Six-year observations of aerosol optical properties at a southern African grassland savannah site

Atmospheric aerosols have a significant effect on earth's radiative budget, particularly on regional scales. This paper presents a similar to 6 year, in situ, ground level aerosol scattering and absorption dataset, measured at a background site strategically positioned to enable differentiation of the effect of anthropogenic, population density and open biomass burning activities on a regional scale. Relatively well-defined seasonal and diurnal patterns were observed for all the aerosol optical properties, i.e. scattering coefficient (sigma(SP)), absorption coefficient (sigma(AP)), single scattering albedo (omega(0)) and Angstrom exponent of scattering (sigma(SP)). These patterns were explained by considering southern African specific sources and metrological conditions. Using a receptor modelling method (auto-generated source maps) it was found that air masses that had higher sigma(SP), sigma(AP) and omega(0), and lower alpha(SP), if compared with the relatively clean background, passed over source regions with significant industrial or other anthropogenic activities, higher population density, re-circulation of polluted air masses and higher open biomass burning frequency. To quantify differences, four source regions were defined, i.e. Karoo, Kalahari, anti-cyclonic recirculation pattern and the industrial hub of South Africa. Air masses that had passed over the Karoo source region represented the cleanest regional background conditions, while air masses that had passed either over the industrial hub and/or the anti-cyclonic recirculation pattern represented the most significant anthropogenically impacted, as indicated by the aerosol optical properties. The omega(0) medians of air masses that had passed over the Karoo (0.80-0.86) were 9, 12 and 7% lower than in air masses that had passed over source regions with the highest omega(0) median, in the warmest/wettest, coldest, and driest, peak open biomass burning periods, respectively.Peer reviewe

Size-resolved characteristics of inorganic ionic species in atmospheric aerosols at a regional background site on the South African Highveld

Aerosols consist of organic and inorganic species, and the composition and concentration of these species depends on their sources, chemical transformation and sinks. In this study an assessment of major inorganic ions determined in three aerosol particle size ranges collected for 1year at Welgegund in South Africa was conducted. SO42- and ammonium (NH4+) dominated the PM1 size fraction, while SO42- and nitrate (NO3) dominated the PM1-2.5 and PM2.5-10 size fractions. SO42- had the highest contribution in the two smaller size fractions, while NO3- had the highest contribution in the PM2.5-10 size fraction. SO42- and NO3- levels were attributed to the impacts of aged air masses passing over major anthropogenic source regions. Comparison of inorganic ion concentrations to levels thereof within a source region influencing Welgegund, indicated higher levels of most species within the source region. However, the comparative ratio of SO42- was significantly lower due to SO42- being formed distant from SO2 emissions and submicron SO42- having longer atmospheric residencies. The PM at Welgegund was determined to be acidic, mainly due to high concentrations of SO42-. PM1 and PM1-2.5 fractions revealed a seasonal pattern, with higher inorganic ion concentrations measured from May to September. Higher concentrations were attributed to decreased wet removal, more pronounced inversion layers trapping pollutants, and increases in household combustion and wild fires during winter. Back trajectory analysis also revealed higher concentrations of inorganic ionic species corresponding to air mass movements over anthropogenic source regions.Peer reviewe

Size-resolved characteristics of inorganic ionic species in atmospheric aerosols at a regional background site on the South African Highveld

Aerosols consist of organic and inorganic species, and the composition and concentration of these species depends on their sources, chemical transformation and sinks. In this study an assessment of major inorganic ions determined in three aerosol particle size ranges collected for 1year at Welgegund in South Africa was conducted. SO42- and ammonium (NH4+) dominated the PM1 size fraction, while SO42- and nitrate (NO3) dominated the PM1-2.5 and PM2.5-10 size fractions. SO42- had the highest contribution in the two smaller size fractions, while NO3- had the highest contribution in the PM2.5-10 size fraction. SO42- and NO3- levels were attributed to the impacts of aged air masses passing over major anthropogenic source regions. Comparison of inorganic ion concentrations to levels thereof within a source region influencing Welgegund, indicated higher levels of most species within the source region. However, the comparative ratio of SO42- was significantly lower due to SO42- being formed distant from SO2 emissions and submicron SO42- having longer atmospheric residencies. The PM at Welgegund was determined to be acidic, mainly due to high concentrations of SO42-. PM1 and PM1-2.5 fractions revealed a seasonal pattern, with higher inorganic ion concentrations measured from May to September. Higher concentrations were attributed to decreased wet removal, more pronounced inversion layers trapping pollutants, and increases in household combustion and wild fires during winter. Back trajectory analysis also revealed higher concentrations of inorganic ionic species corresponding to air mass movements over anthropogenic source regions.Peer reviewe

Assessment of polar organic aerosols at a regional background site in southern Africa

