scholarly journals Comprehensive evaluations of diurnal NO<sub>2</sub> measurements during DISCOVER-AQ 2011: Effects of resolution dependent representation of NO<sub>x</sub> emissions

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.


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.


2017 ◽  
Vol 10 (2) ◽  
pp. 721-750 ◽  
Author(s):  
Jason E. Williams ◽  
K. Folkert Boersma ◽  
Phillipe Le Sager ◽  
Willem W. Verstraeten

Abstract. We provide a comprehensive description of the high-resolution version of the TM5-MP global chemistry transport model, which is to be employed for deriving highly resolved vertical profiles of nitrogen dioxide (NO2), formaldehyde (CH2O), and sulfur dioxide (SO2) for use in satellite retrievals from platforms such as the Ozone Monitoring Instrument (OMI) and the Sentinel-5 Precursor, and the TROPOspheric Monitoring Instrument (tropOMI). Comparing simulations conducted at horizontal resolutions of 3°  ×  2° and 1°  ×  1° reveals differences of ±20 % exist in the global seasonal distribution of 222Rn, being larger near specific coastal locations and tropical oceans. For tropospheric ozone (O3), analysis of the chemical budget terms shows that the impact on globally integrated photolysis rates is rather low, in spite of the higher spatial variability of meteorological data fields from ERA-Interim at 1°  ×  1°. Surface concentrations of O3 in high-NOx regions decrease between 5 and 10 % at 1°  ×  1° due to a reduction in NOx recycling terms and an increase in the associated titration term of O3 by NO. At 1°  ×  1°, the net global stratosphere–troposphere exchange of O3 decreases by  ∼  7 %, with an associated shift in the hemispheric gradient. By comparing NO, NO2, HNO3 and peroxy-acetyl-nitrate (PAN) profiles against measurement composites, we show that TM5-MP captures the vertical distribution of NOx and long-lived NOx reservoirs at background locations, again with modest changes at 1°  ×  1°. Comparing monthly mean distributions in lightning NOx and applying ERA-Interim convective mass fluxes, we show that the vertical re-distribution of lightning NOx changes with enhanced release of NOx in the upper troposphere. We show that surface mixing ratios in both NO and NO2 are generally underestimated in both low- and high-NOx scenarios. For Europe, a negative bias exists for [NO] at the surface across the whole domain, with lower biases at 1°  ×  1° at only  ∼  20 % of sites. For NO2, biases are more variable, with lower (higher) biases at 1°  ×  1° occurring at  ∼  35 % ( ∼  20 %) of sites, with the remainder showing little change. For CH2O, the impact of higher resolution on the chemical budget terms is rather modest, with changes of less than 5 %. The simulated vertical distribution of CH2O agrees reasonably well with measurements in pristine locations, although column-integrated values are generally underestimated relative to satellite measurements in polluted regions. For SO2, the performance at 1°  ×  1° is principally governed by the quality of the emission inventory, with limited improvements in the site-specific biases, with most showing no significant improvement. For the vertical column, improvements near strong source regions occur which reduce the biases in the integrated column. For remote regions missing biogenic source terms are inferred.


2017 ◽  
Vol 10 (12) ◽  
pp. 4979-4994
Author(s):  
Germar Bernhard ◽  
Irina Petropavlovskikh ◽  
Bernhard Mayer

Abstract. A new method is presented to determine vertical ozone profiles from measurements of spectral global (direct Sun plus upper hemisphere) irradiance in the ultraviolet. The method is similar to the widely used Umkehr technique, which inverts measurements of zenith sky radiance. The procedure was applied to measurements of a high-resolution spectroradiometer installed near the centre of the Greenland ice sheet. Retrieved profiles were validated with balloon-sonde observations and ozone profiles from the space-borne Microwave Limb Sounder (MLS). Depending on altitude, the bias between retrieval results presented in this paper and MLS observations ranges between −5 and +3 %. The magnitude of this bias is comparable, if not smaller, to values reported in the literature for the standard Dobson Umkehr method. Total ozone columns (TOCs) calculated from the retrieved profiles agree to within 0.7±2.0 % (±1σ) with TOCs measured by the Ozone Monitoring Instrument on board the Aura satellite. The new method is called the Global-Umkehr method.


2011 ◽  
Vol 11 (11) ◽  
pp. 29807-29843 ◽  
Author(s):  
J.-T. Lin

Abstract. Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NOx from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25° long × 0.25° lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN (±38%), 0.22 TgN (±46%), and 0.40 TgN (±48%) for the a posteriori anthropogenic, lightning and soil emissions, respectively, each about 24% higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are each less than 6% of anthropogenic emissions annually, increasing to about 13% for July. Overall, anthropogenic emissions are found to be the dominant source of NOx over East China with important implications for nitrogen control.


Atmosphere ◽  
2020 ◽  
Vol 11 (4) ◽  
pp. 401
Author(s):  
Qing Zhou ◽  
Yong Zhang ◽  
Shuze Jia ◽  
Junli Jin ◽  
Shanshan Lv ◽  
...  

