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There are growing concerns on contribution of vegetation dynamics to atmospheric turbidity and quality of regional water towers. The study sought to determine the trends in the MODIS/TERRA-derived normalized difference vegetation index (NDVI) and aerosol optical depth (AOD) for Lesotho Highland over 2000–2020. The predictive relationship between the two variables was also examined using regression analysis. Irrespective of yearly AOD patterns, the AOD showed biphasic patterns peaking between mid-winter to early spring (July–October) (highest) and autumn (Feb–April) (next highest), and lowest in the summer (Nov–January). The monthly NDVI was largest in January–March (summer–early fall) with smaller values in winter and spring. This seasonality can be related to the peak of anthropogenic biomass combustion during the winter and strong winds during the spring and early summer. The AOD relationship with NDVI showed quadratic patterns peaking and plunging with changes in season. About 30–80% (R2 = 0.3–0.8%) changes in annual AOD from 2000 to 2020 were explainable by the dynamics of NDVI indicating that increased NDVI contributes to about a 50% decrease in AOD in the Lesotho Highlands. However, an outlier trend was observed in 2007 (R2 = 13%). Incidences of high AOD in months of high NDVI may be indicative of traveling aerosols, i.e., aerosols from non-local sources/activity. On the other hand, high AOD in months of low NDVI implicates local aerosol sources. Trend relationship studies on vegetation loss and AOD in mountain areas of other regions could improve knowledge of contaminant dynamics and risk implications for downstream populations. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Naturally and anthropogenically emitted aerosols, which are determined by their physical and chemical properties, have an impact on both air quality and the radiative properties of the earth. An important source of atmospheric particulate matter (PM) in South Africa is household combustion for space heating and cooking, which predominantly occurs in low-income urban settlements. The aim of this study was to conduct a detailed size-resolved assessment of chemical characteristics of aerosols associated with household combustion through the collection of particulates in low-income urban settlements in South Africa to quantify the extent of the impacts of atmospheric pollution. Outdoor (ambient) and indoor aerosols in different size fractions were collected during summer and winter in four low-income urban settlements located in the north-eastern interior on the South African Highveld, i.e. Kwadela, Kwazamokuhle, Zamdela, and Jouberton. Mass concentration and chemical composition was determined for three size fractions, namely, PM 1 , PM 2.5 , and PM 2.5-10. The highest concentrations of particulates were measured indoors with the highest mass concentration determined in the indoor PM 2.5-10 (coarse) size fraction. However, the highest mass concentrations were determined in PM 1 in all outdoor aerosol samples collected during winter and summer, and in indoor samples collected during summer. Significantly higher concentrations were determined for SO 4-2 in outdoor and indoor particulates compared to other ionic species, with NH 4+ and NO 3- being the second most abundant. SO 4-2 and NH 4+ almost exclusively occurred in the PM 1 size fraction, while NO 3- was the major constituent in the larger size fractions. The highest SO 4-2 levels were recorded for the winter and summer outdoor campaigns conducted at Zamdela, while NO 3- and NH 4+ concentrations were higher during the winter outdoor campaign. The combined concentrations of trace elements were higher for indoor particulates compared to outdoor aerosols, while the total trace element concentrations in PM 1 were substantially higher than levels thereof in the two larger size fractions of particulates collected during all sampling campaigns. No distinct seasonal trend was observed for the concentrations of trace elements. Na, Ca, and Cr had the highest concentrations in particulates collected during outdoor and indoor sampling campaigns. Ni concentrations in outdoor and indoor aerosols exceeded the annual average European standard. PM 1 collected during all sampling campaigns in low-income urban settlements had the highest organic carbon (OC) and elemental carbon (EC) concentrations. The highest OC and EC levels were determined in PM 1 collected during the winter indoor campaign. OC and EC concentrations were highest during winter, which can be attributed to changes in meteorological patterns and increased household combustion during winter. Low OC/EC ratios determined for particulates collected in low-income urban settlements are indicative of OC and EC being mainly associated with local sources of these species. OC concentrations determined in this study were an order of magnitude lower than OC concentrations determined for ambient aerosols collected in the north-eastern interior of South Africa, while similar EC levels were measured. According to estimated dust concentrations, it was indicated that dust is the major constituent in all size ranges of particulates collected in this study, while trace elements were the second most abundant. However, trace elements made the highest contribution to indoor PM 1 and PM 1-2.5 mass. Mass concentrations and chemical concentrations determined for aerosols collected in low-income settlements reflect the regional impacts of anthropogenic sources in the north-eastern interior of South Africa and the influence of local sources. [ABSTRACT FROM AUTHOR]

