scholarly journals Long-term MAX-DOAS network observations of NO<sub>2</sub> in Russia and Asia (MADRAS) during the period 2007–2012: instrumentation, elucidation of climatology, and comparisons with OMI satellite observations and global model simulations

2014 ◽  
Vol 14 (15) ◽  
pp. 7909-7927 ◽  
Author(s):  
Y. Kanaya ◽  
H. Irie ◽  
H. Takashima ◽  
H. Iwabuchi ◽  
H. Akimoto ◽  
...  

Abstract. We conducted long-term network observations using standardized Multi-Axis Differential optical absorption spectroscopy (MAX-DOAS) instruments in Russia and ASia (MADRAS) from 2007 onwards and made the first synthetic data analysis. At seven locations (Cape Hedo, Fukue and Yokosuka in Japan, Hefei in China, Gwangju in Korea, and Tomsk and Zvenigorod in Russia) with different levels of pollution, we obtained 80 927 retrievals of tropospheric NO2 vertical column density (TropoNO2VCD) and aerosol optical depth (AOD). In the technique, the optimal estimation of the TropoNO2VCD and its profile was performed using aerosol information derived from O4 absorbances simultaneously observed at 460–490 nm. This large data set was used to analyze NO2 climatology systematically, including temporal variations from the seasonal to the diurnal scale. The results were compared with Ozone Monitoring Instrument (OMI) satellite observations and global model simulations. Two NO2 retrievals of OMI satellite data (NASA ver. 2.1 and Dutch OMI NO2 (DOMINO) ver. 2.0) generally showed close correlations with those derived from MAX-DOAS observations, but had low biases of up to ~50%. The bias was distinct when NO2 was abundantly present near the surface and when the AOD was high, suggesting a possibility of incomplete accounting of NO2 near the surface under relatively high aerosol conditions for the satellite observations. Except for constant biases, the satellite observations showed nearly perfect seasonal agreement with MAX-DOAS observations, suggesting that the analysis of seasonal features of the satellite data were robust. Weekend reduction in the TropoNO2VCD found at Yokosuka and Gwangju was absent at Hefei, implying that the major sources had different weekly variation patterns. While the TropoNO2VCD generally decreased during the midday hours, it increased exceptionally at urban/suburban locations (Yokosuka, Gwangju, and Hefei) during winter. A global chemical transport model, MIROC-ESM-CHEM (Model for Interdisciplinary Research on Climate–Earth System Model–Chemistry), was validated for the first time with respect to background NO2 column densities during summer at Cape Hedo and Fukue in the clean marine atmosphere.

2014 ◽  
Vol 14 (2) ◽  
pp. 2883-2934 ◽  
Author(s):  
Y. Kanaya ◽  
H. Irie ◽  
H. Takashima ◽  
H. Iwabuchi ◽  
H. Akimoto ◽  
...  

Abstract. We conducted long-term network observations using standardized Multi-Axis Differential optical absorption spectroscopy (MAX-DOAS) instruments in Russia and ASia (MADRAS) from 2007 onwards. At seven locations (Cape Hedo, Fukue, and Yokosuka in Japan, Hefei in China, Gwangju in Korea, and Tomsk and Zvenigorod in Russia) with different levels of pollution, we obtained 80 927 retrievals of tropospheric NO2 vertical column density (TropoNO2VCD) and aerosol optical depth (AOD). In the technique, the optimal estimation of the TropoNO2VCD and its profile was performed using aerosol information derived from O4 absorbances simultaneously observed at 460–490 nm. This large data set was used to analyze NO2 climatology systematically, including temporal variations from the seasonal to the diurnal scale. The results were compared with Ozone Monitoring Instrument (OMI) satellite observations and global model simulations. Two NO2 retrievals of OMI satellite data (NASA ver. 2.1 and Dutch OMI NO2 (DOMINO) ver. 2.0) generally showed close correlations with those derived from MAX-DOAS observations, but had low biases of ~50%. The bias was distinct when NO2 was abundantly present near the surface and when the AOD was high, suggesting that the aerosol shielding effect could be important, especially for clean sites where the difference could not be attributed to the spatial inhomogeneity. Except for constant biases, the satellite observations showed nearly perfect seasonal agreement with MAX-DOAS observations, suggesting that the analysis of seasonal features of the satellite data were robust. The prevailing seasonal patterns with a wintertime maximum implied the dominance of anthropogenic emissions around our sites. The presence of weekend reductions at Yokosuka and Gwangju suggested the dominance of emissions from diesel vehicles, with significant weekly cycles, whereas the absence of such a reduction at Hefei suggested the importance of other sources. A global chemical transport model, MIROC-ESM-CHEM, was validated for the first time with respect to background NO2 column densities during summer at Cape Hedo and Fukue in the clean marine atmosphere.