Clouds are significant in the global radiation budget, atmospheric circulation, and hydrological cycle. However, knowledge regarding the observed climatology of the cloud vertical structure (CVS) over Beijing is still poor. Based on high-resolution radiosonde observations at Beijing Nanjiao Weather Observatory (BNWO) during the period 2010–2017, the method for identifying CVS depending on height-resolved relative humidity thresholds is improved, and CVS estimation by radiosonde is compared with observations by millimeter-wave cloud radar and ceilometer at the same site. Good consistency is shown between the three instruments. Then, the CVS climatology, including the frequency distribution and seasonal variation, is investigated. Overall, the occurrence frequency (OF) of cloudy cases in Beijing is slightly higher than that of clear-sky cases, and the cloud OF is highest in summer and lowest in winter. Single-layer clouds and middle-level clouds are dominant in Beijing. In addition, the average cloud top height (CTH), cloud base height (CBH), and cloud thickness in Beijing are 6.2 km, 4.0 km, and 2.2 km, respectively, and show the trend of reaching peaks in spring and minimums in winter. In terms of frequency distribution, the CTH basically resides below an altitude of 16 km, and approximately 43% of the CBHs are located at altitudes of 0.5–1.5 km. The cloud OF has only one peak located at altitudes of 4–8 km in spring, whereas it shows a trimodal distribution in other seasons. The height at which the cloud OF reaches its peak is highest in summer and lowest in winter. To the best of our knowledge, the cloud properties analyzed here are the first to elucidate the distribution and temporal variation of the CVS in Beijing from a long-term sounding perspective, and these results will provide a scientific observation basis for improving the atmospheric circulation model, as well as comparisons and verifications for measurements by ground-based remote sensing equipment.


2019 ◽  
Vol 12 (11) ◽  
pp. 6091-6111 ◽  
Author(s):  
Laura M. Judd ◽  
Jassim A. Al-Saadi ◽  
Scott J. Janz ◽  
Matthew G. Kowalewski ◽  
R. Bradley Pierce ◽  
...  

Abstract. NASA deployed the GeoTASO airborne UV–visible spectrometer in May–June 2017 to produce high-resolution (approximately 250 m×250 m) gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r2=0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and spatial heterogeneity that may be observed differently by the sunward-viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO (Tropospheric Emissions: Monitoring Pollution), TROPOMI (TROPOspheric Monitoring Instrument), and OMI (Ozone Monitoring Instrument), the agreement with Pandora measurements degraded, particularly for the most polluted columns as localized large pollution enhancements observed by Pandora and GeoTASO are spatially averaged with nearby less-polluted locations within the larger area representative of the satellite spatial resolutions (aircraft-to-Pandora slope: TEMPO scale =0.88; TROPOMI scale =0.77; OMI scale =0.57). In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well at least up to pollution scales of 30×1015 molecules cm−2. Two publicly available OMI tropospheric NO2 retrievals are found to be biased low with respect to these Pandora observations. However, the agreement improves when higher-resolution a priori inputs are used for the tropospheric air mass factor calculation (NASA V3 standard product slope =0.18 and Berkeley High Resolution product slope =0.30). Overall, this work explores best practices for satellite validation strategies with Pandora direct-sun observations by showing the sensitivity to product spatial resolution and demonstrating how the high-spatial-resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high-temporal-resolution ground-based column observations to evaluate the influence of spatial heterogeneity on validation results.


2006 ◽  
Vol 44 (5) ◽  
pp. 1245-1258 ◽  
Author(s):  
E.J. Bucsela ◽  
E.A. Celarier ◽  
M.O. Wenig ◽  
J.F. Gleason ◽  
J.P. Veefkind ◽  
...  

2014 ◽  
Vol 14 (19) ◽  
pp. 10565-10588 ◽  
Author(s):  
S. Choi ◽  
J. Joiner ◽  
Y. Choi ◽  
B. N. Duncan ◽  
A. Vasilkov ◽  
...  

Abstract. We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx.


2017 ◽  
Author(s):  
Germar Bernhard ◽  
Irina Petropavlovskikh ◽  
Bernhard Mayer

Abstract. A new method is presented to determine vertical ozone profiles from measurements of spectral global (direct Sun plus upper hemisphere) irradiance in the UV. The method is similar to the widely used Umkehr technique, which inverts measurements of zenith sky radiance. The procedure was applied to measurements of a high-resolution spectroradiometer installed near the centre of the Greenland ice sheet. Retrieved profiles were validated with balloon sonde observations and ozone profiles from the space-borne Microwave Limb Sounder (MLS). Depending on altitude, the bias between retrieval results presented in this paper and MLS observations ranges between −5 % and +3 %. The magnitude of this bias is comparable, if not smaller, to values reported in the literature for the standard Dobson Umkehr method. Total ozone columns (TOCs) calculated from the retrieved profiles agree to within 0.7 ± 2.0 % (±1σ) with TOCs measured by the Ozone Monitoring Instrument (OMI) onboard the Aura satellite. The new method is called the “Global-Umkehr” method.


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