Khadak Singh Mahata, Maheswar Rupakheti, Arnico Kumar Panday, Piyush Bhardwaj, Manish Naja, Ashish Singh, Andrea Mues, Paolo Cristofanelli, Deepak Pudasainee, Paolo Bonasoni, Mark Lawrence

• Residents of the Kathmandu Valley experience severe particulate and gaseous air pollution throughout most of the year, even during much of the rainy season. The knowledge base for understanding the air pollution in the Kathmandu Valley was previously very limited, but is improving rapidly due to several field measurement studies conducted in the last few years. Thus far, most analyses of observations in the Kathmandu Valley have been limited to short periods of time at single locations. This study extends on the past studies by examining the spatial and temporal characteristics of two important gaseous air pollutant (CO and O3) based on simultaneous observations over a longer period at five locations within the valley and on its rim, including a supersite (at Bode in the valley center, 1345m above sea level) and four satellite sites (at Paknajol, 1380masl in the Kathmandu city center, at Bhimdhunga (1522masl), a mountain pass on the valley's western rim, at Nagarkot (1901masl), another mountain pass on the eastern rim, and Naikhandi,Residents of the Kathmandu Valley experience severe particulate and gaseous air pollution throughout most of the year, even during much of the rainy season. The knowledge base for understanding the air pollution in the Kathmandu Valley was previously very limited, but is improving rapidly due to several field measurement studies conducted in the last few years. Thus far, most analyses of observations in the Kathmandu Valley have been limited to short periods of time at single locations. This study extends on the past studies by examining the spatial and temporal characteristics of two important gaseous air pollutant (CO and O3) based on simultaneous observations over a longer period at five locations within the valley and on its rim, including a supersite (at Bode in the valley center, 1345m above sea level) and four satellite sites (at Paknajol, 1380masl in the Kathmandu city center, at Bhimdhunga (1522masl), a mountain pass on the valley's western rim, at Nagarkot (1901masl), another mountain pass on the eastern rim, and Naikhandi, near the valley's only river outlet). CO and O3 mixing ratios were monitored from January to July 2013, along with other gases and aerosol particles by instruments deployed at the Bode supersite during the international air pollution measurement campaign SusKat-ABC (Sustainable Atmosphere for the Kathmandu Valley – endorsed by the Atmospheric Brown Clouds program of UNEP). The O3 monitoring at Bode, Paknajol and Nagarkot as well as the CO monitoring at Bode were extended beyond July 2013 to investigate their variability over a complete annual cycle. Higher CO mixing ratios were found at Bode than at the outskirt sites (Bhimdhunga, Naikhandi and Nagarkot), and all sites except Nagarkot showed distinct diurnal cycles of CO mixing ratio with morning peaks and daytime lows. Seasonally, CO was higher during the pre-monsoon and winter seasons, especially due to the emissions from brick kiln industries, which only operate during this period, as well as increased domestic heating during winter, and regional forest fires and agro-residue burning. It was lower during the monsoon due to rainfall, which reduces open burning activities within the valley and in the surrounding regions, and thus reduces the sources of CO. The meteorology of the valley also played a key role in determining the CO mixing ratios. Furthermore, there was evidence of some influence of pollution from the greater region around the valley. A top-down estimate of the CO emission flux was made by using the CO mixing ratio and mixing layer height (MLH) measured at Bode. The estimated annual CO flux at Bode was 4.92μgm−2s−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 O3 mixing ratio was found to be highest during the pre-monsoon season at all sites, while the timing of the seasonal minimum varied across the sites. The daily maximum 8 hour average O3 exceeded the WHO recommended guideline of 50ppb on more days at the hilltop station of Nagarkot (159/357 days) than at the urban valley bottom sites of Paknajol (132/354 days) and Bode (102/353 days), presumably due to the influence of free-tropospheric air at the high-altitude site, as well as to titration of O3 by fresh NOx emissions near the urban sites. More than 78% of the exceedance days were during the pre-monsoon period at all sites. This was due to both favorable meteorological conditions as well as contributions of precursors from regional sources such as forest fires and agro-residue burning. The high O3 mixing ratio observed during the pre-monsoon period is of a high concern for human health and ecosystems, including agroecosystems in the Kathmandu Valley and surrounding regions.…