scholarly journals MAX-DOAS measurements of NO<sub>2</sub>, SO<sub>2</sub>, HCHO, and BrO at the Mt. Waliguan WMO GAW global baseline station in the Tibetan Plateau

2020 ◽  
Vol 20 (11) ◽  
pp. 6973-6990 ◽  
Author(s):  
Jianzhong Ma ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Junli Jin ◽  
Siyang Cheng ◽  
...  

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.

2020 ◽  
Author(s):  
Jianzhong Ma ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Junli Jin ◽  
Siyang Cheng ◽  
...  

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 has a representativeness of the pristine atmosphere over the Eurasian continent. We made long-term ground-based MAX-DOAS measurements at WLG during the years 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. We find averaging of 10 original spectra to be an optimum option for reducing both the statistical error of the spectral retrieval and systematic errors in the analysis. We retrieve the dSCDs of NO2, SO2, HCHO and BrO from measured spectra at different elevation angles under clear sky and low aerosol load conditions 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 between about 5 ppt (winter) and 70 ppt (summer) for NO2, fall below 0.5 ppb for SO2, range between about 0.3 and 0.7 ppb for HCHO, and be close to ~ 0 ppt for BrO. Our study provides valuable information and data set for further investigating tropospheric background levels of these trace gases and their relationship to anthropogenic activities.


2021 ◽  
Author(s):  
Sebastian Donner ◽  
Steffen Dörner ◽  
Joelle Buxmann ◽  
Steffen Beirle ◽  
David Campbell ◽  
...  

&lt;p&gt;Multi-AXis (MAX)-Differential Optical Absorption Spectroscopy (DOAS) instruments record spectra of scattered sun light under different elevation angles. From such measurements tropospheric vertical column densities (VCDs) and vertical profiles of different atmospheric trace gases and aerosols can be determined for the lower troposphere. These measurements allow a simultaneous observation of multiple trace gases, e.g. formaldehyde (HCHO), glyoxal (CHOCHO) and nitrogen dioxide (NO&lt;sub&gt;2&lt;/sub&gt;), with the same measurement setup. Since November 2018, a MAX-DOAS instrument has been operating at Bayfordbury Observatory, which is located approximately 30 km north of London. This measurement site is operated by the University of Hertfordshire and equipped with an AERONET station, a LIDAR and multiple instruments to measure meteorological quantities and solar radiation. Depending on the prevailing wind direction the air masses at the measurement site can be dominated by the pollution of London (SE to SW winds) or rather pristine air (northerly winds).&lt;/p&gt;&lt;p&gt;First results already showed that the highest formaldehyde and glyoxal columns are observed for southerly to southeasterly winds indicating the influence of the anthropogenic emissions of London. However, the detailed patterns of the different trace gases were found to be more complex. Therefore, this measurement site is well suited to study the influence of anthropogenic pollution on the atmospheric composition and chemistry at a rather pristine location in the vicinity of London, a major European capital with about 10 million inhabitants and 4 major international airports.&lt;/p&gt;&lt;p&gt;In this study, trace gas and aerosol profiles are retrieved using the MAinz Profile Algorithm (MAPA) with a focus on tropospheric HCHO which plays an important role in tropospheric chemistry. The HCHO results are combined with the results of other trace species such as NO&lt;sub&gt;2&lt;/sub&gt;, CHOCHO and aerosols in order to identify pollution levels, emission sources and different chemical regimes.&lt;/p&gt;


2014 ◽  
Vol 7 (11) ◽  
pp. 11653-11709 ◽  
Author(s):  
I. Ortega ◽  
T. Koenig ◽  
R. Sinreich ◽  
D. Thomson ◽  
R. Volkamer

