MAX-DOAS measurements and satellite validation of tropospheric NO2 and SO2 vertical column densities at a rural site of North China

Abstract North China (NC), namely Huabei in Chinese, is one of the most severely polluted regions in China, and the air pollution issues in this region have received a worldwide attention. We performed ground-based Multi Axis Differential Absorption Spectroscopy (MAX-DOAS) measurements at Gucheng, (39°08′N, 115°40′E), a rural site of North China about 110 km southwest of Beijing, from September 2008 to September 2010. The tropospheric vertical column densities (VCDs) of NO2 and SO2 were retrieved using the so-called geometric approximation. The results show that the tropospheric NO2 and SO2 VCDs over NC have nearly the same seasonal variation pattern, with the maximum in winter and minimum in summer, while their diurnal variations are different. We also compared the tropospheric NO2 and SO2 VCDs from our MAX-DOAS measurements with several products of corresponding OMI (Ozone Monitoring Instrument) satellite observations. While in summer good agreement is found, the satellite observations systematically underestimate the tropospheric NO2 in winter over the polluted rural area of NC, probably mostly due to the so called aerosol shielding effect. In contrast, for SO2 no such clear conclusion can be drawn, probably owing to the larger uncertainties from MAX-DOAS and in particular satellite retrievals. This indicates that improvements of the retrieval algorithm for MAX-DOAS and off-line corrections of satellite measurements for the tropospheric SO2 VCDs should be given more emphasis in the future.

[1]  Nicolas Theys,et al.  Evaluation of tropospheric SO 2 retrieved from MAX-DOAS measurements in Xianghe, China , 2014 .

[2]  K. F. Boersma,et al.  Near-real time retrieval of tropospheric NO 2 from OMI , 2006 .

[3]  R. Draxler NOAA Technical Memorandum ERL ARL-224 DESCRIPTION OF THE HYSPLIT_4 MODELING SYSTEM , 1999 .

[4]  H. Tanimoto,et al.  Validation of OMI tropospheric NO 2 column data using MAX-DOAS measurements deep inside the North China Plain in June 2006 , 2008 .

[5]  Steffen Beirle,et al.  Inversion of tropospheric profiles of aerosol extinction and HCHO and NO 2 mixing ratios from MAX-DOAS observations in Milano during the summer of 2003 and comparison with independent data sets , 2011 .

[6]  U. Platt,et al.  Differential Absorption Spectroscopy , 2008 .

[7]  Steffen Beirle,et al.  Weekly cycle of NO 2 by GOME measurements: a signature of anthropogenic sources , 2003 .

[8]  K. Boersma,et al.  Key chemical NOx sink uncertainties and how they influence top-down emissions of nitrogen oxides , 2013 .

[9]  Henk Eskes,et al.  Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space , 2008 .

[10]  Chunsheng Zhao,et al.  Aircraft study of Mountain Chimney Effect of Beijing, China , 2009 .

[11]  John P. Burrows,et al.  MAX-DOAS measurements of atmospheric trace gases in Ny- ˚ Alesund - Radiative transfer studies and their application , 2004 .

[12]  Henk Eskes,et al.  Detection of the trend and seasonal variation in tropospheric NO2 over China , 2006 .

[13]  Kebin He,et al.  Recent large reduction in sulfur dioxide emissions from Chinese power plants observed by the Ozone Monitoring Instrument , 2010 .

[14]  Ann Carine Vandaele,et al.  Measurements of the NO2 absorption cross-section from 42 000 cm−1 to 10 000 cm−1 (238–1000 nm) at 220 K and 294 K , 1998 .

[15]  P. Yan,et al.  Corrigendum to "Tropospheric NO 2 vertical column densities over Beijing: results of the first three years of ground-based MAX-DOAS measurements (2008-2011) and satellite validation" published in Atmos. Chem. Phys., 13, 1547-1567, 2013 , 2013 .

[16]  Michael B. McElroy,et al.  Detection from space of a reduction in anthropogenic emissions of nitrogen oxides during the Chinese economic downturn , 2011 .

[17]  Nicolas Theys,et al.  Sulfur dioxide vertical column DOAS retrievals from the Ozone Monitoring Instrument: Global observations and comparison to ground‐based and satellite data , 2015 .

