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 characterise 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. In the study, 71 ion peaks (for which measured ambient concentrations exceeded the 2σ 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 / m > 4200) and temporal resolution (1 min) of the PTR-TOF-MS. The concentration ranking in the average VOC mixing ratios dur-ing our wintertime deployment was acetaldehyde (8.8 ppb) > methanol (7.4 ppb) > acetone + propanal (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) > 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 to 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 Published by Copernicus Publications on behalf of the European Geosciences Union. C. Sarkar et al.: Wintertime high acetaldehyde, isoprene and isocyanic acid in Kathmandu Valleyas propyne, propene, benzene and propanenitrile, which correlated strongly with acetonitrile (r 2 > 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 is...

One seventh of the world's population lives in the Indo-Gangetic Plain (IGP) and the fertile region sustains agricultural food crop production for much of South Asia, yet it remains one of the most under-studied regions of the world in terms of atmospheric composition and chemistry. In particular, the emissions and chemistry of volatile organic compounds (VOCs) that form surface ozone and secondary organic aerosol through photochemical reactions involving nitrogen oxides are not well understood. In this study, ambient levels of VOCs such as methanol, acetone, acetaldehyde, acetonitrile and isoprene were measured for the first time in the IGP. A new atmospheric chemistry facility that combines India's first highsensitivity proton transfer reaction mass spectrometer, an ambient air quality station and a meteorological station, was used to quantify in situ levels of several VOCs and air pollutants in May 2012 at a suburban site in Mohali (northwest IGP). Westerly winds arriving at high wind speeds (5-20 m s −1 ) in the pre-monsoon season at the site were conducive for chemical characterization of regional emission signatures. Average levels of VOCs and air pollutants in May 2012 ranged from 1.2 to 2.7 nmol mol −1 for aromatic VOCs, 5.9 to 37.5 nmol mol −1 for the oxygenated VOCs, 1.4 nmol mol −1 for acetonitrile, 1.9 nmol mol −1 for isoprene, 567 nmol mol −1 for carbon monoxide, 57.8 nmol mol −1 for ozone, 11.5 nmol mol −1 for nitrogen oxides, 7.3 nmol mol −1 for sulfur dioxide, 104 µg m −3 for PM 2.5 and 276 µg m −3 for PM 10 . By analyzing the one-minute in situ data with meteorological parameters and applying chemical tracers (e.g., acetonitrile for biomass burning) and inter-VOC correlations, we were able to constrain major emission source

Abstract. In this study we use a high-quality data set of in situ ozone measurements at a suburban site called Mohali in the state of Punjab to estimate ozone-related crop yield losses for wheat, rice, cotton and maize for Punjab and the neighbouring state Haryana for the years 2011–2013. We intercompare crop yield loss estimates according to different exposure metrics, such as AOT40 (accumulated ozone exposure over a threshold of 40) and M7 (mean 7-hour ozone mixing ratio from 09:00 to 15:59), for the two major crop growing seasons of kharif (June–October) and rabi (November–April) and establish a new crop-yield–exposure relationship for southern Asian wheat, maize and rice cultivars. These are a factor of 2 more sensitive to ozone-induced crop yield losses compared to their European and American counterparts. Relative yield losses based on the AOT40 metrics ranged from 27 to 41 % for wheat, 21 to 26 % for rice, 3 to 5 % for maize and 47 to 58 % for cotton. Crop production losses for wheat amounted to 20.8 ± 10.4 million t in the fiscal year of 2012–2013 and 10.3 ± 4.7 million t in the fiscal year of 2013–2014 for Punjab and Haryana taken together. Crop production losses for rice totalled 5.4 ± 1.2 million t in the fiscal year of 2012–2013 and 3.2 ± 0.8 million t in the year 2013–2014 for Punjab and Haryana taken together. The Indian National Food Security Ordinance entitles ~ 820 million of India's poor to purchase about 60 kg of rice or wheat per person annually at subsidized rates. The scheme requires 27.6 Mt of wheat and 33.6 Mt of rice per year. The mitigation of ozone-related crop production losses in Punjab and Haryana alone could provide > 50 % of the wheat and ~ 10 % of the rice required for the scheme. The total economic cost losses in Punjab and Haryana amounted to USD 6.5 ± 2.2 billion in the fiscal year of 2012–2013 and USD 3.7 ± 1.2 billion in the fiscal year of 2013–2014. This economic loss estimate represents a very conservative lower limit based on the minimum support price of the crop, which is lower than the actual production costs. The upper limit for ozone-related crop yield losses in all of India currently amounts to 3.5–20 % of India's GDP. The mitigation of high surface ozone would require relatively little investment in comparison to the economic losses incurred presently. Therefore, ozone mitigation can yield massive benefits in terms of ensuring food security and boosting the economy. The co-benefits of ozone mitigation also include a decrease in the ozone-related mortality and morbidity and a reduction of the ozone-induced warming in the lower troposphere.

