Abstract

Abstract. Mt. Waliguan Observatory (WLG) is a World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) global baseline station in China. WLG is located at the northeastern part of the Tibetan Plateau (36∘17′ N, 100∘54′ E, 3816 m a.s.l.) and is representative of the pristine atmosphere over the Eurasian continent. We made long-term ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements at WLG during the period 2012–2015. In this study, we retrieve the differential slant column densities (dSCDs) and estimate the tropospheric background mixing ratios of different trace gases, including NO2, SO2, HCHO, and BrO, using the measured spectra at WLG. Averaging of 10 original spectra is found to be an “optimum option” for reducing both the statistical error of the spectral retrieval and systematic errors in the analysis. The dSCDs of NO2, SO2, HCHO, and BrO under clear-sky and low-aerosol-load conditions are extracted from measured spectra at different elevation angles at WLG. By performing radiative transfer simulations with the model TRACY-2, we establish approximate relationships between the trace gas dSCDs at 1∘ elevation angle and the corresponding average tropospheric background volume mixing ratios. Mixing ratios of these trace gases in the lower troposphere over WLG are estimated to be in a range of about 7 ppt (January) to 100 ppt (May) for NO2, below 0.5 ppb for SO2, between 0.4 and 0.9 ppb for HCHO, and lower than 0.3 ppt for BrO. The chemical box model simulations constrained by the NO2 concentration from our MAX-DOAS measurements show that there is a little net ozone loss (−0.8 ppb d−1) for the free-tropospheric conditions and a little net ozone production (0.3 ppb d−1) for the boundary layer conditions over WLG during summertime. Our study provides valuable information and data sets for further investigating tropospheric chemistry in the background atmosphere and its links to anthropogenic activities.

Highlights

  • Nitrogen oxides (NOx ≡ Nitric oxide (NO) + NO2), sulfur dioxide (SO2), formaldehyde (HCHO), and bromine monoxide (BrO) are important traces gases in tropospheric chemistry

  • Nitrogen oxides (NOx ≡ NO + NO2), sulfur dioxide (SO2), formaldehyde (HCHO), and bromine monoxide (BrO) are important traces gases in tropospheric chemistry. Both NOx and HCHO participate in the control of the strong oxidant O3, which is an indicator of photochemical smog, and the strongest atmospheric oxidizing agent OH, which determines the lifetimes of many gaseous pollutants and greenhouse gases in the atmosphere (Seinfeld and Pandis, 2006; Ma et al, 2012; Lelieveld et al, 2016)

  • HCHO in the remote atmosphere is produced through the oxidation of methane (CH4) and non-methane volatile organic compounds (NMVOCs), and it is emitted from anthropogenic combustion processes, biomass burning, and natural vegetation (Stavrakou et al, 2009)

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Summary

Introduction

Nitrogen oxides (NOx ≡ NO + NO2), sulfur dioxide (SO2), formaldehyde (HCHO), and bromine monoxide (BrO) are important traces gases in tropospheric chemistry. Both NOx and HCHO participate in the control of the strong oxidant O3, which is an indicator of photochemical smog, and the strongest atmospheric oxidizing agent OH, which determines the lifetimes of many gaseous pollutants and greenhouse gases in the atmosphere (Seinfeld and Pandis, 2006; Ma et al, 2012; Lelieveld et al, 2016). HCHO in the remote atmosphere is produced through the oxidation of methane (CH4) and non-methane volatile organic compounds (NMVOCs), and it is emitted from anthropogenic combustion processes, biomass burning, and natural vegetation (Stavrakou et al, 2009)

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