Statistical relationships between surface ozone (O3) 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 O3 concentrations were considered in these statistical models (dependent variable). MLR models indicated that meteorology and precursor species concentrations are able to explain ~50% of the variability in daily maximum O3 levels. MLR analysis revealed that atmospheric carbon monoxide (CO), temperature and relative humidity were the strongest factors affecting the daily O3 variability. In summer, daily O3 variances were mostly associated with relative humidity, while winter O3 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 O3. Partial residual plots found that temperature, radiation and nitrogen oxides most likely have a non-linear relationship with O3,while the relationship with relative humidity and CO is probably linear. An inter-comparison between O3 levels modelled with the three statistical models compared to measured O3 concentrations showed that the GAM model offered a slight improvement over the MLR model. These findings emphasise the critical role of regional-scale O3 precursors coupled with meteorological conditions in daily variances of O3 levels in continental South Africa. [ABSTRACT FROM AUTHOR]

Air quality is affected by the interaction between emission sources and urban planning factors such as land use. Limited empirical studies have been conducted to determine the influence of land use and population growth on air quality in South Africa. Thus, the purpose of this research is to examine the relationship between land use, population growth and air pollution focusing on black carbon (BC), carbon monoxide (CO) and sulphur dioxide (SO2) pollution in South Africa. Three urban areas; Tshwane, Rustenburg and Emalahleni in South Africa were chosen for this study. We found that the increase in population growth in these areas led directly to the expansion of built-up areas. As a consequence, these led to the increase in BC, CO and SO2 concentrations thus degrading air quality in these areas. Rural-urban migration could be the main reason for the rapid increase in population growth, land expansion and the deterioration in air quality in these areas. This study has shown that there is a close link between, land use, population growth and air quality. [ABSTRACT FROM AUTHOR]

Particulate matter (PM) can affect climate, air quality, human health, acid deposition and visibility, and contain a significant fraction of organic (OC) and elemental carbon (EC). Southern Africa is an important source region for OC and EC, however, little OC and EC data have been published for this region. This paper presents a multi-year, multi-site (an urban-industrial site in the Vaal Triangle, UI-VT; an industrially influenced site at Amerfoort, iI-AF; and two regional background sites at Skukuza and Louis Trichardt, RR-SK and RR-LT) PM with an aerodynamic diameter ≤ 2.5 μm (PM2.5) OC and EC dataset for South Africa. The median OC (9.3) and EC (3.2 μg.m−3) concentrations at UI-VT were 1.3 to 2.5 and 2.7 to 4.4 times higher, if compared to the other sites. OC/EC ratios indicated that sources in close proximity to UI-VT were likely the main contributors, while sources that are more distant contributed fractionally more at the other sites. Household combustion for space heating and regional open biomass burning contributed to elevated levels during the cold and dry months at UI-VT. Regional open biomass burning also lead to higher OC and EC concentrations during the dry season at the industrially influenced site (iI-AF) and one of the regional background sites (RR-SK). From the seasonal concentration patterns, it seemed as if household combustion for space heating also contributed at these two sites during the cold months, but this could not be proven, even if only samples with limited influence of open biomass burning were considered. Such biomass burning influences were semi-quantified by considering MODIS fire pixels occurring within the air mass fetch region for each sample. For the remaining regional background site (RR-LT) the results suggesed that only regional open biomass burning contributed to elevated levels of OC and EC in the dry season and that household combustion for space heating did not contribute significantly. [ABSTRACT FROM AUTHOR]

