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There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements which can provide further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows for the characterisation of the inorganic components of PM10 and PM2.5 (NHC4+, NO3-, SO2-4, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP supersite, Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 µgm-3. Anthropogenically derived secondary inorganic aerosols (sum of NHC 4, NO3- and nss-SO2-4) were the dominating species (63%) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt was the main component (73%) of the PMcoarse fraction (PM10-PM2.5/, though NO3- was also found to make a relatively large contribution to the measured mass (17%) providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high KC concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations >12 µgm-3) were on average dominated by NHC 4 and NO3-, where smaller loadings at the site tended to be dominated by sea salt. As with other western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely that organic acids contributed to the charge balance. This study demonstrates the UK background atmospheric composition is primarily driven by meteorology with sea salt dominating air masses from the Atlantic Ocean and the Arctic, whereas secondary inorganic aerosols tended to dominate air masses from continental Europe. [ABSTRACT FROM AUTHOR]

Leaf nitrogen and leaf surface area influence the exchange of gases between terrestrial ecosystems and the atmosphere, and play a significant role in the global cycles of carbon, nitrogen and water. The purpose of this study is to use field-based and satellite remote-sensing-based methods to assess leaf nitrogen pools in five diverse European agricultural landscapes located in Denmark, Scotland (United Kingdom), Poland, the Netherlands and Italy. REGFLEC (REGularized canopy reFLECtance) is an advanced image-based inverse canopy radiative transfer modelling system which has shown proficiency for regional mapping of leaf area index (LAI) and leaf chlorophyll (CHLl) using remote sensing data. In this study, high spatial resolution (10-20 m) remote sensing images acquired from the multispectral sensors aboard the SPOT (Satellite For Observation of Earth) satellites were used to assess the capability of REGFLEC for mapping spatial variations in LAI, CHL1 and the relation to leaf nitrogen (N1) data in five diverse European agricultural landscapes. REGFLEC is based on physical laws and includes an automatic model parameterization scheme which makes the tool independent of field data for model calibration. In this study, REGFLEC performance was evaluated using LAI measurements and non-destructive measurements (using a SPAD meter) of leaf-scale CHL1 and N1 concentrations in 93 fields representing crop- and grasslands of the five landscapes. Furthermore, empirical relationships between field measurements (LAI, CHL1 and N1) and five spectral vegetation indices (the Normalized Difference Vegetation Index, the Simple Ratio, the Enhanced Vegetation Index-2, the Green Normalized Difference Vegetation Index, and the green chlorophyll index) were used to assess field data coherence and to serve as a comparison basis for assessing REGFLEC model performance. The field measurements showed strong vertical CHL1 gradient profiles in 26% of fields which affected REGFLEC performance as well as the relationships between spectral vegetation indices (SVIs) and field measurements. When the range of surface types increased, the REGFLEC results were in better agreement with field data than the empirical SVI regression models. Selecting only homogeneous canopies with uniform CHL1 distributions as reference data for evaluation, REGFLEC was able to explain 69% of LAI observations (rmse=0.76), 46% of measured canopy chlorophyll contents (rmse=719 mgm-2) and 51% of measured canopy nitrogen contents (rmse=2.7 gm-2). Better results were obtained for individual landscapes, except for Italy, where REGFLEC performed poorly due to a lack of dense vegetation canopies at the time of satellite recording. Presence of vegetation is needed to parameterize the REGFLEC model. Combining REGFLEC- and SVI-based model results to minimize errors for a "snap-shot" assessment of total leaf nitrogen pools in the five landscapes, results varied from 0.6 to 4.0 t km-2. Differences in leaf nitrogen pools between landscapes are attributed to seasonal variations, extents of agricultural area, species variations, and spatial variations in nutrient availability. In order to facilitate a substantial assessment of variations in N1 pools and their relation to landscape based nitrogen and carbon cycling processes, time series of satellite data are needed. The upcoming Sentinel-2 satellite mission will provide new multiple narrowband data opportunities at high spatio-temporal resolution which are expected to further improve remote sensing capabilities for mapping LAI, CHL1 and N1. [ABSTRACT FROM AUTHOR]

Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea salt sulfate 2% nitrate, 7% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea salt signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acids/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25 %), a marine oxygenated OA factor (M-OOA, 40 %), a sea salt OA fraction (SS-OA, 7 %) and locally produced hydrocarbon-like OA (HOA, 9 %). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (C :N ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea salt aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated to sea salt particles during 19% of the time, indicating the presence of biogenic particles in addition to the MSA-OA and AA-OA factors. [ABSTRACT FROM AUTHOR]

