ALBERT

Description: The Kathmandu Valley in South Asia is considered as one of the global "hot spots" in terms of urban air pollution. It is facing severe air quality problems as a result of rapid urbanization and land use change, socioeconomic transformation and high population growth. In this paper, we present the first full year (February 2013–January 2014) analysis of simultaneous measurements of two short-lived climate forcers/pollutants (SLCF/P), i.e. ozone (O3) and equivalent black carbon (hereinafter noted as BC) and aerosol number concentration at Paknajol, in the center of the Kathmandu metropolitan city. The diurnal behavior of equivalent black carbon (BC) and aerosol number concentration indicated that local pollution sources represent the major contributions to air pollution in this city. In addition to photochemistry, the planetary boundary layer (PBL) and wind play important roles in determining O3 variability, as suggested by the analysis of seasonal diurnal cycle and correlation with meteorological parameters and aerosol properties. Especially during pre-monsoon, high values of O3 were found during the afternoon/evening; this could be related to mixing and entrainment processes between upper residual layers and the PBL. The high O3 concentrations, in particular during pre-monsoon, appeared well related to the impact of major open vegetation fires occurring at regional scale. On a synoptic-scale perspective, westerly and regional atmospheric circulations appeared to be especially conducive for the occurrence of the high BC and O3 values. The very high values of SLCF/P, detected during the whole measurement period, indicated persisting adverse air quality conditions, dangerous for the health of over 3 million residents of the Kathmandu Valley, and the environment. Consequently, all of this information may be useful for implementing control measures to mitigate the occurrence of acute pollution levels in the Kathmandu Valley and surrounding area.

Description: The Kathmandu Valley in Nepal suffers from severe wintertime air pollution. Volatile organic compounds (VOCs) are key constituents of air pollution, though their specific role in the Valley is poorly understood due to insufficient data. During the SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley-Atmospheric Brown Clouds) field campaign conducted in Nepal in the winter of 2012–2013, a comprehensive study was carried out to characterize the chemical composition of ambient Kathmandu air, including the determination of speciated VOCs by deploying a Proton Transfer Reaction Time of Flight Mass Spectrometer (PTR-TOF-MS)–the first such deployment in South Asia. 71 ion peaks (for which measured ambient concentrations exceeded the 2 σ detection limit) were detected in the PTR-TOF-MS mass scan data, highlighting the chemical complexity of ambient air in the Valley. Of the 71 species, 37 were found to have campaign average concentrations greater than 200 ppt and were identified based on their spectral characteristics, ambient diel profiles and correlation with specific emission tracers as a result of the high mass resolution (m/Δm 〉 4200) and temporal resolution (1 min) of the PTR-TOF-MS. The highest average VOC mixing ratios during the measurement period were (in rank order): acetaldehyde (8.8 ppb), methanol (7.4 ppb), acetone (4.2 ppb), benzene (2.7 ppb), toluene (1.5 ppb), isoprene (1.1 ppb), acetonitrile (1.1 ppb), C8-aromatics (~ 1 ppb), furan (~ 0.5 ppb), and C9-aromatics (0.4 ppb). Distinct diel profiles were observed for the nominal isobaric compounds isoprene (m/z = 69.070) and furan (m/z = 69.033). Comparison with wintertime measurements from several locations elsewhere in the world showed mixing ratios of acetaldehyde (~ 9 ppb), acetonitrile (~ 1 ppb) and isoprene (~ 1 ppb) to be among the highest reported till date. Two "new" ambient compounds namely, formamide (m/z = 46.029) and acetamide (m/z = 60.051), which can photochemically produce isocyanic acid in the atmosphere, are reported in this study along with nitromethane (a tracer for diesel exhaust) which has only recently been detected in ambient studies. Two distinct periods were selected during the campaign for detailed analysis: the first was associated with high wintertime emissions of biogenic isoprene, and the second with elevated levels of ambient acetonitrile, benzene and isocyanic acid from biomass burning activities. Emissions from biomass burning and biomass co-fired brick kilns were found to be the dominant sources for compounds such as propyne, propene, benzene and propanenitrile which correlated strongly with acetonitrile (r2 〉 0.7), a chemical tracer for biomass burning. The calculated total VOC OH reactivity was dominated by acetaldehyde (24.0 %), isoprene (20.2 %) and propene (18.7 %), while oxygenated VOCs and isoprene collectively contributed to more than 68 % of the total ozone production potential. Based on known SOA yields and measured ambient concentrations in the Kathmandu Valley, the relative SOA production potential of VOCs were: benzene 〉 naphthalene 〉 toluene 〉 xylenes 〉 monoterpenes 〉 trimethyl-benzenes 〉 styrene 〉 isoprene. The first ambient measurements from any site in South Asia of compounds with significant health effects such as isocyanic acid, formamide, acetamide, naphthalene and nitromethane have been reported in this study. Our results suggest that mitigation of intense wintertime biomass burning activities, in particular point sources such biomass co-fired brick kilns, would be important to reduce the emission and formation of toxic VOCs (such as benzene and isocyanic acid) in the Kathmandu Valley and improve its air quality.

