scholarly journals Deriving tropospheric ozone from assimilated profiles

2019 ◽  
Vol 19 (12) ◽  
pp. 8297-8309
Author(s):  
Jacob C. A. van Peet ◽  
Ronald J. van der A

Abstract. We derived global tropospheric ozone (O3) columns from GOME-2A (Global Ozone Monitoring Experiment) and OMI (Ozone Monitoring Instrument) O3 profiles, which were simultaneously assimilated into the TM5 (Tracer Model, version 5) global chemistry transport model for the year 2008. The horizontal model resolution has been increased by a factor of 6 for more accurate results. To reduce computational cost, the number of model layers has been reduced from 44 to 31. The model ozone fields are used to derive tropospheric ozone, which is defined here as the partial column between mean sea level and 6 km altitude. Two methods for calculating the tropospheric columns from the free model run and assimilated O3 fields are compared. In the first method, we calculate the residual between assimilated total columns and the partial model column between 6 km and the top of atmosphere. In the second method, we perform a direct integration of the assimilated O3 fields between the surface and 6 km. The results are validated against tropospheric columns derived from ozone sonde measurements. Our results show that the residual method has too large a variation to be used reliably for the determination of tropospheric ozone, so the direct integration method has been used instead. The median global bias is smaller for the assimilated O3 fields than for the free model run, but the large variation makes it difficult to make definitive statements on a regional or local scale. The monthly mean ozone fields show significant improvements and more detail when comparing the assimilated O3 fields with the free model run, especially for features such as biomass-burning-enhanced O3 concentrations and outflow of O3 rich air from Asia over the Pacific.

2019 ◽  
Author(s):  
Jacob C. A. van Peet ◽  
Ronald J. van der A

Abstract. To derive global tropospheric O3 columns from satellite observations, O3 profiles retrieved from GOME-2A and OMI measurements were simultaneously assimilated into the TM5 global chemistry transport model for the year 2008. The horizontal model resolution has been increased by a factor of 6 for more accurate results, but to reduce computational cost, the number of model layers has been reduced from 44 to 31. The model ozone fields are used to derive tropospheric ozone, which is defined here as the partial column between mean sea level and 6 km altitude. Two methods for calculating the tropospheric columns from the free model run and assimilate O3 fields are compared. In the first method, we calculate the residual between assimilated total columns and the partial model column between 6 km and the top of atmosphere. In the second method, we perform a direct integration of the assimilated O3 fields between the surface and 6 km. The results are validated against tropospheric columns derived from ozone sonde measurements. It turned out that the residual method has a too large variation to be used reliably for the determination of tropospheric ozone, so the direct integration method has been used instead. The median global bias is smaller for the assimilated O3 fields than for the free model run, but the large variation makes it difficult to make definitive statements on a regional or local scale. The monthly mean ozone fields show significant improvements and more detail when comparing the assimilated O3 fields with the free model run, especially for features such as biomass burning enhanced O3 concentrations and outflow of O3 rich air from Asia over the Pacific.


2018 ◽  
Author(s):  
Dejian Fu ◽  
Susan S. Kulawik ◽  
Kazuyuki Miyazaki ◽  
Kevin W. Bowman ◽  
John R. Worden ◽  
...  

