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In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa.

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. This new particle formation frequency is the highest reported from boundary layer so far. Also the new particle formation and growth rates were among the highest reported in the literature for continental boundary layer locations; median 10 nm formation rate was 2.2 cm−3 s−1 and median 10–30 nm growth rate 8.9 nm h−1. The median 2 nm ion formation rate was 0.5 cm−3 s−1 and the median ion growth rates were 6.2, 8.0 and 8.1 nm h−1 for size ranges 1.5–3 nm, 3–7 nm and 7–20 nm, respectively. The growth rates had a clear seasonal dependency with minimum during winter and maxima in spring and late summer. The relative contribution of estimated sulphuric acid to the growth rate was decreasing with increasing particle size and could explain more than 20% of the observed growth rate only for the 1.5–3 nm size range. Also the air mass history analysis indicated the highest formation and growth rates to be associated with the area of highest VOC (Volatile Organic Compounds) emissions following from biological activity rather than the highest estimated sulphuric acid concentrations. The frequency of new particle formation, however, increased nearly monotonously with the estimated sulphuric acid reaching 100% at H2SO4 concentration of 6 · 107 cm−3, which suggests the formation and growth to be independent of each other.

This review is based on ca. 260 publications, 93 of which included data on the temporal and spatial variation of the concentration of small ions (−3. However, concentrations up to 5000 cm−3 have been observed. The results are in agreement with observations of ion production rates in the atmosphere. We also summarised observations on the conversion of small ions to intermediate ions, which can act as embryos for new atmospheric aerosol particles. Those observations include the formation rates (J2[ion]) of 2-nm intermediate ions, growth rates (GR[ion]) of sub-3 nm ions, and information on the chemical composition of the ions. Unfortunately, there were only a few studies which presented J2[ion] and GR[ion]. Based on the publications, the formation rates of 2-nm ions were 0–1.1 cm−3 s−1, while the total 2-nm particle formation rates varied between 0.001 and 60 cm−3 s−1. Due to small changes in J2[ion], the relative importance of ions in 2-nm particle formation was determined by the large changes in J2[tot], and, accordingly the contribution of ions increased with decreasing J2[tot]. Furthermore, small ions were observed to activate for growth earlier than neutral nanometer-sized particles and at lower saturation ratio of condensing vapours.

Tropical montane forest ecosystems are pivotal for sustaining biodiversity and essential terrestrial ecosystem services, including the provision of high-quality fresh water. Nonetheless, the impact of montane deforestation and climate change on the capacity of forests to deliver ecosystem services is yet to be fully understood. In this study, we offer observational evidence demonstrating the response of air temperature and cloud base height to deforestation in African montane forests over the last two decades. Our findings reveal that approximately 18% (7.4 ± 0.5 million hectares) of Africa's montane forests were lost between 2003 and 2022. This deforestation has led to a notable increase in maximum air temperature (1.37 ± 0.58 °C) and cloud base height (236 ± 87 metres), surpassing shifts attributed solely to climate change. Our results call for urgent attention to montane deforestation, as it poses serious threats to biodiversity, water supply, and ecosystem services in the tropics., (© 2024. The Author(s).)

Atmospheric aerosols have significant effects on the climate and on human health. New particle formation (NPF) is globally an important source of aerosols but its relevance especially towards aerosol mass loadings in highly polluted regions is still controversial. In addition, uncertainties remain regarding the processes leading to severe pollution episodes, concerning e.g. the role of atmospheric transport. In this study, we utilize air mass history analysis in combination with different fields related to the intensity of anthropogenic emissions in order to calculate air mass exposure to anthropogenic emissions (AME) prior to their arrival at Beijing, China. The AME is used as a semi-quantitative metric for describing the effect of air mass history on the potential for aerosol formation. We show that NPF events occur in clean air masses, described by low AME. However, increasing AME seems to be required for substantial growth of nucleation mode (diameter < 30 nm) particles, originating either from NPF or direct emissions, into larger mass-relevant sizes. This finding assists in establishing and understanding the connection between small nucleation mode particles, secondary aerosol formation and the development of pollution episodes. We further use the AME, in combination with basic meteorological variables, for developing a simple and easy-to-apply regression model to predict aerosol volume and mass concentrations. Since the model directly only accounts for changes in meteorological conditions, it can also be used to estimate the influence of emission changes on pollution levels. We apply the developed model to briefly investigate the effects of the COVID-19 lockdown on PM 2.5 concentrations in Beijing. While no clear influence directly attributable to the lockdown measures is found, the results are in line with other studies utilizing more widely applied approaches., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)

