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...

Abstract. 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, O 3 ) 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 , PM 1 was 3.6-197.6 µg m −3 , PM 2.5 was 6.1-272.2 µg m −3 , PM 10 was 10.5-604.0 µg m −3 , O 3 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 coarsemode PM was found as compared to other nearby sites in the Indo-Gangetic Plain region. The BC / CO ratio obtained in Lumbini indicated considerable contributions of emissions from both residential and transportation sectors. The 24 h average PM 2.5 and PM 10 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 PM 10 , 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 Published by Copernicus Publications on behalf of the European Geosciences Union.

Kathmandu Valley is one of the largest and most polluted metropolitan regions in the Himalayan foothills. Rapidly expanding urban sprawl and a growing fleet of vehicles, and industrial facilities such as brick factories across the valley have led to conditions where ambient concentrations of key gaseous air pollutants are expected to exceed Nepal's National Ambient Air Quality Standards (NAAQS) and World Health Organization (WHO) guidelines. In order to understand the spatial variation of the trace gases in the Kathmandu Valley, passive samples of SO 2 , NO x , NO 2 , NH 3, and O 3 were collected simultaneously from fifteen locations between March and May 2013. A follow-up study during two separate campaigns in 2014 sampled these gases, except ammonia, one site at a time from thirteen urban, suburban and rural stationary sites. In 2013, urban sites were observed to have higher weekly averaged NO 2 and SO 2 (22.4 ± 8.1 µg m -3 and 14.5 ± 11.1 µg m -3 , respectively) than sub-urban sites (9.2 ± 3.9 µg m -3 and 7.6 ± 2.8 µg m -3 , respectively). Regions located within 3 km of brick factories had higher SO 2 concentrations (22.3 ± 14.7 µg m -3 ) than distant sites (5.8 ± 1.1 µg m -3 ). Higher O 3 (108.5 ± 31.4 µg m -3 ) was observed in rural locations compared to urban sites (87.1 ± 9.2 µg m -3 ), emphasizing the importance of meteorological factors and precursor species for ozone production and titration. Parallel to previous studies, these results suggest that ground-level O 3 , as its levels frequently exceeded guidelines throughout the sampling periods, is an important concern throughout the valley. NH 3 near polluted rivers and SO 2 around brick factories are also important pollutants that need more intensive monitoring, primarily due to their importance in particulate matter formation chemistry.

The Indo-Gangetic Plains (IGP) experience high levels of airborne particulate matter (PM), especially during the dry season. Contributing to PM are natural and anthropogenic emissions and the atmospheric transformation of gases to form particles. Regional smog events occur frequently during wintertime and provide an atmospheric medium for aerosol processing. Here, we investigate the chemical composition and sources of PM at a representative site in the northern IGP during the second Nepal Ambient Monitoring and Source Testing Experiment (NAMaSTE 2). In Lumbini, Nepal, the 24 h average PM2.5 and PM10 concentrations ranged 48–295 and 60–343 μg m–3, respectively, from December 20, 2017, to January 1, 2018. On average (± standard deviation), PM2.5 was composed of 39 ± 7% organic carbon (OC), 5 ± 2% elemental carbon (EC), and 20 ± 6% secondary inorganic ions (ammonium, nitrate, and sulfate), 2.0% chloride, and 1.3% potassium. Biomass burning was a major PM source, indicated by a median levoglucosan concentration of 3.5 μg m–3. Secondary organic aerosol (SOA) derived from biomass burning was indicated by high concentrations of nitromonoaromatic compounds (e.g., 4-nitrocatechol peaking at 435 ng m–3). During periods of fog, characterized by high relative humidity (RH) and relatively low solar radiation, nitroaromatic concentrations dropped despite levoglucosan remaining high, indicating that their formation was suppressed. Chemical signatures of SOA indicated that volatile organic compound (VOC) precursors were primarily combustion-derived, with small contributions from biogenic VOC. Through molecular markers and chemical mass balance (CMB) modeling, sources of PM2.5 OC were identified as cow dung burning (24 ± 16%), other biomass burning (20 ± 7%), plastic/garbage burning (4.7 ± 3.2%), vehicle emissions (3.1 ± 1.4%), coal combustion (0.3 ± 0.2%), and SOA from monoaromatic VOC (4.1 ± 0.8%), diaromatic VOC (8.9 ± 4.0%), cresol (0.3 ± 0.4%), isoprene (0.4 ± 0.2%), monoterpenes (1.5 ± 0.6%), and sesquiterpenes (3.2 ± 0.7%). Understanding the levels of PM in Lumbini, along with its chemical composition and sources of OC, contributes to a better understanding of regional air quality episodes in the IGP.

