Ocean-atmosphere trace gas exchange

The oceans contribute significantly to the global emissions of a number of atmospherically important volatile gases, notably those containing sulfur, nitrogen and halogens. Such gases play critical roles not only in global biogeochemical cycling but also in a wide range of atmospheric processes including marine aerosol formation and modification, tropospheric ozone formation and destruction, photooxidant cycling and stratospheric ozone loss. A number of marine emissions are greenhouse gases, others influence the Earth's radiative budget indirectly through aerosol formation and/or by modifying oxidant levels and thus changing the atmospheric lifetime of gases such as methane. In this article we review current literature concerning the physical, chemical and biological controls on the sea-air emissions of a wide range of gases including dimethyl sulphide (DMS), halocarbons, nitrogen-containing gases including ammonia (NH3), amines (including dimethylamine, DMA, and diethylamine, DEA), alkyl nitrates (RONO2) and nitrous oxide (N2O), non-methane hydrocarbons (NMHC) including isoprene and oxygenated (O)VOCs, methane (CH4) and carbon monoxide (CO). Where possible we review the current global emission budgets of these gases as well as known mechanisms for their formation and loss in the surface ocean.

Columnar aerosol properties in a northeastern atlantic site (plymouth united kingdom) by means of ground based skyradiometer data during years 2000-2008.

Between 2000 and 2008, columnar optical and radiative properties were measured at the Plymouth Marine Laboratory (PML), UK (50° 21.95′N, 4° 8.85′W) using an automatic Prede POM01L sun–sky photometer. The database was analyzed for aerosol optical properties using the SKYRAD radiative inversion algorithm and calibrated using the in situ SKYIL calibration method. Retrievals include aerosol optical depth, Ångström wavelength exponent, aerosol volume distribution, refractive index and single scattering albedo. The results show that the Plymouth site is characterized by low values of aerosol optical depth with low variability (0.18 ± 0.08 at 500 nm) and a mean annual Ångström exponent of 1.03 ± 0.21. The annual mean of the single scattering albedo is 0.97, indicative of non-absorbing aerosols. The aerosol properties were classified in terms of air mass back trajectories: the area is mainly affected by Atlantic air masses and the dominant aerosol type is a mixture of maritime particles, present in low burdens with variable size. The maritime air masses were defined by annual mean values for the AOD (at 500 nm) of 0.13–0.14 and a wavelength exponent of 0.96–1.03. Episodic anthropogenic and mineral dust intrusions occasionally occur, but they are sporadic and dilute (AOD at 500 nm about 0.20). Tropical continental air masses were characterized by the highest AOD at 500 nm (0.34) and the lowest wavelength exponent (0.83), although they were the least represented in the analysis.

The ESA Climate Change Initiative: Satellite Data Records for Essential Climate Variables

Observations of Earth from space have been made for over 40 years and have contributed to advances in many aspects of climate science. However, attempts to exploit this wealth of data are often hampered by a lack of homogeneity and continuity and by insufficient understanding of the products and their uncertainties. There is, therefore, a need to reassess and reprocess satellite datasets to maximize their usefulness for climate science. The European Space Agency has responded to this need by establishing the Climate Change Initiative (CCI). The CCI will create new climate data records for (currently) 13 essential climate variables (ECVs) and make these open and easily accessible to all. Each ECV project works closely with users to produce time series from the available satellite observations relevant to users' needs. A climate modeling users' group provides a climate system perspective and a forum to bring the data and modeling communities together. This paper presents the CCI program. It outlines its benefit and presents approaches and challenges for each ECV project, covering clouds, aerosols, ozone, greenhouse gases, sea surface temperature, ocean color, sea level, sea ice, land cover, fire, glaciers, soil moisture, and ice sheets. It also discusses how the CCI approach may contribute to defining and shaping future developments in Earth observation for climate science.

Space-based lidar measurements of global ocean carbon stocks

Global ocean phytoplankton biomass (C-phyto) and total particulate organic carbon (POC) stocks have largely been characterized from space using passive ocean color measurements. A space-based light detection and ranging (lidar) system can provide valuable complementary observations for C-phyto and POC assessments, with benefits including day-night sampling, observations through absorbing aerosols and thin cloud layers, and capabilities for vertical profiling through the water column. Here we use measurements from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) to quantify global C-phyto and POC from retrievals of subsurface particulate backscatter coefficients (b(bp)). CALIOP b(bp) data compare favorably with airborne, ship-based, and passive ocean data and yield global average mixed-layer standing stocks of 0.44 Pg C for C-phyto and 1.9 Pg for POC. CALIOP-based C-phyto and POC data exhibit global distributions and seasonal variations consistent with ocean plankton ecology. Our findings support the use of spaceborne lidar measurements for advancing understanding of global plankton systems.