A recent paper reported GCxGC-TOFMS analysis used for the first time in southern Africa to tentatively characterise and semi-quantify 1000 organic compounds in aerosols at Welgegund - a regional background atmospheric monitoring station. Ambient polar organic aerosols characterised are further explored in terms of temporal variations, as well as the influence of meteorology and sources. No distinct seasonal pattern was observed for the total number of polar organic compounds tentatively characterised and their corresponding semi-quantified concentrations (sum of the normalised response factors, Sigma NRFs). However, the total number of polar organic compounds and Sigma NRFs between late spring and early autumn seemed relatively lower compared to the period from mid-autumn to mid-winter, while there was a period during late winter and early spring with significantly lower total number of polar organic compounds and Sigma NRFs. Relatively lower total number of polar organic compounds and corresponding Sigma NRFs were associated with fresher plumes from a source region relatively close to Welgegund. Meteorological parameters indicated that wet removal during late spring to early autumn also contributed to lower total numbers of polar organics and associated Sigma NRFs. Increased anticyclonic recirculation and more pronounced inversion layers contributed to higher total numbers of polar organic species and Sigma NRFs from mid-autumn to mid-winter, while the influence of regional biomass burning during this period was also evident. The period with significantly lower total number of polar organic compounds and Sigma NRFs was attributed to fresh open biomass burning plumes occurring within proximity of Welgegund, consisting mainly of volatile organic compounds and non-polar hydrocarbons. Multiple linear regression substantiated that the temporal variations in polar organic compounds were related to a combination of the factors investigated in this study.Peer reviewe

Statistical analysis of factors driving surface ozone variability over continental South Africa

Statistical relationships between surface ozone (O-3) concentration, precursor species and meteorological conditions in continental South Africa were examined from data obtained from measurement stations in north-eastern South Africa. Three multivariate statistical methods were applied in the investigation, i.e. multiple linear regression (MLR), principal component analysis (PCA) and -regression (PCR), and generalised additive model (GAM) analysis. The daily maximum 8-h moving average O-3 concentrations were considered in these statistical models (dependent variable). MLR models indicated that meteorology and precursor species concentrations are able to explain similar to 50% of the variability in daily maximum O-3 levels. MLR analysis revealed that atmospheric carbon monoxide (CO), temperature and relative humidity were the strongest factors affecting the daily O-3 variability. In summer, daily O-3 variances were mostly associated with relative humidity, while winter O-3 levels were mostly linked to temperature and CO. PCA indicated that CO, temperature and relative humidity were not strongly collinear. GAM also identified CO, temperature and relative humidity as the strongest factors affecting the daily variation of O-3. Partial residual plots found that temperature, radiation and nitrogen oxides most likely have a non-linear relationship with O-3,while the relationship with relative humidity and CO is probably linear. An inter-comparison between O-3 levels modelled with the three statistical models compared to measured O-3 concentrations showed that the GAM model offered a slight improvement over the MLR model. These findings emphasise the critical role of regional-scale O-3 precursors coupled with meteorological conditions in daily variances of O-3 levels in continental South Africa.Peer reviewe

Seasonal influences on surface ozone variability in continental South Africa and implications for air quality

Although elevated surface ozone (O-3) concentrations are observed in many areas within southern Africa, few studies have investigated the regional atmospheric chemistry and dominant atmospheric processes driving surface O-3 formation in this region. Therefore, an assessment of comprehensive continuous surfaceO(3) measurements performed at four sites in continental South Africa was conducted. The regional O-3 problem was evident, with O-3 concentrations regularly exceeding the South African air quality standard limit, while O-3 levels were higher compared to other background sites in the Southern Hemisphere. The temporal O-3 patterns observed at the four sites resembled typical trends for O-3 in continental South Africa, with O-3 concentrations peaking in late winter and early spring. Increased O-3 concentrations in winter were indicative of increased emissions of O-3 precursors from household combustion and other low-level sources, while a spring maximum observed at all the sites was attributed to increased regional biomass burning. Source area maps of O-3 and CO indicated significantly higher O-3 and CO concentrations associated with air masses passing over a region with increased seasonal open biomass burning, which indicated CO associated with open biomass burning as a major source of O-3 in continental South Africa. A strong correlation between O-3 on CO was observed, while O-3 levels remained relatively constant or decreased with increasing NOx, which supports a VOC-limited regime. The instantaneous production rate of O-3 calculated at Welgegund indicated that similar to 40 % of O-3 production occurred in the VOC- limited regime. The relationship between O-3 and precursor species suggests that continental South Africa can be considered VOC limited, which can be attributed to high anthropogenic emissions of NOx in the interior of South Africa. The study indicated that the most effective emission control strategy to reduce 03 levels in continental South Africa should be CO and VOC reduction, mainly associated with household combustion and regional open biomass burning.Peer reviewe

Root-zone soil moisture variability across African savannas : From pulsed rainfall to land‐cover switches