[18]  F. Hendrick,et al.  Multiple wavelength retrieval of tropospheric aerosol optical properties from MAXDOAS measurements in Beijing , 2010 .

[19]  M. King,et al.  Determination of aerosol optical properties from inverse methods , 2013 .

[20]  J. Lelieveld,et al.  The IPAC-NC field campaign: a pollution and oxidization pool in the lower atmosphere over Huabei, China , 2011 .

[21]  R. L. Curier,et al.  The 2005 and 2006 DANDELIONS NO2 and aerosol intercomparison campaigns , 2008 .

[22]  H. Tanimoto,et al.  Validation of OMI tropospheric NO 2 column data using MAX-DOAS measurements deep inside the North China Plain in June 2006: Mount Tai Experiment 2006 , 2008 .

[23]  J. Burrows,et al.  ATMOSPHERIC REMOTE-SENSING REFERENCE DATA FROM GOME — 2 . TEMPERATURE-DEPENDENT ABSORPTION CROSS SECTIONS OF O 3 IN THE 231 — 794 NM RANGE , 1998 .

[24]  Andreas Hilboll,et al.  Long-term changes of tropospheric NO 2 over megacities derived from multiple satellite instruments , 2012 .

[25]  Min Shao,et al.  MAX-DOAS measurements of NO2, HCHO and CHOCHO at a rural site in Southern China , 2012 .

[26]  Xiaobin Xu,et al.  Characteristics of gaseous pollutants at Gucheng, a rural site southwest of Beijing , 2009 .

[27]  Pinhua Xie,et al.  Observations of tropospheric NO2 using ground based MAX-DOAS and OMI measurements during the Shanghai World Expo 2010 , 2015 .

[28]  F. Hendrick,et al.  Retrieval of stratospheric and tropospheric BrO columns from multi-axis DOAS measurements at Reunion Island (21 S, 56 E) , 2007 .

[29]  Nickolay A. Krotkov,et al.  Airborne MAX‐DOAS measurements over California: Testing the NASA OMI tropospheric NO2 product , 2013 .

[30]  Dietrich Althausen,et al.  Retrieval of Aerosol Profiles using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) , 2003 .

[31]  Klaus Pfeilsticker,et al.  The Monte Carlo atmospheric radiative transfer model McArtim: Introduction and validation of Jacobians and 3D features , 2011 .

[32]  Pieter Valks,et al.  Operational total and tropospheric NO 2 column retrieval for GOME-2 , 2011 .

[33]  M. Blumthaler,et al.  Relationship between the NO2 photolysis frequency and the solar global irradiance , 2009 .

[34]  Steffen Beirle,et al.  Tropospheric NO 2 column densities deduced from zenith-sky DOAS measurements in Shanghai, China, and their application to satellite validation , 2008 .

[35]  B. Doddridge,et al.  Seasonal variations in elemental carbon aerosol, carbon monoxide and sulfur dioxide: Implications for sources , 2001 .

[36]  Brittany McClure,et al.  Validation of SO2 Retrievals from the Ozone Monitoring Instrument over NE China , 2008 .

[37]  R. Martin Satellite remote sensing of surface air quality , 2008 .

[38]  Zhiliang Yao,et al.  NOx emission trends for China, 1995–2004: The view from the ground and the view from space , 2007 .

[39]  Henk Eskes,et al.  An improved tropospheric NO 2 column retrieval algorithm for the Ozone Monitoring Instrument , 2011 .

[40]  Andrea Pozzer,et al.  Interactive comment on “A high-resolution emission inventory of primary pollutants for the Huabei region, China” by B. Zhao et al , 2011 .

[41]  C. Clerbaux,et al.  First simultaneous space measurements of atmospheric pollutants in the boundary layer from IASI: A case study in the North China Plain , 2014 .

[42]  K. Boersma,et al.  Trends, seasonal variability and dominant NOx source derived from a ten year record of NO2 measured from space , 2008 .

[43]  James B. Burkholder,et al.  Absorption measurements of oxygen between 330 and 1140 nm , 1990 .

[44]  A. Vandaele,et al.  SO2 Absorption Cross-section Measurement in the UV using a Fourier Transform Spectrometer , 1994 .

[45]  Y. Cohen,et al.  Atmospheric hydrogen peroxide: Does it share a role with ozone in degrading air quality , 1990 .

