Items

Advanced search

Porous aerosol in degassing plumes of Mt. Etna and Mt. Stromboli

Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular-scattering intensities and particle size distributions measured simultaneously with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75); the effective diameter was within the range of 1.5–2.8 µm and the maximal diameter was lower than 20 µm. A principal component analysis applied to the Polar Nephelometer data indicates that scattering features of volcanic aerosols of different crater origins are clearly distinctive from angular-scattering intensities of cirrus and contrails. Retrievals of aerosol properties revealed that the particles were "optically spherical" and the estimated values of the real part of the refractive index are within the interval from 1.35 to 1.38. The interpretation of these results leads to the conclusion that the degassing plume aerosols were porous with air voids. Our estimates suggest that aerosol particles contained about 18 to 35 % of air voids in terms of the total volume.
Molecular composition of organic aerosols in central Amazonia: an ultra-high-resolution mass spectrometry study

The Amazon Basin plays key role in atmospheric chemistry, biodiversity and climate change. In this study we applied nanoelectrospray (nanoESI) ultra-high-resolution mass spectrometry (UHRMS) for the analysis of the organic fraction of PM2.5 aerosol samples collected during dry and wet seasons at a site in central Amazonia receiving background air masses, biomass burning and urban pollution. Comprehensive mass spectral data evaluation methods (e.g. Kendrick mass defect, Van Krevelen diagrams, carbon oxidation state and aromaticity equivalent) were used to identify compound classes and mass distributions of the detected species. Nitrogen- and/or sulfur-containing organic species contributed up to 60 % of the total identified number of formulae. A large number of molecular formulae in organic aerosol (OA) were attributed to later-generation nitrogen- and sulfur-containing oxidation products, suggesting that OA composition is affected by biomass burning and other, potentially anthropogenic, sources. Isoprene-derived organosulfate (IEPOX-OS) was found to be the most dominant ion in most of the analysed samples and strongly followed the concentration trends of the gas-phase anthropogenic tracers confirming its mixed anthropogenic–biogenic origin. The presence of oxidised aromatic and nitro-aromatic compounds in the samples suggested a strong influence from biomass burning especially during the dry period. Aerosol samples from the dry period and under enhanced biomass burning conditions contained a large number of molecules with high carbon oxidation state and an increased number of aromatic compounds compared to that from the wet period. The results of this work demonstrate that the studied site is influenced not only by biogenic emissions from the forest but also by biomass burning and potentially other anthropogenic emissions from the neighbouring urban environments.
A new parameterization of the UV irradiance altitude dependence for clear-sky conditions and its application in the on-line UV tool over Northern Eurasia

A new method for calculating the altitude UV dependence is proposed for different types of biologically active UV radiation (erythemally weighted, vitamin-D-weighted and cataract-weighted types). We show that for the specified groups of parameters the altitude UV amplification (AUV) can be presented as a composite of independent contributions of UV amplification from different factors within a wide range of their changes with mean uncertainty of 1 % and standard deviation of 3 % compared with the exact model simulations with the same input parameters. The parameterization takes into account for the altitude dependence of molecular number density, ozone content, aerosol and spatial surface albedo. We also provide generalized altitude dependencies of the parameters for evaluating the AUV. The resulting comparison of the altitude UV effects using the proposed method shows a good agreement with the accurate 8-stream DISORT model simulations with correlation coefficient r  >  0.996. A satisfactory agreement was also obtained with the experimental UV data in mountain regions. Using this parameterization we analyzed the role of different geophysical parameters in UV variations with altitude. The decrease in molecular number density, especially at high altitudes, and the increase in surface albedo play the most significant role in the UV growth. Typical aerosol and ozone altitude UV effects do not exceed 10–20 %. Using the proposed parameterization implemented in the on-line UV tool (<a href="http://momsu.ru/uv/" target="_blank">http://momsu.ru/uv/</a>) for Northern Eurasia over the PEEX domain we analyzed the altitude UV increase and its possible effects on human health considering different skin types and various open body fraction for January and April conditions in the Alpine region.
Drainage and tillage practices in the winter fallow season mitigate CH4 and N2O emissions from a double-rice field in China