Abstract. We present an innovative instrument telescope, and describe a retrieval method to probe 3-D distributions of atmospheric trace gases that are relevant to air pollution and tropospheric chemistry. The University of Colorado (CU) two dimensional (2-D) Multi-AXis-Differential Optical Absorption Spectroscopy (CU 2D-MAX-DOAS) instrument measures nitrogen dioxide (NO2), formaldehyde (HCHO), glyoxal (CHOCHO), oxygen dimer (O2-O2, or O4) and water vapor (H2O); also nitrous acid (HONO), bromine monoxide (BrO), iodine monoxide (IO) among other gases can in principle be measured. Information about aerosols is derived through coupling with a radiative transfer model (RTM). The 2-D telescope has 3 modes of operation: (mode 1) measures solar scattered photons from any pair of elevation angle (−20° < EA < +90° or zenith; zero is to the horizon) and azimuth angle (−180° < AA < +180°; zero being North), (mode 2) measures any set of AA at constant EA (almucantar scans); and (mode 3) tracks the direct solar beam via a separate view port. Vertical profiles of trace gases are measured, and used to estimate planetary boundary layer height (PBL). Horizontal distributions are then derived using PBL and parameterization of RTM (Sinreich et al., 2013). NO2 is evaluated at different wavelengths (350, 450, and 560 nm), exploiting the fact that the effective path length varies systematically with wavelength. The area probed is constrained by O4 observations at nearby wavelengths, and has an effective radius of 7.5 to 20 km around the instrument location; i.e., up to 1250 km2 can be sampled near-instantaneously, and with high time resolution. The instrument was deployed as part of the Multi Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany from 7 June to 6 July 2013. We present first measurements (modes 1 and 2 only) and describe a four-step retrieval to derive (a) boundary layer vertical profiles of NO2 and PBL; (b) near-surface horizontal distributions of NO2; (c) range resolved NO2 horizontal distribution measurements using an "onion peeling" approach; and (d) the ratios HCHO-to-NO2 (RFN), CHOCHO-to-NO2 (RGN), and CHOCHO-to-HCHO (RGF) at 14 pre-set azimuth angles distributed over a 360° view. 2D-MAX-DOAS provides an innovative, regional perspective about trace gases, their spatial and temporal concentration gradients, and maximizes information to compare near-surface observations with atmospheric models and satellites.


2015 ◽  
Vol 8 (6) ◽  
pp. 2371-2395 ◽  
Author(s):  
I. Ortega ◽  
T. Koenig ◽  
R. Sinreich ◽  
D. Thomson ◽  
R. Volkamer

Abstract. We present an innovative instrument telescope and describe a retrieval method to probe three-dimensional (3-D) distributions of atmospheric trace gases that are relevant to air pollution and tropospheric chemistry. The University of Colorado (CU) two-dimensional (2-D) multi-axis differential optical absorption spectroscopy (CU 2-D-MAX-DOAS) instrument measures nitrogen dioxide (NO2), formaldehyde (HCHO), glyoxal (CHOCHO), oxygen dimer (O2–O2, or O4), and water vapor (H2O); nitrous acid (HONO), bromine monoxide (BrO), and iodine monoxide (IO) are among other gases that can in principle be measured. Information about aerosols is derived through coupling with a radiative transfer model (RTM). The 2-D telescope has three modes of operation: mode 1 measures solar scattered photons from any pair of elevation angle (−20° < EA < +90° or zenith; zero is to the horizon) and azimuth angle (−180° < AA < +180°; zero being north); mode 2 measures any set of azimuth angles (AAs) at constant elevation angle (EA) (almucantar scans); and mode 3 tracks the direct solar beam via a separate view port. Vertical profiles of trace gases are measured and used to estimate mixing layer height (MLH). Horizontal distributions are then derived using MLH and parameterization of RTM (Sinreich et al., 2013). NO2 is evaluated at different wavelengths (350, 450, and 560 nm), exploiting the fact that the effective path length varies systematically with wavelength. The area probed is constrained by O4 observations at nearby wavelengths and has a diurnal mean effective radius of 7.0 to 25 km around the instrument location; i.e., up to 1960 km2 can be sampled with high time resolution. The instrument was deployed as part of the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, from 7 June to 6 July 2013. We present first measurements (modes 1 and 2 only) and describe a four-step retrieval to derive (a) boundary layer vertical profiles and MLH of NO2; (b) near-surface horizontal distributions of NO2; (c) range-resolved NO2 horizontal distribution measurements using an "onion-peeling" approach; and (d) the ratios HCHO to NO2 (RFN), CHOCHO to NO2 (RGN), and CHOCHO to HCHO (RGF) at 14 pre-set azimuth angles distributed over a 360° view. Three-dimensional distribution measurements with 2-D-MAX-DOAS provide an innovative, regional perspective of trace gases as well as their spatial and temporal concentration gradients, and they maximize information to compare near-surface observations with atmospheric models and satellites.