The main source of soil moisture variability in savanna ecosystems is pulsed rainfall. Rainfall pulsing impacts water-stress durations, soil moisture switching between wet-to-dry and dry-to-wet states, and soil moisture spectra as well as derived measures from it such as soil moisture memory. Rainfall pulsing is also responsible for rapid changes in grassland leaf area and concomitant changes in evapotranspirational (ET) losses, which then impact soil moisture variability. With the use of a hierarchy of models and soil moisture measurements, temporal variability in root-zone soil moisture and water-stress periods are analysed at four African sites ranging from grass to miombo savannas. The normalized difference vegetation index (NDVI) and potential ET (PET)-adjusted ET model predict memory timescale and dry persistence in agreement with measurements. The model comparisons demonstrate that dry persistence and mean annual dry periods must account for seasonal and interannual changes in maximum ET represented by NDVI and to a lesser extent PET. Interestingly, the precipitation intensity and soil moisture memory were linearly related across three savannas with ET/infiltration similar to 1.0. This relation and the variability of length and timing of dry periods are also discussed.Peer reviewe

Rapid changes in biomass burning aerosols by atmospheric oxidation

Peer reviewe

The effect of rainfall amount and timing on annual transpiration in a grazed savanna grassland

The role of precipitation (P) variability with respect to evapotranspiration (ET) and its two components, transpiration (T) and evaporation (E), from savannas continues to draw significant research interest given its relevance to a number of ecohydrological applications. Our study reports on 6 years of measured ET and estimated T and E from a grazed savanna grassland at Welgegund, South Africa. Annual P varied significantly with respect to amount (508 to 672 mm yr(-1)), with dry years characterized by infrequent early-season rainfall. T was determined using annual water-use efficiency and gross primary production estimates derived from eddy-covariance measurements of latent heat flux and net ecosystem CO2 exchange rates. The computed annual T for the 4 wet years with frequent early wet-season rainfall was nearly constant, 326 +/- 19 mm yr(-1) (T/ET=0.51), but was lower and more variable between the 2 dry years (255 and 154 mm yr(-1), respectively). Annual T and T/ET were linearly related to the early wet-season storm frequency. The constancy of annual T during wet years is explained by the moderate water stress of C4 grasses as well as trees' ability to use water from deeper layers. During extreme drought, grasses respond to water availability with a dieback-regrowth pattern, reducing leaf area and transpiration and, thus, increasing the proportion of transpiration contributed by trees. The works suggest that the early-season P distribution explains the interannual variability in T, which should be considered when managing grazing and fodder production in these grasslands.Peer reviewe

Spatial, temporal and source contribution assessments of black carbon over the northern interior of South Africa

After carbon dioxide (CO2) aerosol black carbon (BC) is considered to be the second most important contributor to global warming. This paper presents equivalent black carbon (eBC) (derived from an optical absorption method) data collected from three sites in the interior of South Africa where continuous measurements were conducted, i.e. Elandsfontein, Welgegund and Marikana, as well elemental carbon (EC) (determined by evolved carbon method) data at five sites where samples were collected once a month on a filter and analysed offline, i.e. Louis Trichardt, Skukuza, Vaal Triangle, Amersfoort and Botsalano. Analyses of eBC and EC spatial mass concentration patterns across the eight sites indicate that the mass concentrations in the South African interior are in general higher than what has been reported for the developed world and that different sources are likely to influence different sites. The mean eBC or EC mass concentrations for the background sites (Welgegund, Louis Trichardt, Skukuza, Botsalano) and sites influenced by industrial activities and/or nearby settlements (Elandsfontein, Marikana, Vaal Triangle and Amersfoort) ranged between 0.7 and 1.1, and 1.3 and 1.4 ae gm 3, respectively. Similar seasonal patterns were observed at all three sites where continuous measurement data were collected (Elandsfontein, Marikana and Welgegund), with the highest eBC mass concentrations measured from June to October, indicating contributions from household combustion in the cold winter months (June-August), as well as savannah and grassland fires during the dry season (May to mid-October). Diurnal patterns of eBC at Elandsfontein, Marikana and Welgegund indicated maximum concentrations in the early mornings and late evenings, and minima during daytime. From the patterns it could be deduced that for Marikana and Welgegund, household combustion, as well as savannah and grassland fires, were the most significant sources, respectively. Possible contributing sources were explored in greater detail for Elandsfontein, with five main sources being identified as coal-fired power stations, pyrometallurgical smelters, traffic, household combustion, as well as savannah and grassland fires. Industries on the Mpumalanga Highveld are often blamed for all forms of pollution, due to the NO2 hotspot over this area that is attributed to NOx emissions from industries and vehicle emissions from the Johannesburg-Pretoria megacity. However, a comparison of source strengths indicated that household combustion as well as savannah and grassland fires were the most significant sources of eBC, par-ticularly during winter and spring months, while coal-fired power stations, pyrometallurgical smelters and traffic contribute to eBC mass concentration levels year round.Peer reviewe