ALBERT

Description: Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model and evaluated against measurements. Gas/particle partitioning in the EMEP4UK model simulations used a bulk approach, which may lead to uncertainties in simulated secondary inorganic aerosol. However, model simulations were able to accurately represent both the long-term decadal surface concentrations of particle sulfate and nitrate and an episode in early 2003 of substantially elevated nitrate measured across the UK by the AGANet network. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological: a persistent high-pressure system, whose varying location impacted the relative importance of transboundary versus domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and southeast, may be close to or exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on particulate matter concentrations and the need for international agreements to address the transboundary component of air pollution.

Description: The EMEP4UK modelling system is a high resolution (5×5 km2) application of the EMEP chemistry-transport model, designed for scientific and policy studies in the UK. We demonstrate the use and performance of the EMEP4UK system through the study of ground-level ozone (O3) during the extreme August 2003 heat-wave. Meteorology is generated by the Weather Research and Forecast (WRF) model, nudged every six hours with reanalysis data. We focus on SE England, where hourly average O3 reached up to 140 ppb during the heat-wave. EMEP4UK accurately reproduces elevated O3 and much of its day-to-day variability during the heat-wave. Key O3 precursors, nitrogen dioxide and isoprene, are less well simulated, but show generally accurate diurnal cycles and concentrations to within a factor of ~2–3 of observations. The modelled surface O3 distribution has an intricate spatio-temporal structure, governed by a combination of meteorology, emissions and photochemistry. A series of sensitivity runs with the model are used to explore the factors that influenced O3 levels during the heat-wave. Various factors appear to be important on different days and at different sites. Ozone imported from outside the model domain, especially the south, is very important on several days during the heat-wave, contributing up to 85 ppb. The effect of dry deposition is also important on several days. Modelled isoprene concentrations are generally best simulated if isoprene emissions are changed from the base emissions: typically doubled, but elevated by up to a factor of five on one hot day. We found that accurate modelling of the exact positions of nitrogen oxide and volatile organic compound plumes is crucial for the successful simulation of O3 at a particular time and location. Variations in temperature of ±5 K were found to have impacts on O3 of typically less than ±10 ppb.

Description: Base cations exert a large impact on various geochemical and geophysical processes both in the atmosphere and at the Earth surface. One of the essential roles of these compounds is impact on surface pH causing an increase in alkalinity and neutralizing the effects of acidity generated by sulphur and nitrogen deposition. During recent years anthropogenic emissions of base cations in the UK have decreased substantially, by about 70%, 78%, 75% and 48% for Na+, Mg2+, Ca2+ and K+, respectively, over the period 1990–2006. For the island regions, such as the UK, the main source of base cation particles is the aerosol produced from the sea surface. Here, the sea salt aerosol (SSA) emissions are calculated with parameterisations proposed by Mårtensson et al. (2003) for ultra fine particles, Monahan et al. (1986) for fine particles and Smith and Harisson (1998) for coarse particles continuously with a 0.1 μm size step using WRF-modelled wind speed data at a 5 km × 5 km grid square resolution with a 3 h time step for two selected years 2003 and 2006. SSA production has been converted into base cation emissions, with the assumption that the chemical composition of the particle emitted from the sea surface is equal to the chemical composition of sea water, and used as input data in the Fine Resolution Atmospheric Multi-pollutant Exchange Model (FRAME). FRAME model annual mean concentrations and total wet deposition at a 5 km × 5 km grid resolution, are compared with concentrations in air and wet deposition from the National Monitoring Network and measurements based estimates of UK deposition budget. The correlation coefficient for wet deposition achieves high values (R = 0.8) for Na+ and Mg2+, whereas for Ca2+ the correlation is poor (R 〈 0.3). Base cation concentrations are also represented well, with some overestimations on the west coast and underestimations in the centre of the land.