2015 ◽  
Vol 8 (3) ◽  
pp. 2437-2500
Author(s):  
R. Shaiganfar ◽  
S. Beirle ◽  
H. Petetin ◽  
Q. Zhang ◽  
M. Beekmann ◽  
...  

Abstract. We compare tropospheric column densities (vertically integrated concentrations) of NO2 from three data sets for the metropolitan area of Paris during two extensive measurement campaigns (25 days in summer 2009 and 29 days in winter 2010) within the European research project MEGAPOLI. The selected data sets comprise a regional chemical transport model (CHIMERE) as well as two observational data sets: ground based mobile Multi-AXis-Differential Optical Absorption Spectroscopy (car-MAX-DOAS) measurements and satellite measurements from the Ozone Monitoring Instrument (OMI). On most days, car-MAX-DOAS measurements were carried out along large circles (diameter ~35 km) around Paris. The car-MAX-DOAS results are compared to coincident data from CHIMERE and OMI. All three data sets have their specific strengths and weaknesses, especially with respect to their spatio-temporal resolution and coverage as well as their uncertainties. Thus we compare them in two different ways: first, we simply consider the original data sets. Second, we compare modified versions making synergistic use of the complementary information from different data sets. For example, profile information from the regional model is used to improve the satellite data, observations of the horizontal trace gas distribution are used to adjust the respective spatial patterns of the model simulations, or the model is used as a transfer tool to bridge the spatial scales between car-MAX-DOAS and satellite observations. Using the modified versions of the data sets, the comparison results substantially improve compared to the original versions. In general, good agreement between the data sets is found outside the emission plume, but inside the emission plumes the tropospheric NO2 VCDs are systematically underestimated by the CHIMERE model and the satellite observations (compared to the car-MAX-DOAS observations). One major result from our study is that for satellite validation close to strong emission sources (like power plants or megacities) detailed information about the intra-pixel heterogeneity is essential. Such information may be gained from simultaneous car-MAX-DOAS measurements using multiple instruments or by combining (car-) MAX-DOAS measurements with results from regional model simulations.


2021 ◽  
Author(s):  
Jianfeng Li ◽  
Yuhang Wang ◽  
Ruixiong Zhang ◽  
Charles Smeltzer ◽  
Andrew Weinheimer ◽  
...  

Abstract. Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations of NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements, surface EPA Air Quality System (AQS) observations, as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; and GOME-2A: Global Ozone Monitoring Experiment – 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument, in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region. The model simulations at 36- and 4-km resolutions are in reasonably good agreement with the temporospatial NO2 observations in the daytime. However, nighttime mixing in the model needs to be enhanced to reproduce the observed NO2 diurnal cycle in the model. Another discrepancy is that Pandora measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. Relative to the 36-km model simulations, the 4-km model results show larger biases compared to the observations due largely to the larger spatial variations of NO2 in the model when the spatial resolution is increased from 36 to 4 km, although the biases are often comparable to the ranges of the observations. The high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than 4-km model simulations, reflecting likely the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011 at high resolution.


2021 ◽  
Vol 21 (14) ◽  
pp. 11133-11160
Author(s):  
Jianfeng Li ◽  
Yuhang Wang ◽  
Ruixiong Zhang ◽  
Charles Smeltzer ◽  
Andrew Weinheimer ◽  
...  

