Author Correction: Global and regional trends of atmospheric sulfur.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Global and regional trends of atmospheric sulfur.

The profound changes in global SO2 emissions over the last decades have affected atmospheric composition on a regional and global scale with large impact on air quality, atmospheric deposition and the radiative forcing of sulfate aerosols. Reproduction of historical atmospheric pollution levels based on global aerosol models and emission changes is crucial to prove that such models are able to predict future scenarios. Here, we analyze consistency of trends in observations of sulfur components in air and precipitation from major regional networks and estimates from six different global aerosol models from 1990 until 2015. There are large interregional differences in the sulfur trends consistently captured by the models and observations, especially for North America and Europe. Europe had the largest reductions in sulfur emissions in the first part of the period while the highest reduction came later in North America and East Asia. The uncertainties in both the emissions and the representativity of the observations are larger in Asia. However, emissions from East Asia clearly increased from 2000 to 2005 followed by a decrease, while in India a steady increase over the whole period has been observed and modelled. The agreement between a bottom-up approach, which uses emissions and process-based chemical transport models, with independent observations gives an improved confidence in the understanding of the atmospheric sulfur budget.

Tethered balloon-born and ground-based measurements of black carbon and particulate profiles within the lower troposphere during the foggy period in Delhi, India.

The ground and vertical profiles of particulate matter (PM) were mapped as part of a pilot study using a Tethered balloon within the lower troposphere (1000m) during the foggy episodes in the winter season of 2015-16 in New Delhi, India. Measurements of black carbon (BC) aerosol and PM <2.5 and 10µm (PM2.5 & PM10 respectively) concentrations and their associated particulate optical properties along with meteorological parameters were made. The mean concentrations of PM2.5, PM10, BC370nm, and BC880nm were observed to be 146.8±42.1, 245.4±65.4, 30.3±12.2, and 24.1±10.3µgm-3, respectively. The mean value of PM2.5 was ~12 times higher than the annual US-EPA air quality standard. The fraction of BC in PM2.5 that contributed to absorption in the shorter visible wavelengths (BC370nm) was ~21%. Compared to clear days, the ground level mass concentrations of PM2.5 and BC370nm particles were substantially increased (59% and 24%, respectively) during the foggy episode. The aerosol light extinction coefficient (σext) value was much higher (mean: 610Mm-1) during the lower visibility (foggy) condition. Higher concentrations of PM2.5 (89µgm-3) and longer visible wavelength absorbing BC880nm (25.7µgm-3) particles were observed up to 200m. The BC880nm and PM2.5 aerosol concentrations near boundary layer (1km) were significantly higher (~1.9 and 12µgm-3), respectively. The BC (i.e BCtot) aerosol direct radiative forcing (DRF) values were estimated at the top of the atmosphere (TOA), surface (SFC), and atmosphere (ATM) and its resultant forcing were - 75.5Wm-2 at SFC indicating the cooling effect at the surface. A positive value (20.9Wm-2) of BC aerosol DRF at TOA indicated the warming effect at the top of the atmosphere over the study region. The net DRF value due to BC aerosol was positive (96.4Wm-2) indicating a net warming effect in the atmosphere. The contribution of fossil and biomass fuels to the observed BC aerosol DRF values was ~78% and ~22%, respectively. The higher mean atmospheric heating rate (2.71Kday-1) by BC aerosol in the winter season would probably strengthen the temperature inversion leading to poor dispersion and affecting the formation of clouds. Serious detrimental impacts on regional climate due to the high concentrations of BC and PM (especially PM2.5) aerosol are likely based on this study and suggest the need for immediate, stringent measures to improve the regional air quality in the northern India.

Sources and elemental composition of summer aerosols in the Larsemann Hills (Antarctica).