Traditional land management (no tillage, no drainage, NTND) during the winter fallow season results in substantial CH4 and N2O emissions from double-rice fields in China. A field experiment was conducted to investigate the effects of drainage and tillage during the winter fallow season on CH4 and N2O emissions and to develop mitigation options. The experiment had four treatments: NTND, NTD (drainage but no tillage), TND (tillage but no drainage), and TD (both drainage and tillage). The study was conducted from 2010 to 2014 in a Chinese double-rice field. During winter, total precipitation and mean daily temperature significantly affected CH4 emission. Compared to NTND, drainage and tillage decreased annual CH4 emissions in early- and late-rice seasons by 54 and 33 kg CH4 ha−1 yr−1, respectively. Drainage and tillage increased N2O emissions in the winter fallow season but reduced it in early- and late-rice seasons, resulting in no annual change in N2O emission. Global warming potentials of CH4 and N2O emissions were decreased by 1.49 and 0.92 t CO2 eq. ha−1 yr−1, respectively, and were reduced more by combining drainage with tillage, providing a mitigation potential of 1.96 t CO2 eq. ha−1 yr−1. A low total C content and high C / N ratio in rice residues showed that tillage in the winter fallow season reduced CH4 and N2O emissions in both early- and late-rice seasons. Drainage and tillage significantly decreased the abundance of methanogens in paddy soil, and this may explain the decrease of CH4 emissions. Greenhouse gas intensity was significantly decreased by drainage and tillage separately, and the reduction was greater by combining drainage with tillage, resulting in a reduction of 0.17 t CO2 eq. t−1. The results indicate that drainage combined with tillage during the winter fallow season is an effective strategy for mitigating greenhouse gas releases from double-rice fields.
Response of winter fine particulate matter concentrations to emission and meteorology changes in North China

The winter haze is a growing problem in North China, but the causes are not well understood. The chemistry version of the Weather Research and Forecasting model (WRF-Chem) was applied in North China to examine how PM2.5 concentrations change in response to changes in emissions (sulfur dioxide (SO2), black carbon (BC), organic carbon (OC), ammonia (NH3), and nitrogen oxides (NOx)), as well as meteorology (temperature, relative humidity (RH), and wind speeds) changes in winter. From 1960 to 2010, the dramatic changes in emissions lead to +260 % increases in sulfate, +320 % increases in nitrate, +300 % increases in ammonium, +160 % increases in BC, and +50 % increases in OC. The responses of PM2.5 to individual emission species indicate that the simultaneous increases in SO2, NH3, and NOx emissions dominated the increases in PM2.5 concentrations. PM2.5 shows more notable increases in response to changes in SO2 and NH3 as compared to increases in response to changes in NOx emissions. In addition, OC also accounts for a large fraction in PM2.5 changes. These results provide some implications for haze pollution control. The responses of PM2.5 concentrations to temperature increases are dominated by changes in wind fields and mixing heights. PM2.5 shows relatively smaller changes in response to temperature increases and RH decreases compared to changes in response to changes in wind speed and aerosol feedbacks. From 1960 to 2010, aerosol feedbacks have been significantly enhanced due to higher aerosol loadings. The discussions in this study indicate that dramatic changes in emissions are the main cause of increasing haze events in North China, and long-term trends in atmospheric circulations may be another important cause since PM2.5 is shown to be substantially affected by wind speed and aerosol feedbacks. More studies are necessary to get a better understanding of the aerosol–circulation interactions.
Arabian Red Sea coastal soils as potential mineral dust sources