Abstract. Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment – 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore–Washington region. The model simulations at 36 and 4 km resolutions are in reasonably good agreement with the regional mean temporospatial NO2 observations in the daytime. However, we find significant overestimations (underestimations) of model-simulated NO2 (O3) surface concentrations during nighttime, which can be mitigated by enhancing nocturnal vertical mixing in the model. Another discrepancy is that Pandora-measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. The higher-resolution 4 km simulations tend to show larger biases compared to the observations due largely to the larger spatial variations in NOx emissions in the model when the model spatial resolution is increased from 36 to 4 km. OMI, GOME-2A, and the high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than corresponding 36 and 4 km model simulations, likely reflecting the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011.


2011 ◽  
Vol 4 (6) ◽  
pp. 6615-6642
Author(s):  
K. L. Chan ◽  
D. Pöhler ◽  
G. Kuhlmann ◽  
A. Hartl ◽  
U. Platt ◽  
...  

Abstract. In this study we present the first long term measurements of atmospheric nitrogen dioxide (NO2) using a LED based Long Path Differential Optical Absorption Spectroscopy (LP-DOAS) instrument. This instrument is measuring continuously in Hong Kong since December 2009, first in a setup with a 550 m absorption path and then with a 3820 m path at about 30 m to 50 m above street level. The instrument is using a high power blue light LED with peak intensity at 450 nm coupled into the telescope using a Y-fibre bundle. The LP-DOAS instrument measures NO2 concentrations in the Kowloon Tong and Mong Kok district of Hong Kong and we compare the measurement results to concentrations reported by monitoring stations operated by the Hong Kong Environmental Protection Department in that area. Hourly averages of coinciding measurements are in reasonable agreement (R = 0.74). Furthermore, we used the long-term data set to validate the Ozone Monitoring Instrument (OMI) NO2 data product. Monthly averaged LP-DOAS and OMI measurements correlate well (R = 0.84) when comparing the data for the OMI overpass time. We analyzed weekly patterns in both data sets and found that the LP-DOAS detects a clear weekly cycle with a reduction on weekends during rush hour peaks, whereas OMI is not able to observe this weekly cycle due to its fix overpass time.


2016 ◽  
Author(s):  
Yang Wang ◽  
Steffen Beirle ◽  
Johannes lampel ◽  
Mariliza Koukouli ◽  
Isabelle De Smedt ◽  
...  

Abstract. Tropospheric vertical column densities (VCDs) of NO2, SO2 and HCHO derived from Ozone Monitoring Instrument (OMI) on AURA and Global Ozone Monitoring Experiment 2 aboard METOP-A (GOME-2A) and METOP-B (GOME-2B) are widely used to characterize the global distributions, trends, dominating sources of the trace gases and for comparisons with chemical transport models (CTM). We use tropospheric VCDs and vertical profiles of NO2, SO2 and HCHO derived from MAX-DOAS measurements from 2011 to 2014 in Wuxi, China, to validate the corresponding products derived from OMI, GOME-2A/B by different scientific teams (daily and bimonthly averaged data). Prior to the comparison we investigate the effects of the spatial and temporal coincidence criteria for MAX-DOAS and satellite data on the comparison results. We find that the distance of satellite data from the location of the MAX-DOAS station is the dominating effect, and we make suggestions for the spatial (20 km for OMI NO2 and SO2 products and 50 km for OMI HCHO and all GOME-2A/B products) and temporal averaging (2 hours around satellite overpass time). We also investigate the effect of clouds on both MAX-DOAS and satellite observations. Our results indicate that the discrepancies between satellite and MAX-DOAS results increase with increasing effective cloud fractions and are dominated by the cloud effect on the satellite products. Our comparison results indicate a systematic underestimation of all SO2 (40 % to 57 %) and HCHO products (about 20 %) and an overestimation of the GOME-2A/B NO2 products (about 30 %) (DOMINO NO2 product is only slightly underestimated by 1 %). To better understand the reasons for the differences, we recalculated the AMFs for satellite observations based on the shape factors (SFs) derived from MAX-DOAS. The recalculated satellite VCDs agree better with the MAX-DOAS VCDs than those from the original products by up to 10 %, 47 % and 35 % for NO2, SO2 and HCHO, respectively. The improvement is strongest for periods with large trace gas VCDs. Finally we investigate the effect of aerosols on the satellite retrievals. We find an increasing underestimation of the OMI NO2, SO2 and HCHO products with increasing AOD by up to 8 %, 12 % and 2 %, respectively. One reason for this finding is that aerosols systematically affect the satellite cloud retrievals and can lead to apparent effective cloud fractions of up to 10 % and apparent cloud top pressures of down to 830 hPa for the typical urban region in Wuxi. We show that in such cases the implicit aerosol correction could cause a strong underestimation of tropospheric VCDs by up to about 45 %, 77 % and 100 % for NO2, SO2 and HCHO, respectively. For such conditions it might be better to apply AMFs for clear sky conditions than AMFs based on the satellite cloud retrievals. We find that the satellites systematically overestimate the magnitude of the diurnal variations of NO2 and HCHO. No significant weekly cycle for all trace gases is found by either the satellites or the MAX-DOAS measurements.