Atmospheric gas-to-particle conversion is a crucial or even dominant contributor to haze formation in Chinese megacities in terms of aerosol number, surface area and mass. Based on our comprehensive observations in Beijing during 15 January 2018-31 March 2019, we are able to show that 80-90% of the aerosol mass (PM 2.5 ) was formed via atmospheric reactions during the haze days and over 65% of the number concentration of haze particles resulted from new particle formation (NPF). Furthermore, the haze formation was faster when the subsequent growth of newly formed particles was enhanced. Our findings suggest that in practice almost all present-day haze episodes originate from NPF, mainly since the direct emission of primary particles in Beijing has considerably decreased during recent years. We also show that reducing the subsequent growth rate of freshly formed particles by a factor of 3-5 would delay the buildup of haze episodes by 1-3 days. Actually, this delay would decrease the length of each haze episode, so that the number of annual haze days could be approximately halved. Such improvement in air quality can be achieved with targeted reduction of gas-phase precursors for NPF, mainly dimethyl amine and ammonia, and further reductions of SO 2 emissions. Furthermore, reduction of anthropogenic organic and inorganic precursor emissions would slow down the growth rate of newly-formed particles and consequently reduce the haze formation.

Uncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of -0.07 W m -2 , and regional changes of -2 W m -2 (Africa) and -0.5 W m -2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.

Coal combustion is one of the most significant anthropogenic CO 2 and air pollution sources globally. This paper studies the atmospheric emissions of a power plant fuelled with a mixture of industrial pellets (10.5%) and coal (89.5%). Based on the stack measurements, the solid particle number emission, which was dominated by sub-200 nm particles, was 3.4×10 11 MJ -1 for the fuel mixture when electrostatic precipitator (ESP) was cleaning the flue gas. The emission factor was 50 mg MJ -1 for particulate mass and 11 740 ng MJ -1 for the black carbon with the ESP. In the normal operation situation of the power plant, i.e., including the flue-gas desulphurisation and fabric filters (FGD and FF), the particle number emission factor was 1.7×10 8 MJ -1 , particulate mass emission factor 2 mg MJ -1 and black carbon emission factor 14 ng MJ -1 . Transmission electron microscopy (TEM) analysis supported the particle number size distribution measurement in terms of particle size and the black carbon concentration. The TEM images of the particles showed variability of the particle sizes, morphologies and chemical compositions. The atmospheric measurements, conducted in the flue-gas plume, showed that the flue-gas dilutes closed to background concentrations in 200 sec. However, an increase in particle number concentration was observed when the flue gas aged. This increase in particle number concentration was interpret as formation of new particles in the atmosphere. In general, the study highlights the importance of detailed particle measurements when utilizing new fuels in existing power plants. Implications: CO 2 emissions of energy production decrease when substituting coal with biofuels. The effects of fuels changes on particle emission characteristics have not been studied comprehensively. In this study conducted for a real-scale power plant, co-combustion of wood pellets and coal caused elevated black carbon emissions. However, it was beneficial from the total particle number and particulate mass emission point of view. Flue-gas cleaning can significantly decrease the pollutant concentrations but also changes the characteristics of emitted particles. Atmospheric measurements implicated that the new particle formation in the atmospheric flue-gas plume should be taken into account when evaluating all effects of fuel changes." Are implication statements part of the manuscript?

Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and Earth's radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia-a process experimentally investigated by the CERN CLOUD experiment-as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 10 7 molecules cm -3 , are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.

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 surface O 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 NO x , which supports a VOC-limited regime. The instantaneous production rate of O 3 calculated at Welgegund indicated that ~ 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 NO x in the interior of South Africa. The study indicated that the most effective emission control strategy to reduce O 3 levels in continental South Africa should be CO and VOC reduction, mainly associated with household combustion and regional open biomass burning., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.