Xanthoria parietina as a biomonitor of airborne heavy metal pollution in forest sites in the North East of Morocco

Xanthoria parietina, common foliose lichen, growing in its natural habitat, was analysed for the concentration of five heavy metals (Fe, Cr, Zn, Pb and Cu) from different forest sites of North East of Morocco (Kenitra, Sidi Boughaba, Mkhinza, Ceinture Verte near Temara city, Skhirate, Bouznika and Mohammedia). The quantification was carried out by inductively coupled plasma - atomic emission spectrometry (ICP-AES). Results were highly significant p<0,001. The concentration of metals is correlated with the vehicular activity and urbanization. The total metal concentration is highest at the Kenitra area, followed by Ceinture Verte site near Temara city, which experience heavy traffic throughout the year. Scanning electron microscopy (SEM) of particulate matter on lichen of Xanthoria parietina was assessed as a complementary technique to wet chemical analysis for source apportionment of airborne contaminant. Analysis revealed high level of Cu, Cr, Zn and Pb in samples near roads.  

Large carbon isotope fractionation associated with oxidation of methyl halides by methylotrophic bacteria

The largest biological fractionations of stable carbon isotopes observed in nature occur during production of methane by methanogenic archaea. These fractionations result in substantial (as much as 70) shifts in 13C relative to the initial substrate. We now report that a stable carbon isotopic fractionation of comparable magnitude (up to 70) occurs during oxidation of methyl halides by methylotrophic bacteria. We have demonstrated biological fractionation with whole cells of three methylotrophs (strain IMB-1, strain CC495, and strain MB2) and, to a lesser extent, with the purified cobalamin-dependent methyltransferase enzyme obtained from strain CC495. Thus, the genetic similarities recently reported between methylotrophs, and methanogens with respect to their pathways for C1-unit metabolism are also reflected in the carbon isotopic fractionations achieved by these organisms. We found that only part of the observed fractionation of carbon isotopes could be accounted for by the activity of the corrinoid methyltransferase enzyme, suggesting fractionation by enzymes further along the degradation pathway. These observations are of potential biogeochemical significance in the application of stable carbon isotope ratios to constrain the tropospheric budgets for the ozone-depleting halocarbons, methyl bromide and methyl chloride.

Are there clinical features of a sensitized cough reflex?

Cough reflex hypersensitization is a key feature in patients with troublesome cough. The clinical consequence of this hypersensitive state is typified by bouts of coughing often triggered by low threshold stimuli encountered by the patient during normal daily activities including exposure to aerosols, scents and odours, a change in air temperature and when talking or laughing. These features are often perceived by cough patients to be the most disruptive aspect of their condition and undoubtedly contribute to impaired quality of life. Patients with troublesome cough may describe a range of additional symptoms and sensations including an 'urge to cough' or the feeling of an 'itch' at the back of the throat, or a choking sensation and occasionally chest pain or breathlessness. It is uncertain if these features arise due to the processes responsible for cough reflex sensitization or as a direct consequence of the underlying cough aetiology. In an attempt to understand the clinical features of a sensitized cough reflex, the spectrum of symptoms typically described by cough patients will be reviewed and possible underlying mechanisms considered. Since an intact cough reflex is crucial to airway protection, anti-tussive treatment that attenuates the hypersensitive cough state rather than abolishing the cough reflex completely would be preferable. Identifying such agents remains a clinical, scientific and pharmacological challenge. (c) 2008 Elsevier Ltd. All rights reserved.

Temporal variation in the water chemistry of northern Victoria Land lakes (Antarctica)

Concentrations of major ions, silicate and nutrients (total N and P) were measured in samples of surface water from 28 lakes in ice-free areas of northern Victoria Land (East Antarctica). Sixteen lakes were sampled during austral summers 2001/02, 2003/04, 2004/05 and 2005/06 to assess temporal variation in water chemistry. Although samples showed a wide range in ion concentrations, their composition mainly reflected that of seawater. In general, as the distance from the sea increased, the input of elements from the marine environment (through aerosols and seabirds) decreased and there was an increase in nitrate and sulfate concentrations. Antarctic lakes lack outflows and during the austral summer the melting and/or ablation of ice cover, water evaporation and leaching processes in dry soils determine a progressive increase in water ion concentrations. During the five-year monitoring survey, no statistically significant variation in the water chemistry were detected, except for a slight (hardly significant) increase in TN concentrations. However, Canonical Correspondence Analysis (CCA) indicated that other factors besides distance from the sea, the presence of nesting seabirds, the sampling time and percentage of ice cover affect the composition of water in Antarctic cold desert environments.

