO2 columns were retrieved in order to validate corresponding measurements from the GOME-2 and SCIAMACHY satellite instruments and to estimate tropospheric background concentrations of these trace gases. All instruments reproduced the same characteristic, latitude-dependent shape of stratospheric NO2. SCIAMACHY and GOME-2 data differ by about 1% from each other while yielding lower vertical columns than MAX-DOAS morning values as a consequence of measurement time and stratospheric NO2 diurnal cycle. Due to this diurnal cycle, an increase of 8.7 ± 0.5 × 1013 molec cm−2 h−1 of stratospheric NO2 was estimated from MAX-DOAS data at low latitudes during the day. Tropospheric NO2 was above the detection limit only in regions of higher anthropogenic impact (ship traffic, transport of pollution from land). A background column of 1.3 × 1014 molec cm−2 (or roughly 50 ppt boundary layer concentration) can be estimated as upper limit for the remote ocean, which is in agreement with GOME-2 monthly mean values. In the marine boundary layer close to the islands of Hokkaido and Honshu, up to 0.8 ppbv were retrieved close to the surface. Background HCHO concentrations over the remote ocean exhibit a diurnal cycle with maximum values (depending strongly on weather conditions) of 4 × 1015 molec cm−2 for the vertical column at noontime. Corresponding peak concentrations of up to 1.1 ppbv were retrieved in elevated altitudes (≈ 400 m) around noon while maximum concentrations in the evening are close to the ground. An agreement between MAX-DOAS and GOME-2 data was found for typical vertical columns of 3 × 1015 molec cm−2 over the remote ocean at the time of overpass.
Density currents as a desert dust mobilization mechanism

The formation and propagation of density currents are well studied processes in fluid dynamics with many applications in other science fields. In the atmosphere, density currents are usually meso-β/γ phenomena and are often associated with storm downdrafts. These storms are responsible for the formation of severe dust episodes (haboobs) over desert areas. In the present study, the formation of a convective cool pool and the associated dust mobilization are examined for a representative event over the western part of Sahara desert. The physical processes involved in the mobilization of dust are described with the use of the integrated atmospheric-air quality RAMS/ICLAMS model. Dust is effectively produced due to the development of near surface vortices and increased turbulent mixing along the frontal line. Increased dust emissions and recirculation of the elevated particles inside the head of the density current result in the formation of a moving "dust wall". Transport of the dust particles in higher layers – outside of the density current – occurs mainly in three ways: (1) Uplifting of preexisting dust over the frontal line with the aid of the strong updraft (2) Entrainment at the upper part of the density current head due to turbulent mixing (3) Vertical mixing after the dilution of the system. The role of the dust in the associated convective cloud system was found to be limited. Proper representation of convective processes and dust mobilization requires the use of high resolution (cloud resolving) model configuration and online parameterization of dust production. Haboob-type dust storms are effective dust sources and should be treated accordingly in dust modeling applications.
Iodine emissions from the sea ice of the Weddell Sea

Iodine compounds were measured above, below and within the sea ice of the Weddell Sea during a cruise in 2009, to make progress in elucidating the mechanism of local enhancement and volatilisation of iodine. I2 mixing ratios of up to 12.4 pptv were measured 10 m above the sea ice, and up to 31 pptv was observed above surface snow on the nearby Brunt Ice Shelf – large amounts. Atmospheric IO of up to 7 pptv was measured from the ship, and the average sum of HOI and ICl was 1.9 pptv. These measurements confirm the Weddell Sea as an iodine hotspot. Average atmospheric concentrations of CH3I, C2H5I, CH2ICl, 2-C3H7I, CH2IBr and 1-C3H7I were each 0.2 pptv or less. On the Brunt Ice Shelf, enhanced concentrations of CH3I and C2H5I (up to 0.5 and 1 pptv respectively) were observed in firn air, with a diurnal profile that suggests the snow may be a source. In the sea ice brine, iodocarbons concentrations were over 10 times those of the sea water below. The sum of iodide + iodate was depleted in sea ice samples, suggesting some missing iodine chemistry. Flux calculations suggest I2 dominates the iodine atom flux to the atmosphere, but models cannot reconcile the observations and suggest either a missing iodine source or other deficiencies in our understanding of iodine chemistry. The observation of new particle formation, consistent with the model predictions, strongly suggests an iodine source. This combined study of iodine compounds is the first of its kind in this unique region of sea ice rich in biology and rich in iodine chemistry.
Simulation of nitrate, sulfate, and ammonium aerosols over the United States

Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium) are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. Predicted aerosol concentrations are compared with surface-level measurement data from the Interagency Monitoring of Protected Visual Environments (IMPROVE), the Clean Air Status and Trends Network (CASTNET), and the California Air Resources Board (CARB). Sulfate predictions nationwide are in reasonably good agreement with observations, while nitrate and ammonium are over-predicted in the East and Midwest, but under-predicted in California, where observed concentrations are the highest in the country. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which suggest that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted based on current values of the N2O5 uptake coefficient, γ, onto aerosols. After reducing the value of γ by a factor of 10, predicted nitrate levels in the US Midwest and East still remain higher than those measured, and over-prediction of nitrate in this region remains unexplained. Comparison of model predictions with satellite measurements of ammonia from the Tropospheric Emissions Spectrometer (TES) indicates that ammonia emissions in GEOS-Chem are underestimated in California and that the nationwide seasonality applied to ammonia emissions in GEOS-Chem does not represent California very well, particularly underestimating winter emissions. An ammonia sensitivity study indicates that GEOS-Chem simulation of nitrate is ammonia-limited in southern California and much of the state, suggesting that an underestimate of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in many areas of California. An approximate doubling of ammonia emissions is needed to reproduce observed nitrate concentrations in southern California and in other ammonia sensitive areas of California. However, even a tenfold increase in ammonia emissions yields predicted nitrate concentrations that are still biased low in the central valley of California. The under-prediction of nitrate aerosol in the central valley of California may arise in part from an under-prediction of both ammonia and nitric acid in this region. Since nitrate aerosols are particularly sensitive to mixed layer depths, owing to the gas-particle equilibrium, the nitrate under-prediction could also arise in part from a potential regional overestimate of GEOS-5 mixed layer depths in the central valley due to unresolved topography in this region.