[46]  John P. Burrows,et al.  On the improvement of NO 2 satellite retrievals – aerosol impact on the airmass factors , 2009 .

[47]  Anne M. Thompson,et al.  Aircraft vertical profiles of trace gas and aerosol pollution over the mid‐Atlantic United States: Statistics and meteorological cluster analysis , 2006 .

[48]  Ulrich Platt,et al.  MAX‐DOAS O4 measurements: A new technique to derive information on atmospheric aerosols—Principles and information content , 2004 .

[49]  R. Martin,et al.  Growth in NO x emissions from power plants in China: bottom-up estimates and satellite observations , 2012 .

[50]  R. Martin,et al.  Retrieving tropospheric nitrogen dioxide from the Ozone Monitoring Instrument: effects of aerosols, surface reflectance anisotropy, and vertical profile of nitrogen dioxide , 2013 .

[51]  Piet Stammes,et al.  Retrieval of tropospheric NO 2 using the MAX-DOAS method combined with relative intensity measurements for aerosol correction , 2010 .

[52]  R. Draxler An Overview of the HYSPLIT_4 Modelling System for Trajectories, Dispersion, and Deposition , 1998 .

[53]  J. Veefkind,et al.  Validation of Ozone Monitoring Instrument nitrogen dioxide columns , 2008 .

[54]  J. Burrows,et al.  Increase in tropospheric nitrogen dioxide over China observed from space , 2005, Nature.

[55]  Heikki Saari,et al.  The ozone monitoring instrument , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[56]  Olga Pikelnaya,et al.  Intercomparison of multiaxis and long-path differential optical absorption spectroscopy measurements in the marine boundary layer , 2007 .

[57]  Steffen Beirle,et al.  Megacity Emissions and Lifetimes of Nitrogen Oxides Probed from Space , 2011, Science.

[58]  Johannes Orphal,et al.  ATMOSPHERIC REMOTE-SENSING REFERENCE DATA FROM GOME: PART 1. TEMPERATURE-DEPENDENT ABSORPTION CROSS-SECTIONS OF NO2 IN THE 231–794 nm RANGE , 1998 .

[59]  Zheng Fang-cheng,et al.  Inventory of atmospheric pollutants discharged from biomass burning in China continent , 2005 .

[60]  J. Burrows,et al.  Comparison of model-simulated tropospheric NO2 over China with GOME-satellite data , 2006 .

[61]  Can Li,et al.  A fast and sensitive new satellite SO2 retrieval algorithm based on principal component analysis: Application to the ozone monitoring instrument , 2013 .

[62]  R. Martin,et al.  Application of OMI, SCIAMACHY, and GOME‐2 satellite SO2 retrievals for detection of large emission sources , 2013 .

[63]  Christian Hermans,et al.  Four years of ground-based MAX-DOAS observations of HONO and NO 2 in the Beijing area , 2012 .

[64]  U. Platt,et al.  Ground‐based measurements of halogen oxides at the Hudson Bay by active longpath DOAS and passive MAX‐DOAS , 2004 .

[65]  James F. Gleason,et al.  A new stratospheric and tropospheric NO2 retrieval algorithm for nadir-viewing satellite instruments : applications to OMI , 2013 .

[66]  Y. Wang,et al.  Characteristics and recent trends of sulfur dioxide at urban, rural, and background sites in north China: effectiveness of control measures. , 2012, Journal of environmental sciences.

[67]  Ulrich Platt,et al.  Determination of aerosol properties from MAX-DOAS observations of the Ring effect , 2009 .

[68]  Geert K. Moortgat,et al.  Temperature dependence of the absorption cross sections of formaldehyde between 223 and 323 K in the wavelength range 225–375 nm , 2000 .

[69]  J. Burrows,et al.  The remote sensing of tropospheric composition from space , 2011 .

[70]  Steffen Beirle,et al.  Estimation of NO x emissions from Delhi using Car MAX-DOAS observations and comparison with OMI satellite data , 2011 .

[71]  Stefan Kraus,et al.  DOASIS: a framework design for DOAS , 2006 .

[72]  Ingemar Furenlid,et al.  Solar flux atlas from 296 to 1300 nm , 1985 .

[73]  Nickolay A. Krotkov,et al.  SO2 emissions and lifetimes: Estimates from inverse modeling using in situ and global, space‐based (SCIAMACHY and OMI) observations , 2011 .