2015 ◽  
Vol 8 (7) ◽  
pp. 2827-2852 ◽  
Author(s):  
R. Shaiganfar ◽  
S. Beirle ◽  
H. Petetin ◽  
Q. Zhang ◽  
M. Beekmann ◽  
...  

Abstract. We compare tropospheric column densities (vertically integrated concentrations) of NO2 from three data sets for the metropolitan area of Paris during two extensive measurement campaigns (25 days in summer 2009 and 29 days in winter 2010) within the European research project MEGAPOLI. The selected data sets comprise a regional chemical transport model (CHIMERE) as well as two observational data sets: ground-based mobile Multi-AXis-Differential Optical Absorption Spectroscopy (car-MAX-DOAS) measurements and satellite measurements from the Ozone Monitoring Instrument (OMI). On most days, car-MAX-DOAS measurements were carried out along large circles (diameter ~ 35 km) around Paris. The car-MAX-DOAS results are compared to coincident data from CHIMERE and OMI. All three data sets have their specific strengths and weaknesses, especially with respect to their spatiotemporal resolution and coverage as well as their uncertainties. Thus we compare them in two different ways: first, we simply consider the original data sets. Second, we compare modified versions making synergistic use of the complementary information from different data sets. For example, profile information from the regional model is used to improve the satellite data, observations of the horizontal trace gas distribution are used to adjust the respective spatial patterns of the model simulations, or the model is used as a transfer tool to bridge the spatial scales between car-MAX-DOAS and satellite observations. Using the modified versions of the data sets, the comparison results substantially improve compared to the original versions. In general, good agreement between the data sets is found outside the emission plume, but inside the emission plumes the tropospheric NO2 vertical column densities (VCDs). are systematically underestimated by the CHIMERE model and the satellite observations (compared to the car-MAX-DOAS observations). One major result from our study is that for satellite validation close to strong emission sources (like power plants or megacities), detailed information about the intra-pixel heterogeneity is essential. Such information may be gained from simultaneous car-MAX-DOAS measurements using multiple instruments or by combining (car-) MAX-DOAS measurements with results from regional model simulations.


2012 ◽  
Vol 5 (5) ◽  
pp. 901-912 ◽  
Author(s):  
K. L. Chan ◽  
D. Pöhler ◽  
G. Kuhlmann ◽  
A. Hartl ◽  
U. Platt ◽  
...  

Abstract. In this study we present the first long term measurements of atmospheric nitrogen dioxide (NO2) using a LED based Long Path Differential Optical Absorption Spectroscopy (LP-DOAS) instrument. This instrument is measuring continuously in Hong Kong since December 2009, first in a setup with a 550 m absorption path and then with a 3820 m path at about 30 m to 50 m above street level. The instrument is using a high power blue light LED with peak intensity at 450 nm coupled into the telescope using a Y-fibre bundle. The LP-DOAS instrument measures NO2 levels in the Kowloon Tong and Mongkok district of Hong Kong and we compare the measurement results to mixing ratios reported by monitoring stations operated by the Hong Kong Environmental Protection Department in that area. Hourly averages of coinciding measurements are in reasonable agreement (R = 0.74). Furthermore, we used the long-term data set to validate the Ozone Monitoring Instrument (OMI) NO2 data product. Monthly averaged LP-DOAS and OMI measurements correlate well (R = 0.84) when comparing the data for the OMI overpass time. We analyzed weekly patterns in both data sets and found that the LP-DOAS detects a clear weekly cycle with a reduction on weekends during rush hour peaks, whereas OMI is not able to observe this weekly cycle due to its fix overpass time (13:30–14:30 LT – local time).


