Julian Aherne

Parallelisation and application of a multi-layer atmospheric transport model to quantify dispersion and deposition of ammonia over the British Isles

An atmospheric transport model, FRAME (Fine Resolution AMmonia Exchange), has been used to model the spatial pattern of ammonia concentrations and deposition over the British Isles for the first time. The model uses a multi-layer approach with diffusion through 33 layers to describe vertical concentration profiles in the atmosphere explicitly. Together with the necessary description of atmospheric reactions with sulphur and oxidised nitrogen, this imposes a major computational requirement, with the model having a run-time of 8.5 days on a mid-range workstation. Improvement in the model run-time was sought by developing a parallel implementation coded in a data-parallel approach using High Performance Fortran. Running the code on a Cray T3E with 128 processors provided a speedup by a factor of 69. The codes portability, its validation with measurements and new maps of its application to the British Isles, are presented. Good agreement is found with measured NH3 concentrations, while wet de-position is underestimated. In addition to model uncertainties, this may be due to an underestimation of the NH3 emissions input data.

Controls on greenhouse gas concentrations in polymictic headwater lakes in Ireland

Freshwater lakes are known to release carbon dioxide (CO(2)) and methane (CH(4)) to the atmosphere; however, the importance of lakes in global nitrous oxide (N(2)O) budgets is not yet known. Further, despite the abundance of small lakes on the landscape, neither emissions of these gases nor their drivers are well described. Dissolved concentrations of CO(2), CH(4) and N(2)O greenhouse gases were related to water chemistry, hydrology and catchment characteristics in order to identify factors controlling gas concentrations for 121 small Irish headwater lakes (median area: 2.0ha) in relatively undisturbed catchments; lake-atmosphere gas fluxes were also calculated. The majority of lakes were supersaturated (relative to the atmosphere) with CO(2) and N(2)O while CH(4) was above saturation in all lakes. Dissolved gas concentrations were correlated with land cover (rock, forest and grassland), deuterium excess (an indicator of hydrologic character) and lake organic carbon concentrations, although dissolved CO(2) exhibited few significant relationships. Principal components analysis indicated that higher levels of CH(4) and N(2)O supersaturation were exhibited under different conditions. Methane supersaturation was highest in low elevation catchments with an evaporative hydrologic character and high organic carbon concentrations. In contrast, lakes characteristic of N(2)O supersaturation were low in carbon and located in more rapidly flushed higher elevation catchments. Estimated fluxes of CO(2), CH(4) and N(2)O to the atmosphere averaged 14, 0.36 and 1.3×10(-3)mmolm(-2)d(-1), respectively.

A survey of lakes in the Republic of Ireland: hydrochemical characteristics and acid sensitivity.

Abstract In 1997, as part of a national program to determine and map critical loads, a lake survey was carried out in the Republic of Ireland. In total 200 lakes were sampled, which represents approximately 3.3% of the total lake population. The majority of lakes were situated in remote, high-altitude, acid-sensitive areas along the coastal margins of the country. Lake chemistry was dominated by marine inputs. Approximately 50% of the lakes had DOC > 5 mg L−1 due to the presence of organic soils in a large proportion of the catchments. Nonmarine sulfate concentrations were at background levels (< 20 µeq L−1) in 50% of the lakes. Exceedance of critical load was observed in 7% of the sampled lakes (13 lakes). However, there are uncertainties in the critical load calculations due to the interference of sea salts and organic acids; accurate estimation under such conditions requires long-term lake and deposition chemistry.

Nitrogen deposition and exceedance of critical loads for nutrient nitrogen in Irish grasslands

High resolution nitrogen (N) deposition maps were developed to assess the exceedance of empirical critical loads of nutrient N for grasslands in Ireland. Nitrogen emissions have remained relatively constant during the past 20 yrs and are projected to remain constant under current legislation. Total N deposition (estimated as wet nitrate [NO3(-)] and ammonium [NH4(+)] plus dry NO× and NH3) ranged from 2 to 22 kg Nha(-1)yr(-1) (mean=12 kg Nha(-1)yr(-1)) to grasslands. Empirical critical loads for nutrient N were set at 15 kg Nha(-1)yr(-1) for both acid and calcareous grasslands; exceedance was observed for ~35% (~2,311 km(2)) of mapped acid grasslands. In contrast, only ~9% of calcareous grasslands (~35 km(2)) received N deposition in excess of the critical load. Reduced N deposition (primarily dry NH3) represented the dominant form to grasslands (range 55-90%) owing to significant emissions associated with livestock (primarily cattle). The extent of exceedance in acid grasslands suggests that N deposition to this habitat type may lead to adverse impacts such as a decline in plant species diversity and soil acidification. Further, given that elevated N deposition was dominated by NH3 associated with agricultural emissions rather than long-range transboundary sources, future improvements in air quality need to be driven by national policies.

Past, present, and future exceedance of critical loads of acidity for surface waters in Finland.