The atmospheric boundary layer (BL) is the atmospheric layer coupled to the Earth's surface at relatively short timescales. A key quantity is the BL depth, which is important in many applied areas of weather and climate such as air-quality forecasting. Studying BLs in climates and biomes across the globe is important, particularly in the under-sampled southern hemisphere. The present study is based on a grazed grassland-savannah area in northwestern South Africa during October 2012–August 2014. Ceilometers are probably the cheapest method for measuring continuous aerosol profiles up to several kilometers above ground and are thus an ideal tool for long-term studies of BLs. A ceilometer-estimated BL depth is based on profiles of attenuated backscattering coefficients from atmospheric aerosols; the sharpest drop often occurs at BL top. Based on this, we developed a new method for layer detection that we call the signal-limited layer method. The new algorithm was applied to ceilometer profiles which thus classified BL into classic regime types: daytime convective mixing, and a double layer at night of surface-based stable with a residual layer above it. We employed wavelet fitting to increase successful BL estimation for noisy profiles. The layer-detection algorithm was supported by an eddy-flux station, rain gauges, and manual inspection. Diurnal cycles were often clear, with BL depth detected for 50% of the daytime typically being 1–3 km, and for 80% of the night-time typically being a few hundred meters. Variability was also analyzed with respect to seasons and years. Finally, BL depths were compared with ERA-Interim estimates of BL depth to show reassuring agreement. [ABSTRACT FROM AUTHOR]

Recent studies have shown very high frequencies of atmospheric new particle formation in different environments in South Africa. Our aim here was to investigate the causes for two or three consecutive daytime nucleation events, followed by subsequent particle growth during the same day. We analysed 108 and 31 such days observed in a polluted industrial and moderately polluted rural environments, respectively, in South Africa. The analysis was based on two years of measurements at each site. After rejecting the days having notable changes in the air mass origin or local wind direction, i.e. two major reasons for observed multiple nucleation events, we were able to investigate other factors causing this phenomenon. Clouds were present during, or in between most of the analysed multiple particle formation events. Therefore, some of these events may have been single events, interrupted somehow by the presence of clouds. From further analysis, we propose that the first nucleation and growth event of the day was often associated with the mixing of a residual air layer rich in SO2 (oxidized to sulphuric acid) into the shallow surface-coupled layer. The second nucleation and growth event of the day usually started before midday and was sometimes associated with renewed SO2 emissions from industrial origin. However, it was also evident that vapours other than sulphuric acid were required for the particle growth during both events. This was especially the case when two simultaneously growing particle modes were observed. Based on our analysis, we conclude that the relative contributions of estimated H2SO4 and other vapours on the first and second nucleation and growth events of the day varied from day to day, depending on anthropogenic and natural emissions, as well as atmospheric conditions. [ABSTRACT FROM AUTHOR]