Description: Marine N2 fixing microorganisms, termed diazotrophs, are a key functional group in marine pelagic ecosystems. The biological fixation of dinitrogen (N2) to bioavailable nitrogen provides an important new source of nitrogen for pelagic marine ecosystems and influences primary productivity and organic matter export to the deep ocean. As one of a series of efforts to collect biomass and rates specific to different phytoplankton functional groups, we have constructed a database on diazotrophic organisms in the global pelagic upper ocean by compiling about 12 000 direct field measurements of cyanobacterial diazotroph abundances (based on microscopic cell counts or qPCR assays targeting the nifH genes) and N2 fixation rates. Biomass conversion factors are estimated based on cell sizes to convert abundance data to diazotrophic biomass. The database is limited spatially, lacking large regions of the ocean especially in the Indian Ocean. The data are approximately log-normal distributed, and large variances exist in most sub-databases with non-zero values differing 5 to 8 orders of magnitude. Reporting the geometric mean and the range of one geometric standard error below and above the geometric mean, the pelagic N2 fixation rate in the global ocean is estimated to be 62 (52–73) Tg N yr−1 and the pelagic diazotrophic biomass in the global ocean is estimated to be 2.1 (1.4–3.1) Tg C from cell counts and to 89 (43–150) Tg C from nifH-based abundances. Reporting the arithmetic mean and one standard error instead, these three global estimates are 140 ± 9.2 Tg N yr−1, 18 ± 1.8 Tg C and 590 ± 70 Tg C, respectively. Uncertainties related to biomass conversion factors can change the estimate of geometric mean pelagic diazotrophic biomass in the global ocean by about ±70%. It was recently established that the most commonly applied method used to measure N2 fixation has underestimated the true rates. As a result, one can expect that future rate measurements will shift the mean N2 fixation rate upward and may result in significantly higher estimates for the global N2 fixation. The evolving database can nevertheless be used to study spatial and temporal distributions and variations of marine N2 fixation, to validate geochemical estimates and to parameterize and validate biogeochemical models, keeping in mind that future rate measurements may rise in the future. The database is stored in PANGAEA (doi:10.1594/PANGAEA.774851).

Description: Marine N2 fixing microorganisms, termed diazotrophs, are a key functional group in marine pelagic ecosystems. The biological fixation of dinitrogen (N2) to bioavailable nitrogen provides an important new source of nitrogen for pelagic marine ecosystems and influences primary productivity and organic matter export to the deep ocean. As one of a series of efforts to collect biomass and rates specific to different phytoplankton functional groups, we have constructed a database on diazotrophic organisms in the global pelagic upper ocean by compiling about 12 000 direct field measurements of cyanobacterial diazotroph abundances (based on microscopic cell counts or qPCR assays targeting the nifH genes) and N2 fixation rates. Biomass conversion factors are estimated based on cell sizes to convert abundance data to diazotrophic biomass. The database is limited spatially, lacking large regions of the ocean especially in the Indian Ocean. The data are approximately log-normal distributed, and large variances exist in most sub-databases with non-zero values differing 5 to 8 orders of magnitude. Lower mean N2 fixation rate was found in the North Atlantic Ocean than the Pacific Ocean. Reporting the geometric mean and the range of one geometric standard error below and above the geometric mean, the pelagic N2 fixation rate in the global ocean is estimated to be 62 (53–73) Tg N yr−1 and the pelagic diazotrophic biomass in the global ocean is estimated to be 4.7 (2.3–9.6) Tg C from cell counts and to 89 (40–200) Tg C from nifH-based abundances. Uncertainties related to biomass conversion factors can change the estimate of geometric mean pelagic diazotrophic biomass in the global ocean by about ±70%. This evolving database can be used to study spatial and temporal distributions and variations of marine N2 fixation, to validate geochemical estimates and to parameterize and validate biogeochemical models. The database is stored in PANGAEA (http://doi.pangaea.de/10.1594/PANGAEA.774851).

