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: 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: 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: A high resolution (5×5 km2) UK-scale chemistry-transport model (EMEP4UK) is used to study ground-level ozone (O3) during the 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 observed annual and diurnal cycles of surface O3 at urban and rural sites. Elevated O3 and much of its day-to-day variability during the heat-wave are well captured. Key O3 precursors, nitrogen dioxide and isoprene (C5H8), 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. Dry deposition of O3, when completely switched off, elevated simulated O3 by up to 50 ppb, and this may have been an important factor on several days. Modelled C5H8 concentrations are generally best simulated if C5H8 emissions are changed from the base emissions: typically doubled, but elevated by up to a factor of five on some days. Accurately modelling the exact positions of individual plumes of anthropogenically emitted nitrogen oxides and volatile organic compounds is crucial for the successful simulation of O3 at a particular time and location. Variations in surface temperature of ±5 K were found to have impacts on O3 of typically less than ±10 ppb.

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.

Description: The Fine Resolution Atmospheric Multi-pollutant Exchange model (FRAME) was applied to model the spatial distribution of reactive nitrogen deposition and air concentration over the United Kingdom 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 reactive 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.