2017 ◽  
Author(s):  
Xiufeng Yin ◽  
Shichang Kang ◽  
Benjamin de Foy ◽  
Zhiyuan Cong ◽  
Jiali Luo ◽  
...  

Abstract. Ozone is an important pollutant and greenhouse gas, and tropospheric ozone variations are generally associated with both natural and anthropogenic processes. As one of the most pristine and inaccessible regions in the world, the Tibetan Plateau has been considered as an ideal region for studying processes of the background atmosphere. Due to the vast area of the Tibetan Plateau, sites in the southern, northern and central regions exhibit different patterns of variation in surface ozone. Here, we present long-term measurements for ~ 5 years (January 2011 to October 2015) of surface ozone mixing ratios at Nam Co Station, which is a regional background site in the inland Tibetan Plateau. An average surface ozone mixing ratio of 47.6 ± 11.6 ppb was recorded, and a large annual cycle was observed with maximum ozone mixing ratios in the spring and minimum ratios during the winter. The diurnal cycle is characterized by a minimum in the early morning and a maximum in the late afternoon. Nam Co Station represents a background region where surface ozone receives negligible local anthropogenic emissions. Surface ozone at Nam Co Station is mainly dominated by natural processes involving photochemical reactions and potential local vertical mixing. Model results indicate that the study site is affected by the surrounding areas in different seasons and that air masses from the northern Tibetan Plateau lead to increased ozone levels in the summer. In contrast to the surface ozone levels at the edges of the Tibetan Plateau, those at Nam Co Station are less affected by stratospheric intrusions and human activities which makes Nam Co Station representative of vast background areas in the central Tibetan Plateau. By comparing measurements at Nam Co Station with those from other sites in the Tibetan Plateau and beyond, we aim to expand the understanding of ozone cycles and transport processes over the Tibetan Plateau. This work may provide a reference for model simulations in the future.


2017 ◽  
Author(s):  
Chengzhi Xing ◽  
Cheng Liu ◽  
Shanshan Wang ◽  
Ka Lok Chan ◽  
Yang Gao ◽  
...  

Abstract. Ground based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) and lidar measurements were performed in Shanghai, China during May 2016 to investigate the summertime atmospheric pollutants vertical distribution. In this study, vertical profiles of aerosol extinction coefficient, nitrogen dioxide (NO2) and formaldehyde (HCHO) concentrations were retrieved from MAX-DOAS measurement using the Heidelberg Profile (HeiPro) algorithm, while vertical distribution of ozone (O3) was obtained from an ozone lidar. Sensitivity study of the MAX-DOAS aerosol profile retrieval shows that the a priori aerosol profile shape has significant influences on the aerosol profile retrieval. Aerosol profiles retrieved from MAX-DOAS measurements with Gaussian a priori demonstrate the best agreements with simultaneous lidar measurements and vehicle-based tethered-balloon observations among all a priori aerosol profiles. MAX-DOAS measured tropospheric NO2Vertical Column Densities (VCDs) show a good agreement with OMI satellite observations with Pearson correlation coefficient (R) of 0.95. In addition, measurements of the O3 vertical distribution indicate that the ozone productions do not only occur at surface level but also at higher altitudes (about 1.1 km). Planetary boundary layer (PBL) height, horizontal and vertical wind fields information were integrated to discuss the ozone formation at upper altitudes. The results reveal that enhanced ozone concentrations at ground and upper altitudes are not directly related to horizontal and vertical transportations. Similar patterns of O3 and HCHO vertical distributions were observed during this campaign, which implies that the ozone productions near to the surface and at higher altitudes are mainly influenced by the abundance of volatile organic compounds (VOCs) in the lower troposphere.