Both Moderate Resolution Imaging Spectroradiometer (MODIS) and Spinning Enhanced Visible and InfraRed Imager (SEVIRI) satellite observations suggest that the narrow heterogeneous Red Sea coastal region is a frequent source of airborne dust that, because of its proximity, directly affects the Red Sea and coastal urban centers. The potential of soils to be suspended as airborne mineral dust depends largely on soil texture, moisture content and particle size distributions. Airborne dust inevitably carries the mineralogical and chemical signature of a parent soil. The existing soil databases are too coarse to resolve the small but important coastal region. The purpose of this study is to better characterize the mineralogical, chemical and physical properties of soils from the Arabian Red Sea coastal plain, which in turn will help to improve assessment of dust effects on the Red Sea, land environmental systems and urban centers. Thirteen surface soils from the hot-spot areas of windblown mineral dust along the Red Sea coastal plain were sampled for analysis. Analytical methods included optical microscopy, X-ray diffraction (XRD), inductively coupled plasma optical emission spectrometry (ICP-OES), ion chromatography (IC), scanning electron microscopy (SEM) and laser particle size analysis (LPSA). We found that the Red Sea coastal soils contain major components of quartz and feldspar, as well as lesser but variable amounts of amphibole, pyroxene, carbonate, clays and micas, with traces of gypsum, halite, chlorite, epidote and oxides. The range of minerals in the soil samples was ascribed to the variety of igneous and metamorphic provenance rocks of the Arabian Shield forming the escarpment to the east of the Red Sea coastal plain. The analysis revealed that the samples contain compounds of nitrogen, phosphorus and iron that are essential nutrients to marine life. The analytical results from this study will provide a valuable input into dust emission models used in climate, marine ecology and air quality studies.
Sea salt emission, transport and influence on size-segregated nitrate simulation: a case study in northwestern Europe by WRF-Chem

Sea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of ∼  20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation.
Parameterizing cloud condensation nuclei concentrations during HOPE

An aerosol model was used to simulate the generation and transport of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations; however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterization of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterization. A comparison between the parameterization and the CCN estimates from the model data shows excellent agreement. This parameterization may be used in other regions and time periods with a similar aerosol load; furthermore, the technique demonstrated here may be employed in regions dominated by different aerosol species.
Impacts of the Denver Cyclone on regional air quality and aerosol formation in the Colorado Front Range during FRAPPÉ 2014

We present airborne measurements made during the 2014 Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) project to investigate the impacts of the Denver Cyclone on regional air quality in the greater Denver area. Data on trace gases, non-refractory submicron aerosol chemical constituents, and aerosol optical extinction (βext) at λ  =  632 nm were evaluated in the presence and absence of the surface mesoscale circulation in three distinct study regions of the Front Range: In-Flow, Northern Front Range, and the Denver metropolitan area. Pronounced increases in mass concentrations of organics, nitrate, and sulfate in the Northern Front Range and the Denver metropolitan area were observed during the cyclone episodes (27–28 July) compared to the non-cyclonic days (26 July, 2–3 August). Organic aerosols dominated the mass concentrations on all evaluated days, with a 45 % increase in organics on cyclone days across all three regions, while the increase during the cyclone episode was up to ∼  80 % over the Denver metropolitan area. In the most aged air masses (NOx / NOy  <  0.5), background organic aerosols over the Denver metropolitan area increased by a factor of ∼  2.5 due to transport from Northern Front Range. Furthermore, enhanced partitioning of nitric acid to the aerosol phase was observed during the cyclone episodes, mainly due to increased abundance of gas phase ammonia. During the non-cyclone events, βext displayed strong correlations (r  =  0.71) with organic and nitrate in the Northern Front Range and only with organics (r  =  0.70) in the Denver metropolitan area, while correlation of βext during the cyclone was strongest (r  =  0.86) with nitrate over Denver. Mass extinction efficiency (MEE) values in the Denver metropolitan area were similar on cyclone and non-cyclone days despite the dominant influence of different aerosol species on βext. Our analysis showed that the meteorological patterns associated with the Denver Cyclone increased aerosol mass loadings in the Denver metropolitan area mainly by transporting aerosols and/or aerosol precursors from the northern regions, leading to impaired visibility and air quality deterioration.
Modeling the reactive halogen plume from Ambrym and its impact on the troposphere with the CCATT-BRAMS mesoscale model