Ash from Changbaishan Millennium eruption recorded in Greenland ice: Implications for determining the eruption's timing and impact

Major volcanic eruptions can impact on global climate by injecting large quantities of aerosols and ash into the atmosphere that alter the radiative balance and chemical equilibrium of the stratosphere. The Millennium eruption of Tianchi (Paektu), China/North Korea, was one of the largest Late Holocene eruptions. Uncertainty about the precise timing of the eruption has hindered the recognition of its climate impact in palaeoclimate and historical records. Here we report the compelling identification of the eruption's volcanic signal in Greenland ice cores through the association of geochemically-characterized volcanic glass, represented in by bimodal populations that compare with proximal material from the source eruption. The eruption most probably occurred in the AD 940?s, seven years after the Eldgjá eruption on Iceland. We examine the eruption's potential for climate forcing using the sulfate records from the ice-cores and conclude that it was unlikely to have had a global or extra-regional impact.

Mafic Plinian volcanism and ignimbrite emplacement at Tofua volcano, Tonga

Tofua Island is the largest emergent mafic volcano within the Tofua arc, Tonga, southwest Pacific. The volcano is dominated by a distinctive caldera averaging 4 km in diameter, containing a freshwater lake in the south and east. The latest paroxysmal (VEI 5-6) explosive volcanism includes two phases of activity, each emplacing a high-grade ignimbrite. The products are basaltic andesites with between 52 wt.% and 57 wt.% SiO(2). The first and largest eruption caused the inward collapse of a stratovolcano and produced the 'Tofua' ignimbrite and a sub-circular caldera located slightly northwest of the island's centre. This ignimbrite was deposited in a radial fashion over the entire island, with associated Plinian fall deposits up to 0.5 m thick on islands > 40 km away. Common sub-rounded and frequently cauliform scoria bombs throughout the ignimbrite attest to a small degree of marginal magma-water interaction. The common intense welding of the coarse-grained eruptive products, however, suggests that the majority of the erupted magma was hot, water-undersaturated and supplied at high rates with moderately low fragmentation efficiency and low levels of interaction with external water. We propose that the development of a water-saturated dacite body at shallow (<6 km) depth resulted in failure of the chamber roof to cause sudden evacuation of material, producing a Plinian eruption column. Following a brief period of quiescence, largescale faulting in the southeast of the island produced a second explosive phase believed to result from recharge of a chemically distinct magma depleted in incompatible elements. This similar, but smaller eruption, emplaced the 'Hokula' Ignimbrite sheet in the northeast of the island. A maximum total volume of 8 km(3) of juvenile material was erupted by these events. The main eruption column is estimated to have reached a height of similar to 12 km, and to have produced a major atmospheric injection of gas, and tephra recorded in the widespread series of fall deposits found on coral islands 40-80 km to the east (in the direction of regional upper-tropospheric winds). Radiocarbon dating of charcoal below the Tofua ignimbrite and organic material below the related fall units imply this eruption sequence occurred post 1,000 years BP. We estimate an eruption magnitude of 2.24x10(13) kg, sulphur release of 12 Tg and tentatively assign this eruption to the AD 1030 volcanic sulphate spike recorded in Antarctic ice sheet records.

Combination aerosol therapy to treat Burkholderia cepacia complex

Burkholderia cepacia infection in cystic fibrosis (CF) patients is associated with significant morbidity and mortality, yet no definitive treatment is currently available. This report describes a new approach to treat B. cepacia infection in CF patients, using a combination of amiloride and tobramycin aerosols. Four adults with the typical clinical syndrome of CF were recruited after repeated positive sputum cultures for B. cepacia. Aerosols of amiloride and tobramycin were given three times daily for 1-6 months, and repeated sputum cultures were collected to assess efficacy. Three of the four patients treated with the combined therapy eradicated B. cepacia from their sputum cultures for at least 2 yrs, and there were no adverse events. This novel combination may provide a new therapeutic option for Burkholderia cepacia infections. Furthermore, the strategy of combining antibiotics with ion transport agents may have ramifications for the treatment of other multi-resistant organisms.