Description: Combustion of fuels in the residential sector for cooking and heating, results in the emission of aerosol and aerosol precursors impacting air quality, human health and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the uncertainties in the impact of residential fuel combustion on atmospheric aerosol. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia and Eastern Europe. We use a concentration response function to estimate the health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (〉 30 years of age) premature mortality of 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect of between −66 and +21 mW m-2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m-2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

Description: Aerosol black carbon is a unique primary tracer for combustion emissions. It affects the optical properties of the atmosphere and is recognized as the second most important anthropogenic forcing agent for climate change. It is the primary tracer for adverse health effects caused by air pollution. For the accurate determination of mass equivalent black carbon concentrations in the air and for source apportionment of the concentrations, optical measurements by filter-based absorption photometers must take into account the "filter loading effect". We present a new real-time loading effect compensation algorithm based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer model AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier Aethalometer models and other filter-based absorption photometers. The real-time loading effect compensation algorithm provides the high-quality data necessary for real-time source apportionment and for determination of the temporal variation of the compensation parameter k.

Description: The Kathmandu Valley in south Asia is considered as one of the global "hot spots" in terms of urban air pollution. It is facing severe air quality problems as a result of rapid urbanization and land use change, socioeconomic transformation, and high population growth. In this paper, we present the first full year (February 2013–January 2014) analysis of simultaneous measurements of two short-lived climate forcers/pollutants (SLCF/P), i.e., ozone (O3) and equivalent black carbon (hereinafter noted as BC) and aerosol number concentration at Paknajol, in the city center of Kathmandu. The diurnal behavior of equivalent BC and aerosol number concentration indicated that local pollution sources represent the major contributions to air pollution in this city. In addition to photochemistry, the planetary boundary layer (PBL) and wind play important roles in determining O3 variability, as suggested by the analysis of seasonal changes of the diurnal cycles and the correlation with meteorological parameters and aerosol properties. Especially during pre-monsoon, high values of O3 were found during the afternoon/evening. This could be related to mixing and entrainment processes between upper residual layers and the PBL. The high O3 concentrations, in particular during pre-monsoon, appeared well related to the impact of major open vegetation fires occurring at the regional scale. On a synoptic-scale perspective, westerly and regional atmospheric circulations appeared to be especially conducive for the occurrence of the high BC and O3 values. The very high values of SLCF/P, detected during the whole measurement period, indicated persisting adverse air quality conditions, dangerous for the health of over 3 million residents of the Kathmandu Valley, and the environment. Consequently, all of this information may be useful for implementing control measures to mitigate the occurrence of acute pollution levels in the Kathmandu Valley and surrounding area.

Description: Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (〉  30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

Description: The Himalayas and the Tibetan Plateau region (HTP), despite being a remote and sparsely populated area, is regularly exposed to polluted air masses with significant amounts of aerosols including black carbon. These dark, light-absorbing particles are known to exert a great melting potential on mountain cryospheric reservoirs through albedo reduction and radiative forcing. This study combines ground-based and satellite remote sensing data to identify a severe aerosol pollution episode observed simultaneously in central Tibet and on the southern side of the Himalayas during 13–19 March 2009 (pre-monsoon). Trajectory calculations based on the high-resolution numerical weather prediction model COSMO are used to locate the source regions and study the mechanisms of pollution transport in the complex topography of the HTP. We detail how polluted air masses from an atmospheric brown cloud (ABC) over South Asia reach the Tibetan Plateau within a few days. Lifting and advection of polluted air masses over the great mountain range is enabled by a combination of synoptic-scale and local meteorological processes. During the days prior to the event, winds over the Indo-Gangetic Plain (IGP) are generally weak at lower levels, allowing for accumulation of pollutants and thus the formation of ABCs. The subsequent passing of synoptic-scale troughs leads to southwesterly flow in the middle troposphere over northern and central India, carrying the polluted air masses across the Himalayas. As the IGP is known to be a hotspot of ABCs, the cross-Himalayan transport of polluted air masses may have serious implications for the cryosphere in the HTP and impact climate on regional to global scales. Since the current study focuses on one particularly strong pollution episode, quantifying the frequency and magnitude of similar events in a climatological study is required to assess the total impact.