Abstract.A positive matrix factorization model (US EPA PMF version 5.0) was applied for the source apportionment of the dataset of 37 non-methane volatile organic compounds (NMVOCs) measured from 19 December 2012 to 30 January 2013 during the SusKat-ABC international air pollution measurement campaign using a proton-transfer-reaction time-of-flight mass spectrometer in the Kathmandu Valley. In all, eight source categories were identified with the PMF model using the new constrained model operation mode. Unresolved industrial emissions and traffic source factors were the major contributors to the total measured NMVOC mass loading (17.9 and 16.8 %, respectively) followed by mixed industrial emissions (14.0 %), while the remainder of the source was split approximately evenly between residential biofuel use and waste disposal (10.9 %), solvent evaporation (10.8 %), biomass co-fired brick kilns (10.4 %), biogenic emissions (10.0 %) and mixed daytime factor (9.2 %). Conditional probability function (CPF) analyses were performed to identify the physical locations associated with different sources. Source contributions to individual NMVOCs showed that biomass co-fired brick kilns significantly contribute to the elevated concentrations of several health relevant NMVOCs such as benzene. Despite the highly polluted conditions, biogenic emissions had the largest contribution (24.2 %) to the total daytime ozone production potential, even in winter, followed by solvent evaporation (20.2 %), traffic (15.0 %) and unresolved industrial emissions (14.3 %).Secondary organic aerosol (SOA) production had approximately equal contributions from biomass co-fired brick kilns (28.9 %) and traffic (28.2 %). Comparison of PMF results based on the in situ data versus REAS v2.1 and EDGAR v4.2 emission inventories showed that both the inventories underestimate the contribution of traffic and do not take the contribution of brick kilns into account. In addition, the REAS inventory overestimates the contribution of residential biofuel use and underestimates the contribution of solvent use and industrial sources in the Kathmandu Valley. The quantitative source apportionment of major NMVOC sources in the Kathmandu Valley based on this study will aid in improving hitherto largely un-validated bottom-up NMVOC emission inventories, enabling more focused mitigation measures and improved parameterizations in chemical transport models.

O 3 , CO, and NO x affect air quality and tropospheric chemistry but factors that control them in the densely populated N.W. Indo-Gangetic Plain (IGP) are poorly understood. This work presents the first simultaneous 2 year long in situ data set acquired from August 2011 to September 2013 at a N.W. IGP site (30.667°N, 76.729°E; 310 m asl). We investigate the impact of emissions and meteorology on the diel and seasonal variability of O 3 , CO, and NO x . Regional post-harvest crop residue fires contribute majorly to an enhancement of 19 ppb in hourly averaged ozone concentrations under similar meteorological conditions in summer and 7 ppb under conditions of lower radiation during the post monsoon. d [O 3 ]/dt (from sunrise to daytime O 3 maxima) was highest during periods influenced by post-harvest fires in post monsoon season (9.2 ppb h À1 ) and lowest during monsoon season (4.1 ppb h À1 ). Analysis of air mass clusters revealed that enhanced chemical formation of O 3 and not transport was the driver of the summertime and post monsoon ambient O 3 maxima. Despite having high daytime NO x (>12 ppb) and CO (>440 ppb) in winter, average daytime O 3 was less than 40 ppb due to reduced photochemistry and fog. Average daytime O 3 during the monsoon was less than 45 ppb due to washout of precursors and suppressed photochemistry due to cloud cover. The 8 h ambient air quality O 3 standard was violated on 451 days in the period August 2011-September 2013. The results show that substantial mitigation efforts are required to reduce regional O 3 pollution in the N.W. IGP.

Abstract. Biogenic volatile organic compounds (BVOCs) are important components of the atmosphere due to their contribution to atmospheric chemistry and biogeochemical cycles. Tropical forests are the largest source of the dominant BVOC emissions (e.g. isoprene and monoterpenes). In this study, we report isoprene and total monoterpene flux measurements with a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) using the eddy covariance (EC) method at the Tapajós National Forest (2.857∘ S, 54.959∘ W), a primary rainforest in eastern Amazonia. Measurements were carried out from 1 to 16 June 2014, during the wet-to-dry transition season. During the measurement period, the measured daytime (06:00–18:00 LT) average isoprene mixing ratios and fluxes were 1.15±0.60 ppb and 0.55±0.71 mg C m−2 h−1, respectively, whereas the measured daytime average total monoterpene mixing ratios and fluxes were 0.14±0.10 ppb and 0.20±0.25 mg C m−2 h−1, respectively. Midday (10:00–14:00 LT) average isoprene and total monoterpene mixing ratios were 1.70±0.49 and 0.24±0.05 ppb, respectively, whereas midday average isoprene and monoterpene fluxes were 1.24±0.68 and 0.46±0.22 mg C m−2 h−1, respectively. Isoprene and total monoterpene emissions in Tapajós were correlated with ambient temperature and solar radiation. Significant correlation with sensible heat flux, SHF (r2=0.77), was also observed. Measured isoprene and monoterpene fluxes were strongly correlated with each other (r2=0.93). The MEGAN2.1 (Model of Emissions of Gases and Aerosols from Nature version 2.1) model could simulate most of the observed diurnal variations (r2=0.7 to 0.8) but declined a little later in the evening for both isoprene and total monoterpene fluxes. The results also demonstrate the importance of site-specific vegetation emission factors (EFs) for accurately simulating BVOC fluxes in regional and global BVOC emission models.