Cumulus momentum fluxes in cloud-resolving model simulations of toga-coare

O objectivo deste trabalho científico é o estudo do transporte vertical de momento linear horizontal (CMT) realizado por sistemas de nuvens de convecção profunda sobre o oceano tropical. Para realizar este estudo, foram utilizadas simulações tridimensionais produzidas por um modelo explícito de nuvens (CRM) para os quatro meses de duração da campanha observacional TOGA COARE que ocorreu sobre as águas quentes do Pacífico ocidental. O estudo foca essencialmente as características estatísticas e à escala da nuvem do CMT durante um episódio de fortes ventos de oeste e durante um período de tempo maior que incluí este evento de convecção profunda. As distribuições verticais e altitude-temporais de campos atmosféricos relacionados com o CMT são avaliadas relativamente aos campos observacionais disponíveis, mostrando um bom acordo com os resultados de estudos anteriores, confirmando assim a boa qualidade das primeiras e fornecendo a confiança necessária para continuar a investigação. A sensibilidade do CMT em relação do domínio espacial do model é analisada, utilizando dois tipos de simulações tridimensionais produzidas por domínios horizontais de diferente dimensão, sugerindo que o CMT não depende da dimensão do domínio espacial horizontal escolhido para simular esta variável. A capacidade da parameterização do comprimento de mistura simular o CMT é testada, destacando as regiões troposféricas onde os fluxos de momento linear horizontal são no sentido do gradiente ou contra o gradiente. Os fluxos no sentido do gradiente apresentam-se relacionados a uma fraca correlação entre os campos atmosféricos que caracterizam esta parameterização, sugerindo que as formulações dos fluxos de massa dentro da nuvem e o fenómeno de arrastamento do ar para dentro da nuvem devem ser revistos. A importância do ar saturado e não saturado para o CMT é estudada com o objectivo de alcançar um melhor entendimento acerca dos mecanismos físicos responsáveis pelo CMT. O ar não saturado e saturado na forma de correntes descendentes contribuem de forma determinante para o CMT e deverão ser considerados em futuras parameterizações do CMT e da convecção em nuvens cumulus. Métodos de agrupamento foram aplicados às contribuições do ar saturado e não saturado, analisando os campos da força de flutuação e da velocidade vertical da partícula de ar, concluindo-se a presença de ondas gravíticas internas como mecanismo responsável pelo ar não saturado. A força do gradiente de pressão dentro da nuvem é também avaliada, utilizando para este efeito a fórmula teórica proposta por Gregory et al. (1997). Uma boa correlação entre esta força e o produto entre efeito de cisalhamento do vento e a perturbação da velocidade vertical é registada, principalmente para as correntes ascendentes dentro da nuvem durante o episódio de convecção profunda. No entanto, o valor ideal para o coeficiente empírico c*, que caracteriza a influência da força do gradiente de pressão dentro da nuvem sobre a variação vertical da velocidade horizontal dentro da nuvem, não é satisfatoriamente alcançado. Bons resultados são alcançados através do teste feito à aproximação do fluxo de massa proposta por Kershaw e Gregory (1997) para o cálculo do CMT total, revelando mais uma vez a importância do ar não saturado para o CMT.

Contribution of biomass combustion to air pollutant emissions

In Portugal, it was estimated that around 1.95 Mton/year of wood is used in residential wood burning for heating and cooking. Additionally, in the last decades, burnt forest area has also been increasing. These combustions result in high levels of toxic air pollutants and a large perturbation of atmospheric chemistry, interfere with climate and have adverse effects on health. Accurate quantification of the amounts of trace gases and particulate matter emitted from residential wood burning, agriculture and garden waste burning and forest fires on a regional and global basis is essential for various purposes, including: the investigation of several atmospheric processes, the reporting of greenhouse gas emissions, and quantification of the air pollution sources that affect human health at regional scales. In Southern Europe, data on detailed emission factors from biomass burning are rather inexistent. Emission inventories and source apportionment, photochemical and climate change models use default values obtained for US and Northern Europe biofuels. Thus, it is desirable to use more specific locally available data. The objective of this study is to characterise and quantify the contribution of biomass combustion sources to atmospheric trace gases and aerosol concentrations more representative of the national reality. Laboratory (residential wood combustion) and field (agriculture/garden waste burning and experimental wildland fires) sampling experiments were carried out. In the laboratory, after the selection of the most representative wood species and combustion equipment in Portugal, a sampling program to determine gaseous and particulate matter emission rates was set up, including organic and inorganic aerosol composition. In the field, the smoke plumes from agriculture/garden waste and experimental wildland fires were sampled. The results of this study show that the combustion equipment and biofuel type used have an important role in the emission levels and composition. Significant differences between the use of traditional combustion equipment versus modern equipments were also observed. These differences are due to higher combustion efficiency of modern equipment, reflecting the smallest amount of particulate matter, organic carbon and carbon monoxide released. With regard to experimental wildland fires in shrub dominated areas, it was observed that the largest organic fraction in the samples studied was mainly composed by vegetation pyrolysis products. The major organic components in the smoke samples were pyrolysates of vegetation cuticles, mainly comprising steradienes and sterol derivatives, carbohydrates from the breakdown of cellulose, aliphatic lipids from vegetation waxes and methoxyphenols from the lignin thermal degradation. Despite being a banned practice in our country, agriculture/garden waste burning is actually quite common. To assess the particulate matter composition, the smoke from three different agriculture/garden residues have been sampled into 3 different size fractions (PM2.5, PM2.5-10 and PM>10). Despite distribution patterns of organic compounds in particulate matter varied among residues, the amounts of phenolics (polyphenol and guaiacyl derivatives) and organic acids were always predominant over other organic compounds in the organosoluble fraction of smoke. Among biomarkers, levoglucosan, β-sitosterol and phytol were detected in appreciable amounts in the smoke of all agriculture/garden residues. In addition, inositol may be considered as an eventual tracer for the smoke from potato haulm burning. It was shown that the prevailing ambient conditions (such as high humidity in the atmosphere) likely contributed to atmospheric processes (e.g. coagulation and hygroscopic growth), which influenced the particle size characteristics of the smoke tracers, shifting their distribution to larger diameters. An assessment of household biomass consumption was also made through a national scale survey. The information obtained with the survey combined with the databases on emission factors from the laboratory and field tests allowed us to estimate the pollutant amounts emitted in each Portuguese district. In addition to a likely contribution to the improvement of emission inventories, emission factors obtained for tracer compounds in this study can be applied in receptor models to assess the contribution of biomass burning to the levels of atmospheric aerosols and their constituents obtained in monitoring campaigns in Mediterranean Europe.