Description: Lumbini, in southern Nepal, is a UNESCO world heritage site of universal value as the birthplace of Buddha. Poor air quality in Lumbini and surrounding regions is a great concern for public health as well as for preservation, protection and promotion of Buddhist heritage and culture. We present here results from measurements of ambient concentrations of key air pollutants (PM, BC, CO, O3) in Lumbini, first of its kind for Lumbini, conducted during an intensive measurement period of 3 months (April–June 2013) in the pre-monsoon season. The measurements were carried out as a part of the international air pollution measurement campaign; SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley – Atmospheric Brown Clouds). The main objective of this work is to understand and document the level of air pollution, diurnal characteristics and influence of open burning on air quality in Lumbini. The hourly average concentrations during the entire measurement campaign ranged as follows: BC was 0.3–30.0 µg m−3, PM1 was 3.6–197.6 µg m−3, PM2. 5 was 6.1–272.2 µg m−3, PM10 was 10.5–604.0 µg m−3, O3 was 1.0–118.1 ppbv and CO was 125.0–1430.0 ppbv. These levels are comparable to other very heavily polluted sites in South Asia. Higher fraction of coarse-mode PM was found as compared to other nearby sites in the Indo-Gangetic Plain region. The ΔBC ∕ ΔCO ratio obtained in Lumbini indicated considerable contributions of emissions from both residential and transportation sectors. The 24 h average PM2. 5 and PM10 concentrations exceeded the WHO guideline very frequently (94 and 85 % of the sampled period, respectively), which implies significant health risks for the residents and visitors in the region. These air pollutants exhibited clear diurnal cycles with high values in the morning and evening. During the study period, the worst air pollution episodes were mainly due to agro-residue burning and regional forest fires combined with meteorological conditions conducive of pollution transport to Lumbini. Fossil fuel combustion also contributed significantly, accounting for more than half of the ambient BC concentration according to aerosol spectral light absorption coefficients obtained in Lumbini. WRF-STEM, a regional chemical transport model, was used to simulate the meteorology and the concentrations of pollutants to understand the pollutant transport pathways. The model estimated values were ∼ 1. 5 to 5 times lower than the observed concentrations for CO and PM10, respectively. Model-simulated regionally tagged CO tracers showed that the majority of CO came from the upwind region of Ganges Valley. Model performance needs significant improvement in simulating aerosols in the region. Given the high air pollution level, there is a clear and urgent need for setting up a network of long-term air quality monitoring stations in the greater Lumbini region.

Description: PAH concentrations were measured in total suspended particle (TSP) samples collected from six sites along two south-north transects across the central Himalayas from April 2013 to March 2014. The annual average TSP and PAH (especially 5- and 6-ring compounds) concentrations were found to decrease noticeably northwards along both transects. At rural and urban sites, the TSP and PAH concentrations showed clear seasonal variations, with the lower concentrations around the mid-monsoon season and the higher values in the winter season. Meanwhile, at the remote sites (e.g., Nyalam and Zhongba), these pollutants generally remained constant throughout the year but with relatively higher levels during the pre-monsoon season. Both IndP/(IndP + BghiP) and Fla/(Fla + Pyr) ratios suggested that atmospheric PAHs from urban and rural sites were mainly associated with emissions from biomass burning, coal burning and petroleum combustion. However, the contribution of biomass burning increased at remote sites. Similar compositions of PAHs were found at three remote sites located on both sides of the Himalayas (Jomsom, Zhongba, and Nyalam), suggesting that the northern side of the Himalayas may be affected by anthropogenic emissions from the Indo-Gangetic Plain (IGP) via long-range atmospheric transport. This work provides a database of PAHs in central Himalayas for further assessing environmental risk of air pollution in the remote regions.