Abstract. The SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley-Atmospheric Brown Clouds) international air pollution measurement campaign was carried out from December 2012 to June 2013 in the Kathmandu Valley and surrounding regions in Nepal. The Kathmandu Valley is a bowl-shaped basin with a severe air pollution problem. This paper reports measurements of two major greenhouse gases (GHGs), methane (CH 4 ) and carbon dioxide (CO 2 ), along with the pollutant CO, that began during the campaign and were extended for 1 year at the SusKat-ABC supersite in Bode, a semi-urban location in the Kathmandu Valley. Simultaneous measurements were also made during 2015 in Bode and a nearby rural site (Chanban) ∼ 25 km (aerial distance) to the southwest of Bode on the other side of a tall ridge. The ambient mixing ratios of methane (CH 4 ), carbon dioxide (CO 2 ), water vapor, and carbon monoxide (CO) were measured with a cavity ring-down spectrometer (G2401; Picarro, USA) along with meteorological parameters for 1 year (March 2013-March 2014. These measurements are the first of their kind in the central Himalayan foothills. At Bode, the annual average mixing ratios of CO 2 and CH 4 were 419.3 (±6.0) ppm and 2.192 (±0.066) ppm, respectively. These values are higher than the levels observed at background sites such as Mauna Loa, USA (CO 2 : 396.8 ± 2.0 ppm, CH 4 : 1.831 ± 0.110 ppm) and Waliguan, China (CO 2 : 397.7 ± 3.6 ppm, CH 4 : 1.879 ± 0.009 ppm) during the same period and at other urban and semi-urban sites in the region, such as Ahmedabad and Shadnagar (India). They varied slightly across the seasons at Bode, with seasonal average CH 4 mixing ratios of 2.157 (±0.230) ppm in the pre-monsoon season, 2.199 (±0.241) ppm in the monsoon, 2.210 (±0.200) ppm in the post-monsoon, and 2.214 (±0.209) ppm in the winter season. The average CO 2 mixing ratios were 426.2 (±25.5) ppm in the pre-monsoon, 413.5 (±24.2) ppm in the monsoon, 417.3 (±23.1) ppm in the postmonsoon, and 421.9 (±20.3) ppm in the winter season. The maximum seasonal mean mixing ratio of CH 4 in winter was only 0.057 ppm or 2.6 % higher than the seasonal minimum during the pre-monsoon period, while CO 2 was 12.8 ppm or 3.1 % higher during the pre-monsoon period (seasonal maximum) than during the monsoon (seasonal minimum). On the other hand, the CO mixing ratio at Bode was 191 % higher during the winter than during the monsoon season. The enhancement in CO 2 mixing ratios during the pre-monsoon season is associated with additional CO 2 emissions from forest fires and agro-residue burning in northern South Asia in addition to local emissions in the Kathmandu Valley. Published CO/CO 2 ratios of different emission sources in Nepal and India were compared with the observed CO/CO 2 ratios in this study. This comparison suggested that the major sources in the Kathmandu Valley were residential cooking and vehicle exhaust in all seasons except winter. In winter, brick kiln emissions were a major source. Simultaneous measurements in Bode and Chanban (15 July-3 O...

Abstract. Air pollution resulting from rapid urbanization and associated human activities in the Kathmandu Valley of Nepal has been leading to serious public health concerns over the past 2 decades. These concerns led to a multinational field campaign SusKat-ABC (Sustainable atmosphere for the Kathmandu Valley – Atmospheric Brown Clouds) that measured different trace gases, aerosols and meteorological parameters in the Kathmandu Valley and surrounding regions during December 2012 to June 2013 to understand local- to regional-scale processes influencing air quality of the Kathmandu Valley. This study provides information about the regional distribution of ozone and some precursor gases using simultaneous in situ measurements from a SusKat-ABC supersite at Bode, Nepal, and two Indian sites: a high-altitude site, Nainital, located in the central Himalayan region and a low-altitude site, Pantnagar, located in the Indo-Gangetic Plain (IGP). The diurnal variations at Bode showed a daytime buildup in O3 while CO shows morning and evening peaks. Similar variations (with lower levels) were also observed at Pantnagar but not at Nainital. Several events of hourly ozone levels exceeding 80 ppbv were also observed at Bode. The CO levels showed a decrease from their peak level of about 2000 ppbv in January to about 680 ppbv in June at Bode. The hourly mean ozone and CO levels showed a strong negative correlation during winter (r2 = 0.82 in January and r2 = 0.71 in February), but this negative correlation gradually becomes weaker, with the lowest value in May (r2 = 0.12). The background O3 and CO mixing ratios at Bode were estimated to be about 14 and 325 ppbv, respectively. The rate of change of ozone at Bode showed a more rapid increase ( ∼ 17 ppbv h−1) during morning than the decrease in the evening (5–6 ppbv h−1), suggesting the prevalence of a semi-urban environ. The lower CO levels during spring suggest that regional transport also contributes appreciably to springtime ozone enhancement in the Kathmandu Valley on top of the local in situ ozone production. We show that regional pollution resulting from agricultural crop residue burning in northwestern IGP led to simultaneous increases in O3 and CO levels at Bode and Nainital during the first week of May 2013. A biomass-burning-induced increase in ozone and related gases was also confirmed by a global model and balloon-borne observations over Nainital. A comparison of surface ozone variations and composition of light non-methane hydrocarbons among different sites indicated the differences in emission sources of the Kathmandu Valley and the IGP. These results highlight that it is important to consider regional sources in air quality management of the Kathmandu Valley.