Application of the WRF-Chem Model for a High Ozone Episode in SW Poland – Preliminary Results

The Weather Research and Forecasting model, integrated online with chemistry module, is a multi-scale model suitable for both research and operational forecasts of meteorology and air quality. It is used by many institutions for a variety of applications. In this study, the WRF v3.5 with chemistry (WRF-Chem) is applied to the area of Poland, for a period of 3-20 July 2006, when high concentrations of ground level ozone were observed. The meteorological and chemistry simulations were initiated with ERA-Interim reanalysis and TNO MACC II emissions database, respectively. The model physical parameterization includes RRTM shortwave radiation, Kain-Fritsch cumulus scheme, Purdue Lin microphysics and ACM2 PBL, established previously as the optimal configuration. Chemical mechanism used for the study was RADM2 with MADE/SORGAM aerosols. Simulations were performed for three one-way nested domains covering Europe (36 km x 36 km), Central Europe (12 km x 12 km) and Poland (4 km x 4 km). The results from the innermost domain were analyzed and compared to measurements of ozone concentration at three stations in different environments. The results show underestimation of observed values and daily amplitude of ozone concentrations.

Aerosol-Radiation Feedback and PM10 Air Concentrations Over Poland

We have implemented the WRF-Chem model version 3.5 over Poland to quantify the direct and indirect feedback effects of aerosols on simulated meteorology and aerosol concentrations. Observations were compared with results from three simulations at high spatial resolutions of 5 × 5 km: (1) BASE—without any aerosol feedback effects; (2) DIR—with direct aerosol-radiative effects (3) INDIR—with direct and indirect aerosol-radiative effects. We study the overall effect during January 2011 as well as selected episodes of the highest differences in PM10 concentrations between the three simulations. For the DIR simulation, the decrease in monthly mean incoming solar radiation (SWDOWN) appears for the entire study area. It changes geographically, from about −8.0 to −2.0 W m−2, respectively for the southern and northern parts of the country. The highest changes do not correspond to the highest PM10 concentration. Due to the solar radiation changes, the surface mean monthly temperature (T2) decreases for 96 % of the area of Poland, but not more than 1.0 °C. Monthly mean PBLH changes by more than ±5 m for 53 % of the domain. Locally the differences in PBLH between the DIR and BASE are higher than ± 20 m. Due to the direct effect, for 84 % of the domain, the mean monthly PM10 concentrations increase by up to 1.9 µg m−3. For the INDIR simulation the spatial distribution of changes in incoming solar radiation as well as air temperature is similar to the DIR simulation. The decrease of SWDOWN is noticed for the entire domain and for 23 % of the domain is higher than −5.0 W m−2. The absolute differences of PBLH are slightly higher for INDIR than DIR but similarly distributed spatially. For daily episodes, the differences between the simulations are higher, both for meteorology and PM10 concentrations, and the pattern of changes is usually more complex. The results indicate the potential importance of the aerosol feedback effects on modelled meteorology and PM10 concentrations.