Description: Simulation of atmospheric nitrogen (N) deposition in the North China Plain (NCP) at high resolution, 5 × 5 km2, was conducted for the first time by the Fine Resolution Atmospheric Multi-pollutant Exchange (FRAME) model. The total N deposition budget was 1481 Gg in this region, with 77 % from reduced N and 23 % from oxidized N, and the annual deposition rate (47 kg ha−1) was much higher than previously reported values for other parts of the world such as the UK (13 kg ha−1), Poland (7.3 kg ha−1) and EU27 (8.6 kg ha−1). The exported N budget (1981 Gg) was much higher than the imported N budget (584 Gg), suggesting that the NCP is an important net emission source of N pollutants. Seven provinces in the region contributed N deposition budgets that were proportional to their area ratios. The calculated spatial distributions of N deposition displayed high rates of reduced N deposition in the south and of oxidized N deposition in the eastern part. The N deposition exceeded an upper limit of 30 kg N ha−1 for natural ecosystems over more than 90 % of the region, resulting in terrestrial ecosystem deterioration, impaired air quality and coastal eutrophication not only in the NCP itself but also in surrounding areas including the Bohai Sea and the Yellow Sea.

Description: The Fine Resolution Atmospheric Multi-pollutant Exchange model (FRAME) has been applied to model the spatial distribution of nitrogen deposition and air concentration over the UK at a 1 km spatial resolution. The modelled deposition and concentration data were gridded at resolutions of 1 km, 5 km and 50 km to test the sensitivity of calculations of the exceedance of critical loads for nitrogen deposition to the deposition data resolution. The modelled concentrations of NO2 were validated by comparison with measurements from the rural sites in the national monitoring network and were found to achieve better agreement with the high resolution 1 km data. High resolution plots were found to represent a more physically realistic distribution of nitrogen air concentrations and deposition resulting from use of 1 km resolution precipitation and emissions data as compared to 5 km resolution data. Summary statistics for national scale exceedance of the critical load for nitrogen deposition were not highly sensitive to the grid resolution of the deposition data but did show greater area exceedance with coarser grid resolution due to spatial averaging of high nitrogen deposition hot spots. Local scale deposition at individual Sites of Special Scientific Interest and high precipitation upland sites was sensitive to choice of grid resolution of deposition data. Use of high resolution data tended to generate lower deposition values in sink areas for nitrogen dry deposition (Sites of Scientific Interest) and higher values in high precipitation upland areas. In areas with generally low exceedance (Scotland) and for certain vegetation types (montane), the exceedance statistics were more sensitive to model data resolution.

Description: 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.

Description: Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model. In early 2003 an episode of substantially elevated surface concentrations of ammonium nitrate was measured across the UK by the AGANET network. The EMEP4UK model was able accurately to represent both the long-term decadal surface concentrations and the episode in 2003. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological, a persistent high pressure system, but whose varying location impacted the relative importance of transboundary vs. domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and south-east, may be close to or actually exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on PM concentrations and the need for international agreements to address the transboundary component of air pollution.

Description: Base cations exerts a large impact on various geochemical and geophysical processes both in the atmosphere and at the Earth surface. One of the essential roles of these compounds is impact on surface pH causing an increase in alkalinity and neutralizing the effects of acidity generated by sulphur and nitrogen deposition. During recent years anthropogenic emissions of base cations in the UK have decreased substantially, by about 70% for Na+, 78% for Mg2+, 75% for Ca2+ and about 48% for K+ for the period 1990–2006. For the island regions, such as the is UK, the main source of base cation particles is the aerosol produced from the sea surface. Here, the sea salt aerosol (SSA) emissions are calculated with parameterisations proposed by Maårtensson et al. (2003); ultra fine particles, Monahan et al. (1986); fine particles and Smith and Harisson (1998); coarse particles continuously with a 0.1 μ m size step using WRF-modelled wind speed data at a 5 km × 5 km grid square resolution with a 3 h time step for two selected years 2003 and 2006. SSA production has been converted into base cation emissions, with the assumption that the chemical composition of the particle emitted from the sea surface is equal to the chemical composition of sea water, and used as input data in the Fine Resolution Atmospheric Multi-pollutant Exchange Model (FRAME). FRAME model results, yearly mean concentrations and total wet deposition at a 5 km × 5 km grid resolution, are compared with concentrations in air and wet deposition from the National Monitoring Network and measurements based estimates of UK deposition budget. The correlation coefficient for wet deposition achieves high values for Na+ and Mg2+, and for Ca2+ there is significant scattering. Base cation concentration is also represented well, with some overestimations on the west coast and underestimations in the centre of the land.