A critical load is a deposition limit below which harmful effects for a given ecosystem do not occur; the approach has underpinned European sulfur (S) and nitrogen (N) effects-based emission reduction policies during the last two decades. Surface waters are an important resource in Finland, as such the development of models and determination of critical loads has played a central role in supporting their recovery from acidification or preservation of ecosystem health. Critical loads of acidity for Finnish lakes were determined using the steady-state First-order Acidity Balance (FAB) model in conjunction with comprehensive national surveys of surface waters (headwater lakes; n = 1066) and soils. In the 1980s almost 60% of the study lakes were exceeded, impacting brown trout and perch populations. The steep decline in emissions and acidic (S and N) deposition during the last two decades has reduced exceedance to <10%, and by 2020 exceedance is predicted to reach preindustrial (1880) levels. In concert with these reductions, chemical and biological recovery has been observed. The critical load approach has been instrumental in assessing impacts to surface waters in Finland and directing effects-based emission reduction policies.

Critical loads of acidity for Irish lakes

Abstract. Critical loads of acidity have been estimated for Irish lakes (277) using survey data from the Republic of Ireland and Northern Ireland, and compatible inputs and methods across both regions. This is the first trans-region application of the Steady-State Water Chemistry model for the island of Ireland. Results indicate that a small percentage of lakes (10.8%, 30 lakes) have low critical loads of acidity (<50.0 mmolc m–2 yr–1). Based on bulk sulphate deposition, exceedance of critical load was observed in 6.9% of the sampled lakes (19 lakes). Inferences relating to the whole lake population cannot be made, as statistical lake surveys were not carried out. However, as the surveys were weighted towards acid-sensitive lakes, the current study suggests that Irish lakes are not under a significant threat from anthropogenic acidification. The acidifying impact of nitrogen was incorporated into the exceedance calcula tion by superimposing the present leaching of nitrogen onto sulphate deposition. This increased exceedance by 40% (i.e., from 11 to 19 lakes). Despite the potential uncertainties associated with using default values and relationships in the Steady-State Water Chemistry model, uncertainty analysis indicated that the critical loads were relatively stable. The critical acid neutralising capacity limit (specified water quality criterion) had the greatest effect on the critical load. In the current study, a catchment dependent limit was employed (ranged: 0–50 μmolc L–1; mean: 35 μmolc L–1) rather than a single fixed value.

Long-Term Monitoring of Atmospheric Deposition and the Implications of Ionic Inputs for the Sustainability of a Coniferous Forest Ecosystem

Ionic fluxes in a semi-mature stand of Sitka spruce (Picea sitchensis (Bong.) Carr.), on a spodosol in eastern Ireland, were monitored over an eight-year period, 1991-1998. The paper focuses on the long-term viability of forests in this region. Input-output balances, proton budgets and critical loads suggest that the long-term sustainability of forests in the region is threatened unless atmospheric emissions of anthropogenic substances can be controlled.

The Importance of Selecting Appropriate Criteria for Calculating Acidity Critical Loads for Terrestrial Ecosystems Using the Simple Mass Balance Equation

The Simple Mass Balance (SMB) equationis commonly used throughout Europe for thecalculation of acidity critical loads for forestsoils. Different criteria can be set in themodel depending on whether the receptor (e.g. treeroots) is more sensitive to the toxic effects ofaluminium or to unfavourable pH conditions. Thispaper examines the effects on critical loadscalculations of using different criteria andcritical limits, and demonstrates the importanceof selecting the most appropriate and justifiablecriteria for the chosen receptor, since they caneffect the critical loads values obtained. Abrief review of the range of different criteriaand limits used throughout Europe is included. In addition, the gibbsite equilibrium constant,used in the SMB equation to represent therelationship between dissolved aluminium andhydrogen ions in soil solution, is discussed. This relationship is not generally described inthe literature as a criterion in the equation,but this work highlights the effects differentgibbsite values have on critical loadcalculations and the importance of applying themost appropriate value for the soil in therooting zone of the receptor.

Critical Loads of Acidity for Surface Waters in South-Central Ontario, Canada: Regional Application of the First-Order Acidity Balance (FAB) Model

Major sulphur emission control programs have been implemented in North America, resulting in current emissions being ∼30% less than those in 1980. However, the level of acidic deposition remaining is still unlikely to promote widespread recovery of aquatic ecosystems. The First-order Acidity Balance (FAB) model has been applied to south-central Ontario (285 lakes in the Muskoka River Catchment) to evaluate the need for further reductions in emissions. As a result of the past decline in deposition, the proportion of lakes with critical loads exceedance has dropped substantially; however, further reductions in sulphur and nitrogen emissions are required to eliminate critical loads exceedance. Based on bulk deposition of sulphate and nitrogen (41.1 mmolc m-2 yr-1 and 62.5 mmolc m-2 yr-1, respectively) for the period 1995–1999, 166 lakes (58.3%) exceedcritical loads. Even with full implementation of SO2 abatementprograms in Canada (achieved in 1994) and the United States (legislated for 2010), critical loads will be exceeded in a large proportion (46.6%) of the study lakes.

Investigating the Uncertainties in the Simple Mass Balance Equation for Acidity Critical Loads for Terrestrial Ecosystems in the United Kingdom

The Simple Mass Balance (SMB)equation has been developed and used as one ofthe principal methods for calculating criticalloads of acidity for forest ecosystems. Criticalloads have formed the basis for informing policyrelated to the control and abatement of emissionsof acidifying pollutants. The SMB equationrelies on a variety of assumptions and dataderived from a variety of sources. Each of thesecomponent constituents has a potential source oferror depending on the method(s) used for theirderivation and the value(s) assigned. The resultis the possibility of generating a range ofcritical load values for a single ecosystem. This paper summarises the SMB equation, examinesthe uncertainties in deriving input values andreviews other works on the key assumptions.