Abstract. Anthropogenic emissions from the combustion of fossil fuels and biomass in Asia have increased in recent years. High concentrations of reactive trace gases and lightabsorbing and light-scattering particles from these sources form persistent haze layers, also known as atmospheric brown clouds, over the Indo-Gangetic plains (IGP) from December through early June. Models and satellite imagery suggest that strong wind systems within deep Himalayan valleys are major pathways by which pollutants from the IGP are transported to the higher Himalaya. However, observational evidence of the transport of polluted air masses through Himalayan valleys has been lacking to date. To evaluate this pathway, we measured black carbon (BC), ozone (O 3 ), and associated meteorological conditions within the Kali Gandaki Valley (KGV), Nepal, from January 2013 to July 2015. BC and O 3 varied over both diurnal and seasonal cycles. Relative to nighttime, mean BC and O 3 concentrations within the valley were higher during daytime when the up-valley flow (average velocity of 17 m s −1 ) dominated. BC and O 3 concentrations also varied seasonally with minima during the monsoon season (July to September). Concentrations of both species subsequently increased post-monsoon and peaked during March to May. Average concentrations for O 3 during the seasonally representative months of April, August, and November were 41.7, 24.5, and 29.4 ppbv, respectively, while the corresponding BC concentrations were 1.17, 0.24, and 1.01 µg m −3 , respectively. Up-valley fluxes of BC were significantly greater than down-valley fluxes during all seasons. In addition, frequent episodes of BC concentrations 2-3 times higher than average persisted from several days to a week during non-monsoon months. Our observations of increases in BC concentration and fluxes in the valley, particularly during pre-monsoon, provide evidence that trans-Himalayan valleys are important conduits for transport of pollutants from the IGP to the higher Himalaya.

Published by Copernicus Publications on behalf of the European Geosciences Union. 14114 K. S. Mahata et al.: Ozone and carbon monoxide in the Kathmandu Valleythe night and early morning. The MLH slowly increases after sunrise and decreases in the afternoon. As a result, the westerly wind becomes active and reduces the mixing ratio during the daytime. Furthermore, there was evidence of an increase in the O 3 mixing ratios in the Kathmandu Valley as a result of emissions in the Indo-Gangetic Plain (IGP) region, particularly from biomass burning including agroresidue burning. A top-down estimate of the CO emission flux was made by using the CO mixing ratio and mixing layer height measured at Bode. The estimated annual CO flux at Bode was 4.9 µg m −2 s −1 , which is 2-14 times higher than that in widely used emission inventory databases (EDGAR HTAP, REAS and INTEX-B). This difference in CO flux between Bode and other emission databases likely arises from large uncertainties in both the top-down and bottom-up approaches to estimating the emission flux. The O 3 mixing ratio was found to be highest during the premonsoon season at all sites, while the timing of the seasonal minimum varied across the sites. The daily maximum 8 h average O 3 exceeded the WHO recommended guideline of 50 ppb on more days at the hilltop station of Nagarkot (159 out of 357 days) than at the urban valley bottom sites of Paknajol (132 out of 354 days) and Bode (102 out of 353 days), presumably due to the influence of free-tropospheric air at the high-altitude site (as also indicated by Putero et al., 2015, for the Paknajol site in the Kathmandu Valley) as well as to titration of O 3 by fresh NO x emissions near the urban sites. More than 78 % of the exceedance days were during the premonsoon period at all sites. The high O 3 mixing ratio observed during the premonsoon period is of a concern for human health and ecosystems, including agroecosystems in the Kathmandu Valley and surrounding regions.