Leaf nitrogen and leaf surface area influence the exchange of gases between terrestrial ecosystems and the atmosphere, and they play a significant role in the global cycles of carbon, nitrogen and water. Remote sensing data from satellites can be used to estimate leaf area index (LAI), leaf chlorophyll (CHLl) and leaf nitrogen density (Nl). However, methods are often developed using plot scale data and not verified over extended regions that represent a variety of soil spectral properties and canopy structures. In this paper, field measurements and high spatial resolution (10-20m) remote sensing images acquired from the HRG and HRVIR sensors aboard the SPOT satellites were used to assess the predictability of LAI, CHLl and Nl. Five spectral vegetation indices (SVIs) were used (the Normalized Difference Vegetation index, the Simple Ratio, the Enhanced Vegetation Index-2, the Green Normalized Difference Vegetation Index, and the green Chlorophyll Index) together with the image-based inverse canopy radiative transfer modelling system, REGFLEC (REGularized canopy reFLECtance). While the SVIs require field data for empirical model building, REGFLEC can be applied without calibration. Field data measured in 93 fields within crop- and grasslands of five Euro- pean landscapes showed strong vertical CHLl gradient profiles in 20% of fields. This affected the predictability of SVIs and REGFLEC. However, selecting only homogeneous canopies with uniform CHLl distributions as reference data for statistical evaluation, significant (p < 0.05) predictions were achieved for all landscapes, by all methods. The best performance was achieved by REGFLEC for LAI (r² = 0.7; rmse=0.73), canopy chlorophyll content (r² = 0.51; rmse=439mg m-2 ) and canopy nitrogen con- tent (r² = 0.53; rmse=2.21 gm-2 ). Predictabilities of SVIs and REGFLEC simulations generally improved when constrained to single land use categories (wheat, maize, bar- ley, grass) across the European landscapes, reflecting sensitivity to canopy structures. Predictability further improved when constrained to local (10x10 km² ) landscapes, thereby reflecting sensitivity to local environmental conditions. All methods showed different predictabilities for land use categories and landscapes. Combining the best methods, LAI, canopy chlorophyll content (CHLc) and canopy nitrogen content (Nc) for the five landscapes could be predicted with improved accuracy (LAI rmse=0.59; CHLc rmse=346 gm-2; Nc rmse=1.49 gm-2 ). Remote sensing-based results showed that the vegetation nitrogen pools of the five agricultural landscapes varied from 0.6 to 4.0 tkm-2. Differences in nitrogen pools were attributed to seasonal variations, extents of agricultural area, species variations, and spatial variations in nutrient availability. Information on Nl and total Nc pools within the landscapes is important for the spatial evaluation of nitrogen and carbon cycling processes. The upcoming Sentinel-2 satellite mission will provide new multiple narrow-band data opportunities at high spatioemporal resolution which are expected to further improve remote sensing predictabilities of LAI, CHLl and Nl. [ABSTRACT FROM AUTHOR]

A comprehensive assessment of nitrogen (N) flows at the landscape scale is fundamental to understand spatial interactions in the N cascade and to inform the development of locally optimised N management strategies. To explore this interactions, complete N budgets were estimated for two contrasting hydrological catchments (dominated by agricultural grassland vs. semi-natural peat-dominated moorland), forming part of an intensively studied landscape in southern Scotland. Local scale atmospheric dispersion modelling and detailed farm and field inventories provided high resolution estimations of input fluxes. Agricultural inputs (i.e. grazing excreta, organic and synthetic fertiliser) accounted for most of the catchment N inputs with 80% in the grassland and 57% in the moorland catchment, while atmospheric deposition made a significant contribution, particularly in the moorland catchment with 38% of the N inputs. The estimated catchment N budgets highlighted areas of key uncertainty, particularly N2 emissions from denitrification and stream N export. The resulting N balances suggest that the study catchments have a limited capacity to store N within soils, vegetation and groundwater. The "catchment N retention", i.e. the amount of N which is either stored within the catchment or lost through atmospheric emissions, was estimated to be 3% of the net anthropogenic input in the moorland and 55% in the grassland catchment. These values contrast with regional scale estimates: catchment retentions of net anthropogenic input estimated within Europe at the regional scale range from 50% to 90% with an average of 82% (Billen et al., 2011). This study emphasises the need for detailed budget analyses to identify the N status of European landscapes. [ABSTRACT FROM AUTHOR]

The phase transitions and hygroscopic growth of two humic acid aerosols (Aldrich sodium salt and Leonardite Standard (IHSS)) and their mixtures with ammonium sulphate have been investigated using a combination of two techniques, Fourier transform infra-red (FTIR) spectroscopy and tandem differential mobility analysis (TDMA). A growth factor of 1.16 at 85% relative humdity (RH) was found for the Aldrich humic acid which can be regarded as an upper limit for growth factors of humic-like substances (HULIS) found in atmospheric aerosol and is significantly smaller than that of typical atmospheric inorganics. We find that the humic acid aerosols exhibit water uptake over all relative humidites with no apparent phase changes, suggesting that these aerosols readily form supersaturated droplets. In the mixed particles, the humic acid component decreases the deliquescence relative humidity (DRH) and increases the efflorescence relative humidity (ERH) of the ammonium sulphate component, and there is some degree of water uptake prior to ammonium sulphate deliquescence. In addition, at low RH, the FTIR spectra show that the ammonium is present in a different chemical environment in the mixed aerosols than in crystalline ammonium sulphate, perhaps existing as a complex with the humic materials. The growth factors of the mixed aerosols are intermediate between those of the single component aerosols and can be predicted assuming that the inorganic and organic fractions take up water independently. [ABSTRACT FROM AUTHOR]