2007 ◽  
Vol 8 (4) ◽  
pp. 770-789 ◽  
Author(s):  
Guoxiong Wu ◽  
Yimin Liu ◽  
Qiong Zhang ◽  
Anmin Duan ◽  
Tongmei Wang ◽  
...  

Abstract This paper attempts to provide some new understanding of the mechanical as well as thermal effects of the Tibetan Plateau (TP) on the circulation and climate in Asia through diagnosis and numerical experiments. The air column over the TP descends in winter and ascends in summer and regulates the surface Asian monsoon flow. Sensible heating on the sloping lateral surfaces appears from the authors’ experiments to be the major driving source. The retarding and deflecting effects of the TP in winter generate an asymmetric dipole zonal-deviation circulation, with a large anticyclone gyre to the north and a cyclonic gyre to the south. Such a dipole deviation circulation enhances the cold outbreaks from the north over East Asia, results in a dry climate in south Asia and a moist climate over the Indochina peninsula and south China, and forms the persistent rainfall in early spring (PRES) in south China. In summer the TP heating generates a cyclonic spiral zonal-deviation circulation in the lower troposphere, which converges toward and rises over the TP. It is shown that because the TP is located east of the Eurasian continent, in summertime the meridional winds and vertical motions forced by the Eurasian continental-scale heating and the TP local heating are in phase over the eastern and central parts of the continent. The monsoon in East Asia and the dry climate in middle Asia are therefore intensified.


2018 ◽  
Author(s):  
Yang Wang ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Sebastian Böhnke ◽  
Isabelle De Smedt ◽  
...  

Abstract. A Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18° N, 114.36° E) in the suburban area of Xingtai (one of the most polluted cities in China) during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ~ 3.5 ppb. Underestimates of MAX-DOAS results compared to in situ measurements of NO2 (~ 60 %), SO2 (~ 20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2, SO2 are reasonably consistent with those measured by a collocated Raman Lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO, and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ~ 1.4 km) than did NO2, SO2, and HONO (with 75 % integrated column below ~ 0.5 km) under polluted condition. Lifted layers were systematically observed for all species, (except HONO), indicating accumulation, secondary formation, or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2, and HONO, but around noon for aerosols, HCHO, and CHOCHO, mainly dominated by photochemistry, characteristic upslope/downslope circulation and PBL dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution from the southern areas such as industrialized Wuan. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases, and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations of HCHO, CHOCHO and aerosols.


2020 ◽  
Author(s):  
Ermioni Dimitropoulou ◽  
Francois Hendrick ◽  
Martine M. Friedrich ◽  
Gaia Pinardi ◽  
Frederik Tack ◽  
...  