2008 ◽  
Vol 8 (5) ◽  
pp. 17393-17422 ◽  
Author(s):  
M. F. Khokhar ◽  
U. Platt ◽  
T. Wagner

Abstract. We report on satellite observations of atmospheric Sulfur Dioxide (SO2) emitted from metal smelting industries in Peru, South America and Siberia, Russia. Most of the non-ferrous metal ores are sulfidic and during the smelting process the sulfur is emitted as SO2. In addition to Norilsk, Russia, Peruvian copper smelters are among the most polluting point sources in the world. We retrieve SO2 column amounts from spectra of the Global Ozone Monitoring Experiment (GOME) on the Earth Research Satellite 2 (ERS-2) for the years 1996 to 2002 using an algorithm based on differential Optical Absorption Spectroscopy (DOAS). Areas of enhanced SO2 column amounts are clearly identified on a 7-years mean map of GOME observations over the regions with La Oroya and Ilo copper smelters of Peru and Norilsk smelters of Russia. Since the instrument sensitivity is highly dependent on surface albedo, SO2 vertical profile, solar zenith angle (SZA), wavelength, clouds, and aerosol, radiative transfer modelling is used to convert the analysed slant column densities into vertical column densities. In this study, the full spherical Monte-Carlo radiative transport model TRACY-II is used for SO2 AMF calculation. GOME data is analysed in further detail by calculating time series over these regions. For the different locations, the results demonstrate both, increasing and decreasing trends in the SO2 column amounts over the time period of 1996–2002. The decreasing trend for the Ilo copper smelter is in good agreement with implemented measures for emission reductions. However, even for the cases with decreasing trends, these point sources are still a dominant source of anthropogenic SO2 emissions in their region. For the smelters in Peru, the potential influence due to SO2 emission by the nearby volcanoes is investigated and found to be negligible.


2009 ◽  
Vol 9 (11) ◽  
pp. 3641-3662 ◽  
Author(s):  
D. Chen ◽  
B. Zhou ◽  
S. Beirle ◽  
L. M. Chen ◽  
T. Wagner

Abstract. Zenith-sky scattered sunlight observations using differential optical absorption spectroscopy (DOAS) technique were carried out in Shanghai, China (31.3° N, 121.5° E) since December 2006. At this polluted urban site, the measurements provided NO2 total columns in the daytime. Here, we present a new method to extract time series of tropospheric vertical column densities (VCDs) of NO2 from these observations. The derived tropospheric NO2 VCDs are important quantities for the estimation of emissions and for the validation of satellite observations. Our method makes use of assumptions on the relative NO2 height profiles and the diurnal variation of stratospheric NO2 VCDs. The main error sources arise from the uncertainties in the estimated stratospheric slant column densities (SCDs) and the determination of tropospheric NO2 air mass factor (AMF). For a polluted site like Shanghai, the accuracy of our method is conservatively estimated to be <25% for solar zenith angle (SZA) lower than 70°. From simultaneously performed long-path DOAS measurements, the NO2 surface concentrations at the same site were observed and the corresponding tropospheric NO2 VCDs were estimated using the assumed seasonal NO2 profiles in the planetary boundary layer (PBL). By making a comparison between the tropospheric NO2 VCDs from zenith-sky and long-path DOAS measurements, it is found that the former provides more realistic information about total tropospheric pollution than the latter, so it's more suitable for satellite data validation. A comparison between the tropospheric NO2 VCDs from ground-based zenith-sky measurements and SCIAMACHY was also made. Satellite validation for a strongly polluted area is highly needed, but exhibits also a great challenge. Our comparison shows good agreement, considering in particular the different spatial resolutions between the two measurements. Remaining systematic deviations are most probably related to the uncertainties of satellite data caused by the assumptions on aerosol properties as well as the layer heights of aerosols and NO2.


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