Ambrym Volcano (Vanuatu, southwest Pacific) is one of the largest sources of continuous volcanic emissions worldwide. As well as releasing SO2 that is oxidized to sulfate, volcanic plumes in the troposphere are shown to undergo reactive halogen chemistry whose atmospheric impacts have been little explored to date. Here, we investigate with the regional-scale model CCATT-BRAMS (Coupled Chemistry Aerosol-Tracer Transport model, Brazilian developments on the Regional Atmospheric Modeling System, version 4.3) the chemical processing in the Ambrym plume and the impact of this volcano on the atmospheric chemistry on both local and regional scales. We focus on an episode of extreme passive degassing that occurred in early 2005 and for which airborne DOAS (differential optical absorption spectroscopy) measurements of SO2 and BrO columns in the near-downwind plume between 15 and 40 km from the vents have been reported. The model was developed to include reactive halogen chemistry and a volcanic emission source specific to this extreme degassing event. In order to test our understanding of the volcanic plume chemistry, we performed very high-resolution (500 m  ×  500 m) simulations using the model nesting grid capability and compared each DOAS measurement to its temporally and spatially interpolated model counterpart “point-by-point”. Simulated SO2 columns show very good quantitative agreement with the DOAS observations, suggesting that the plume direction as well as its dilution in the near-downwind plume are well captured. The model also reproduces the salient features of volcanic chemistry as reported in previous work, such as HOx and ozone depletion in the core of the plume. When a high-temperature chemistry initialization is included, the model is able to capture the observed BrO ∕ SO2 trend with distance from the vent. The main discrepancy between observations and model is the bias between the magnitudes of observed and simulated BrO columns that ranges from 60 % (relative to the observations) for the transect at 15 km to 14 % for the one at 40 km from the vents. We identify total in-plume depletion of ozone as a limiting factor for the partitioning of reactive bromine into BrO in the near-source (concentrated) plume under these conditions of extreme emissions and low background ozone concentrations (15 ppbv). Impacts of Ambrym in the southwest Pacific region were also analyzed. As the plume disperses regionally, reactive halogen chemistry continues on sulfate aerosols produced by SO2 oxidation and promotes BrCl formation. Ozone depletion is weaker than on the local scale but still between 10 and 40 % in an extensive region a few thousands of kilometers from Ambrym. The model also predicts the transport of bromine to the upper troposphere and stratosphere associated with convection events. In the upper troposphere, HBr is re-formed from Br and HO2. Comparison of SO2 regional-scale model fields with OMI (Ozone Monitoring Instrument) satellite SO2 fields confirms that the Ambrym SO2 emissions estimate based on the DOAS observations used here is realistic. The model confirms the potential of volcanic emissions to influence the oxidizing power of the atmosphere: methane lifetime (calculated with respect to OH and Cl) is increased overall in the model due to the volcanic emissions. When considering reactive halogen chemistry, which depletes HOx and ozone, the lengthening of methane lifetime with respect to OH is increased by a factor of 2.6 compared to a simulation including only volcanic SO2 emissions. Cl radicals produced in the plume counteract 41 % of the methane lifetime lengthening due to OH depletion. Including the reactive halogen chemistry in our simulation also increases the lifetime of SO2 in the plume with respect to oxidation by OH by 36 % compared to a simulation including only volcanic SO2 emissions. This study confirms the strong influence of Ambrym emissions during the extreme degassing event of early 2005 on the composition of the atmosphere on both local and regional scales. It also stresses the importance of considering reactive halogen chemistry when assessing the impact of volcanic emissions on climate.