Abstract. Many sites in the densely populated Indo-Gangetic Plain (IGP) frequently exceed the national ambient air quality standard (NAAQS) of 100 μg m−3 for 24 h average PM10 and 60 μg m−3 for 24 h average PM2.5 mass loadings, exposing residents to hazardous levels of particulate matter (PM) throughout the year. We quantify the contribution of long-range transport to elevated PM levels and the number of exceedance events through a back-trajectory climatology analysis of air masses arriving at the IISER Mohali Atmospheric Chemistry facility (30.667° N, 76.729° E; 310 m a.m.s.l.) for the period August 2011–June 2013. Air masses arriving at the receptor site were classified into six clusters, which represent synoptic-scale air-mass transport patterns. Long-range transport from the west leads to significant enhancements in the average fine- and coarse-mode PM mass loadings during all seasons. The contribution of long-range transport from the west and south-west (source regions: Arabia, Thar Desert, Middle East and Afghanistan) to coarse-mode PM varied between 9 and 57 % of the total PM10–2.5 mass. Local pollution episodes (wind speed < 1 m s−1) contributed to enhanced PM2.5 mass loadings during both the winter and summer seasons and to enhanced coarse-mode PM only during the winter season. South-easterly air masses (source region: eastern IGP) were associated with significantly lower fine- and coarse-mode PM mass loadings during all seasons. The fraction of days in each season during which the PM mass loadings exceeded the national ambient air quality standard was controlled by long-range transport to a much lesser degree. For the local cluster, which represents regional air masses (source region: NW-IGP), the fraction of days during which the national ambient air quality standard (NAAQS) of 60 μg m−3 for 24 h average PM2.5 was exceeded varied between 36 % of the days associated with this synoptic-scale transport during the monsoon, and 95 % during post-monsoon and winter seasons; the fraction of days during which the NAAQS of 100 μg m−3 for the 24 h average PM10 was exceeded, varied between 48 % during the monsoon and 98 % during the post-monsoon season. Long-range transport was responsible for both, bringing air masses with a significantly lower fraction of exceedance days from the eastern IGP and air masses with a moderate increase in the fraction of exceedance days from the west (source regions: Arabia, Thar Desert, Middle East and Afghanistan). In order to bring PM mass loadings into compliance with the NAAQS and to reduce the number of exceedance days, mitigation of regional combustion sources in the NW-IGP needs to be given highest priority.

&lt;p&gt;&lt;strong&gt;Abstract.&lt;/strong&gt; A positive matrix factorization model (US EPA PMF version 5.0) was applied for the source apportionment of the dataset of 37 NMVOCs measured over a period of 19 December 2012&amp;#8211;30 January 2013 during the SusKat-ABC international air pollution measurement campaign using a Proton Transfer Reaction Time of Flight Mass Spectrometer in the Kathmandu Valley. In all, eight source categories were identified with the PMF model using the new &quot;constrained model operation&quot; mode. Unresolved industrial emissions and traffic source factors were the major contributors to the total measured NMVOC mass loading (17.9&amp;#8201;% and 16.8&amp;#8201;%, respectively) followed by mixed industrial emissions (14.0&amp;#8201;%), while the remainder of the source was split approximately evenly between residential biofuel use and waste disposal (10.9&amp;#8201;%), solvent evaporation (10.8&amp;#8201;%), biomass co-fired brick kilns (10.4&amp;#8201;%), biogenic emissions (10.0&amp;#8201;%) and mixed daytime factor (9.2&amp;#8201;%). Conditional probability function (CPF) analyses were performed to identify the physical locations associated with different sources. Source contributions to individual NMVOCs showed biomass co-fired brick kilns significantly contribute to the elevated concentrations of several health relevant NMVOCs such as benzene. Despite the highly polluted conditions, biogenic emissions had largest contribution (24.2&amp;#8201;%) to the total daytime ozone production potential, even in winter, followed by solvent evaporation (20.2&amp;#8201;%), traffic (15.0&amp;#8201;%) and unresolved industrial emissions (14.3&amp;#8201;%). Secondary organic aerosol (SOA) production had approximately equal contributions from biomass co-fired brick kilns (28.9&amp;#8201;%) and traffic (28.2&amp;#8201;%). Comparison of PMF results based on the in-situ data versus REASv2.1 and EDGAR v4.2 emission inventories showed that both the inventories underestimate the contribution of traffic and do not take the contribution of brick kilns into account. In addition, the REAS inventory overestimates the contribution of residential biofuel use and underestimates the contribution of solvent use and industrial sources in the Kathmandu Valley. The quantitative source apportionment of major NMVOC sources in the Kathmandu Valley based on this will aid in improving hitherto largely un-validated bottom up NMVOC emission inventories, enabling more focused mitigation measures and improved parameterizationsin chemical-transport models.&lt;/p&gt;