&lt;p&gt;Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of aerosols, tropospheric nitrogen dioxide (NO&lt;sub&gt;2&lt;/sub&gt;) and formaldehyde (HCHO) have been carried out in Uccle, Brussels, during two years (March 2018 &amp;#8211; March 2020). The MAX-DOAS instrument has been operating in both UV and visible (Vis) wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction (the so-called main azimuthal direction) pointing and (2) an azimuthal scan in a fixed low elevation angle (2&lt;sup&gt;o&lt;/sup&gt;). By applying a vertical profile inversion algorithm in the main azimuthal direction and an adapted version of the parameterization technique proposed by Sinreich et al. (2013) in the other azimuthal directions, near-surface &amp;#160;concentrations (VMRs) and vertical column densities (VCDs) are retrieved in ten different azimuthal directions.&lt;/p&gt;&lt;p&gt;The present work focuses on the seasonal horizontal variation of NO&lt;sub&gt;2 &lt;/sub&gt;and HCHO around the measurement site. The observations show a clear seasonal cycle of these trace gases. An important application of the dual-scan MAX-DOAS measurements is the validation of satellite missions with high spatial resolution, such as TROPOMI/S5P. Measuring the tropospheric &amp;#160;VCDs in different azimuthal directions is shown to improve the spatial colocation with satellite measurements leading to a better agreement between both datasets. By using &amp;#160;vertical profile information derived from the MAX-DOAS measurements, we show that a persistent systematic underestimation of the TROPOMI &amp;#160;data can be explained by uncertainties in the a-priori NO&lt;sub&gt;2&lt;/sub&gt; profile shape in the satellite retrieval. A similar validation study for TROPOMI HCHO is currently under progress and preliminary results will be presented.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;References:&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;Sinreich, R., Merten, A., Molina, L., and Volkamer, R.: Parameterizing radiative transfer to convert MAX-DOAS dSCDs into near-surface box-averaged mixing ratios, Atmos. Meas. Tech., 6, 1521&amp;#8211;1532, https://doi.org/10.5194/amt-6-1521-2013, 2013.&lt;/p&gt;


2016 ◽  
Author(s):  
X. L. Yan ◽  
J. S. Wright ◽  
X. D. Zheng ◽  
N. Livesey ◽  
H. Vömel ◽  
...  

Abstract. We validate Aura Microwave Limb Sounder (MLS) version 3 (v3) and version 4 (v4) retrievals of summertime temperature, water vapour and ozone in the upper troposphere and lower–middle stratosphere (UTLS; 10–316 hPa) against balloon soundings collected during the Study of Ozone, Aerosols and Radiation over the Tibetan Plateau (SOAR-TP). Mean v3 and v4 profiles of temperature, water vapour and ozone in this region during the measurement campaigns are almost identical through most of the stratosphere (10–68 hPa), but differ in several respects in the upper troposphere and tropopause layer. Differences in v4 relative to v3 include slightly colder mean temperatures from 100–316 hPa, smaller mean water vapour mixing ratios in the upper troposphere (215–316 hPa), and a more vertically homogeneous profile of mean ozone mixing ratios below the climatological tropopause (100–316 hPa). These changes substantially improve agreement between ozonesondes and MLS ozone retrievals in the upper troposphere, but slightly worsen existing cold and dry biases in the upper troposphere. Aura MLS v3 and v4 temperature profiles contain significant cold biases relative to collocated temperature measurements in several layers of the lower–middle stratosphere (mean biases of −1.3 to −1.8 K centered at 10–12 hPa, 26–32 hPa and 68– 83 hPa) and in the upper troposphere (mean biases of approximately −2.3±0.3 K in v3 and −2.6±0.4 K in v4 between 147 and 261 hPa). MLS v3 and v4 profiles of water vapour volume mixing ratio generally compare well with collocated measurements, with a slight dry bias (v4: −8±4%) near 22–26 hPa, a slight wet bias (v4: +12±5%) near 68–83 hPa, and a more substantial dry bias (v4: −32±11%) in the upper troposphere (121–261 hPa). MLS v3 and v4 retrievals of ozone volume mixing ratio are biased high relative to collocated ozonesondes through most of the stratosphere (18–83 hPa), but are biased low at 100 hPa. The largest positive biases in ozone retrievals are located at 83 hPa (approximately +70%); this peak was not identified by earlier validations and may be regionally or seasonally specific. Ozone retrievals are substantially improved in v4 relative to v3, with smaller biases in the tropopause layer, reduced variance below 68 hPa, larger data yields, and smoother gradients in the vertical profile of ozone biases in the upper troposphere.


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