Atmospheric aerosols play a major role in the global climate change. A better physical characterization of the chemical composition of atmospheric aerosols, especially in remote atmosphere, is an important step to reduce the current uncertainty in their effect on the radiative forcing of the climate. In the present work, surface aerosols have been studied over the Southern Ocean and over Bharati, Indian Research Station at Larsemann Hills at the Antarctic coast during the summer season of 2009-2010. Aerosol samples were collected using optical particle counter (OPC) and high-volume air sampler. PM10 and PM2.5 aerosol samples were analyzed for various water-soluble and acid-soluble ionic constituents. The Hysplit model was used to compute the history of the air masses for their possible origin. Supplementary measurements of meteorological parameters were also used. The average mass concentration for PM10 over the Southern Ocean was found to be 13.4 µg m(3). Over coastal Antarctica, the mass of PM10 was 5.13 µg m(-3), whereas that of PM2.5 was 4.3 µg m(-3). Contribution of marine components, i.e., Na, Cl and Mg was dominant over the Southern Ocean (79 %) than over the coastal Antarctica where they were dominant in coarse mode (67 %) than in fine mode (53 %) aerosols. The NH4/nss-SO4 ratio of 1.12 in PM2.5 indicates that the NH4 and SO4 ions were in the form of NH4HSO4. Computation of enrichment factors indicate that elements of anthropogenic origin, e.g., Zn, Cu, Pb, etc., were highly enriched with respect to crustal composition.

Vertical profiles of black carbon aerosols over the urban locations in South India.

Vertical profiles of black carbon (BC) aerosol were determined from aircraft measurements under the Cloud Aerosol Interaction and Precipitation Enhancement Experiment (CAIPEEX) program conducted by the Indian Institute of Tropical Meteorology, India during 2009 over Bangalore and Hyderabad in south India. BC mass loadings decreased approximately monotonically from 10(3) to 10(4) ng/m(3) at the surface to ~10(2) ng/m(3) at an altitude of about 7 km; although layers at intermediate levels containing anomalously high BC loadings were frequently encountered that were attributed mainly to the convective transport from surface sources accompanied by changes in the local boundary layer and atmospheric stability. In addition, as evidenced from air mass back trajectories; long range transport from distant sources contributed to some anomalous spikes in BC concentration. The presence of BC in cloud forming regions of the free troposphere could have important implications for cloud microphysics and subsequent rainfall mechanism over this region. Apart from this, the effects on human health are equally important.

Seasonal factors influencing in chemical composition of total suspended particles at Pune, India.

A study on the chemical characterization of boundary layer aerosols is made based on the collection of TSP and size separated aerosol mass samples at Pune during March 2007-February 2008. This study will be helpful in simulating atmospheric processes responsible for aerosol development over Pune region and understanding its environmental implications related to radiation budget and climate. It is found that major fraction of Ca(2+) is locally generated by suspension of soil dust during all the seasons. During pre-monsoon season, coarse Mg(2+) is originated from the soil and the sea salt, whereas fine Mg(2+) is generated from the local biomass burning. Sizeable amount of SO(4)(2-) is emitted from local industrial and brick kiln's activities. Neutralization of NO(3)(-), generated both from biogenic and anthropogenic sources, is made by NH(3) gas generated mainly from anthropogenic sources. The data are further examined in terms of the factors specific to the individual seasons influencing physical and chemical characteristics of the boundary layer aerosols. The specific factors are: (a) Intense local convection during pre-monsoon season; (b) southwesterly wind flow and rainfall activity during monsoon season; and (c) Day time convection and occurrence of low level inversion during post-monsoon and winter seasons.

Brown clouds over South Asia: biomass or fossil fuel combustion?

Carbonaceous aerosols cause strong atmospheric heating and large surface cooling that is as important to South Asian climate forcing as greenhouse gases, yet the aerosol sources are poorly understood. Emission inventory models suggest that biofuel burning accounts for 50 to 90% of emissions, whereas the elemental composition of ambient aerosols points to fossil fuel combustion. We used radiocarbon measurements of winter monsoon aerosols from western India and the Indian Ocean to determine that biomass combustion produced two-thirds of the bulk carbonaceous aerosols, as well as one-half and two-thirds of two black carbon subfractions, respectively. These constraints show that both biomass combustion (such as residential cooking and agricultural burning) and fossil fuel combustion should be targeted to mitigate climate effects and improve air quality.