The South African savannah region is a complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that the knowledge of controlling aerosol processes in this environment is limited. Here we use a recent dataset of 18 months of aerosol size distribution observations trying to understand the annual cycle of cloud condensation nuclei (CCN). Our observations show that the concentration of CCN-sized particles remains, in line with previous studies, high throughout the year with the highest concentrations during the dry winter and the lowest during the wet summer. During the wet season with reduced anthropogenic and biomass burning primary emissions, this pool of CCN is partly filled by boundary layer nucleation with subsequent growth. The enhanced importance of formation and growth during the wet season is addressed to increased biogenic activity together with enhanced free tropospheric removal decreasing the concentration of pre-existing CCN. During the dry season, while frequent new particle formation takes place, particle growth is reduced due to reduced condensing vapour concentrations. Thus in the dry season particles are not able to grow to sizes where they may act as CCN nearly as efficiently as during the wet season. The observations are compared to simulations by a global aerosol model GLOMAP. To our surprise, the global aerosol model utilized to explain the observations was not capable of re-producing the characteristics of particle formation and the annual CCN cycle, despite earlier good performance in predicting the particle concentrations in a number of diverse environments, including the South African savannah region. While the average yearly CCN concentrations of modelled CCN is close to observed concentrations, the characteristics of nucleation bursts and subsequent growth are not captured satisfactory by the model. Our sensitivity tests using different nucleation parameterizations and condensing organic vapour production rates show that neither of these is likely to explain the differences between observed and modelled nucleation and growth rates. A sensitivity study varying 28 modelling parameters indicates that the main uncertainties in the result are due to uncertainties in biomass burning emissions during the dry season, and anthropogenic sulphur emissions during the wet season, both in terms or emitted mass and particle sizes. The uncertainties appear to be mostly related to uncertainties in primary particle emissions, including the emissions variability not captured by monthly emission inventories. The results of this paper also highlights the fact that deficiencies in emissions estimates may result in deficiencies in particle production fluxes, while the end product such as modelled CCN concentration may be in line with observations. [ABSTRACT FROM AUTHOR]

This study presents a total of four years of submicron aerosol particle size distribution measurements in the southern African savannah, an environment with few previous observations covering a full seasonal cycle and the size range below 100 nm. During the first 19 months, July 2006-January 2008, the measurements were carried out at Botsalano, a semi-clean location, whereas during the latter part, February 2008-May 2010, the measurements were carried out at Marikana (approximately 150 km east of Botsalano), which is a more polluted location with both pyrometallurgical industries and informal settlements nearby. The median total concentration of aerosol particles was more than four times as high at Marikana than at Botsalano. In the size ranges of 12-840 nm, 50-840 nm and 100-840 nm the median concentrations were 1856, 1278 and 698 particles cm-3 at Botsalano and 7805, 3843 and 1634 particles cm-3 at Marikana, respectively. The diurnal variation of the size distribution for Botsalano arose as a result of frequent regional new particle formation. However, for Marikana the diurnal variation was dominated by the morning and evening household burning in the informal settlements, although regional new particle formation was even more frequent than at Botsalano. The effect of the industrial emissions was not discernible in the size distribution at Marikana although it was clear in the sulphur dioxide diurnal pattern, indicating the emissions to be mostly gaseous. Seasonal variation was strongest in the concentration of particles larger than 100 nm, which was clearly elevated at both locations during the dry season from May to September. In the absence of wet removal during the dry season, the concentration of particles larger than 100 nm had a correlation above 0.7 with CO for both locations, which implies incomplete burning to be an important source of aerosol particles during the dry season. However, the sources of burning differ: at Botsalano the rise in concentration originates from regional wild fires, while at Marikana domestic heating in the informal settlements is the main source. Air mass history analysis for Botsalano identified four regional scale source areas in southern Africa and enabled the differentiation between fresh and aged rural background aerosol originating from the clean sector, i.e., western sector with very few large anthropogenic sources. Comparison to size distributions published for other comparable environments in Northern Hemisphere shows southern African savannah to have a unique combination of sources and meteorological parameters. The observed strong link between combustion and seasonal variation is comparable only to the Amazon basin; however, the lack of long-term observations in the Amazonas does not allow a quantitative comparison. All the data presented in the figures, as well as the time series of monthly mean and median size distributions are included in numeric form as a Supplement to provide a reference point for the aerosol modelling community. [ABSTRACT FROM AUTHOR]

South Africa holds significant mineral resources, with a substantial fraction of these reserves occurring and being processed in a large geological structure termed the Bushveld Igneous Complex (BIC). The area is also highly populated by informal, semi-formal and formal residential developments. However, knowledge of air quality and research related to the atmosphere is still very limited in the area. In order to investigate the characteristics and processes affecting sub-micron particle number concentrations and formation events, air ion and aerosol particle size distributions and number concentrations, together with meteorological parameters, trace gases and particulate matter (PM) were measured for over two years at Marikana in the heart of the western BIC. The observations showed that trace gas (i.e. SO2, NOx, CO) and black carbon concentrations were relatively high, but in general within the limits of local air quality standards. The area was characterised by very high condensation sink due to background aerosol particles, PM10 and O3 concentration. The results indicated that high amounts of Aitken and accumulation mode particles originated from domestic burning for heating and cooking in the morning and evening, while during daytime SO2-based nucleation followed by the growth by condensation of vapours from industrial, residential and natural sources was the most probable source for large number concentrations of nucleation and Aitken mode particles. Nucleation event day frequency was extremely high, i.e. 86% of the analysed days, which to the knowledge of the authors is the highest frequency ever reported. The air mass back trajectory and wind direction analyses showed that the secondary particle formation was influenced both by local and regional pollution and vapour sources. Therefore, our observation of the annual cycle and magnitude of the particle formation and growth rates during nucleation events were similar to results previously published for a semi-clean savannah site in South Africa. [ABSTRACT FROM AUTHOR]

While the stratospheric ozone protects the biosphere against ultraviolet (UV) radiation, tropospheric ozone acts like a greenhouse gas and an indicator of anthropogenic pollution. In this paper, we combined ground-based and satellite ozone observations over Irene site (25.90° S, 28.22° E), one of the most ancient ozone-observing stations in the southern tropics. The dataset is made of daily total columns and weekly profiles of ozone collected over 20 years, from 1998 to 2017. In order to fill in some missing data and split the total column of ozone into a tropospheric and a stratospheric column, we used satellite observations from TOMS (Total Ozone Mapping Spectrometer), OMI (Ozone Monitoring Instrument), and MLS (Microwave Limb Sounder) experiments. The tropospheric column is derived by integrating ozone profiles from an ozonesonde experiment, while the stratospheric column is obtained by subtracting the tropospheric column from the total column (recorded by the Dobson spectrometer), and by assuming that the mesospheric contribution is negligible. Each of the obtained ozone time series was then analyzed by applying the method of wavelet transform, which permitted the determination of the main forcings that contribute to each ozone time series. We then applied the multivariate Trend-Run model and the Mann–Kendall test for trend analysis. Despite the different analytical approaches, the obtained results are broadly similar and consistent. They showed a decrease in the stratospheric column (−0.56% and −1.7% per decade, respectively, for Trend-Run and Mann–Kendall) and an increase in the tropospheric column (+2.37% and +3.6%, per decade, respectively, for Trend-Run and Mann–Kendall). Moreover, the results presented here indicated that the slowing down of the total ozone decline is somewhat due to the contribution of the tropospheric ozone concentration. [ABSTRACT FROM AUTHOR]

Although atmospheric organic N compounds are considered to be important, especially in new particle formation and their contribution to brown carbon, these species are not that well understood. This can be partially attributed to their chemical complexity. Therefore, the aim of this study was to assess the characteristics of organic N compounds utilising comprehensive two-dimensional gas chromatography coupled with a time-of-flight mass spectrometer (GCxGC-TOFMS) in aerosol samples that were collected at a savanna-grassland background region and to determine the possible sources. 135 atmospheric organic N compounds were tentatively characterised and semi-quantified, which included amines, nitriles, amides, urea, pyridine derivatives, amino acids, nitro-and nitroso compounds, imines, cyanates and isocyanates, and azo compounds. Amines contributed to 51% of the semi-quantified concentrations, while nitriles, pyridine derivatives, and amides comprised 20%, 11%, and 8%, respectively, of the semi-quantified concentrations. Amines, nitriles, amides, and pyridine derivatives concentrations were higher during the dry season, which were attributed to meteorology and open biomass burning. Anthropogenic sources impacting air masses measured at Welgegund, as well as regional agricultural activities, were considered as the major sources of amines, while the regional influence of household combustion was most likely the main source of nitriles, amides, and pyridine derivatives. The other organic N species were most likely related to the influence of local and regional agricultural activities. [ABSTRACT FROM AUTHOR]