Abstract. The Tropospheric Emission Spectrometer (TES) on the A-Train Aura satellite was designed to profile tropospheric ozone and its precursors, taking measurements from 2004 to 2018. Starting in 2008, TES global sampling of tropospheric ozone was gradually reduced in latitude with global coverage stopping in 2011. To extend the record of TES, this work presents a multispectral approach that will provide O3 data products with vertical resolution and measurement uncertainty similar to TES by combining the single-footprint thermal infrared (TIR) hyperspectral radiances from the Aqua Atmospheric Infrared Sounder (AIRS) instrument and the ultraviolet (UV) channels from the Aura Ozone Monitoring Instrument (OMI). The joint AIR+OMI O3 retrievals are processed through the MUlti-SpEctra, MUlti-SpEcies, MUlti-SEnsors (MUSES) retrieval algorithm. Comparisons of collocated joint AIRS+OMI and TES to ozonesonde measurements show that both systems have similar errors, with mean and standard deviation of the differences well within the estimated measurement uncertainty. AIRS+OMI and TES have slightly different biases (within 5 parts per billion) versus the sondes. Both AIRS and OMI have wide swath widths (~ 1,650 km for AIRS; ~ 2,600 km for OMI) across satellite ground tracks. Consequently, the joint AIRS+OMI measurements have the potential to maintain TES vertical sensitivity while increasing coverage by two orders of magnitude, thus providing an unprecedented new dataset to quantify the evolution of tropospheric ozone.


2011 ◽  
Vol 11 (17) ◽  
pp. 9237-9251 ◽  
Author(s):  
J. R. Ziemke ◽  
S. Chandra ◽  
G. J. Labow ◽  
P. K. Bhartia ◽  
L. Froidevaux ◽  
...  

Abstract. A global climatology of tropospheric and stratospheric column ozone is derived by combining six years of Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) ozone measurements for the period October 2004 through December 2010. The OMI/MLS tropospheric ozone climatology exhibits large temporal and spatial variability which includes ozone accumulation zones in the tropical south Atlantic year-round and in the subtropical Mediterranean/Asia region in summer months. High levels of tropospheric ozone in the Northern Hemisphere also persist in mid-latitudes over the eastern part of the North American continent extending across the Atlantic Ocean and the eastern part of the Asian continent extending across the Pacific Ocean. For stratospheric ozone climatology from MLS, largest column abundance is in the Northern Hemisphere in the latitude range 70° N–80° N in February–April and in the Southern Hemisphere around 40° S–50° S during August–October. Largest stratospheric ozone lies in the Northern Hemisphere and extends from the eastern Asian continent eastward across the Pacific Ocean and North America. With the advent of many newly developing 3-D chemistry and transport models it is advantageous to have such a dataset for evaluating the performance of the models in relation to dynamical and photochemical processes controlling the ozone distributions in the troposphere and stratosphere. The OMI/MLS gridded ozone climatology data are made available to the science community via the NASA Goddard Space Flight Center ozone and air quality website http://ozoneaq.gsfc.nasa.gov/.


2013 ◽  
Vol 13 (4) ◽  
pp. 8901-8937 ◽  
Author(s):  
P. S. Kim ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. X. Warner ◽  
K. Yang ◽  
...  

Abstract. We present a global data set of free tropospheric ozone–CO correlations with 2° × 2.5° spatial resolution from the Ozone Monitoring Instrument (OMI) and Atmospheric Infrared Sounder (AIRS) satellite instruments for each season of 2008. OMI and AIRS have near daily global coverage of ozone and CO respectively and observe coincident scenes with similar vertical sensitivities. The resulting ozone–CO correlations are highly statistically significant (positive or negative) in most regions of the world, and are less noisy than previous satellite-based studies that used sparser data. We interpret the observed ozone–CO correlations with the GEOS-Chem chemical transport model to infer constraints on ozone sources. Driving GEOS-Chem with different meteorological fields generally shows consistent ozone–CO correlation patterns, except in some tropical regions where the correlations are strongly sensitive to model transport error associated with deep convection. GEOS-Chem reproduces the general structure of the observed ozone–CO correlations and regression slopes (dO3/dCO), although there are some large regional discrepancies. We examine the model sensitivity of dO3/dCO to different ozone sources (combustion, biosphere, stratosphere, and lightning NOx) by correlating the ozone change from that source to CO from the standard simulation. The model reproduces the observed positive dO3/dCO in the extratropical Northern Hemisphere in spring–summer, driven by combustion sources. Stratospheric influence there is also associated with a positive dO3/dCO because of the interweaving of stratospheric downwelling with continental outflow. The well-known ozone maximum over the tropical South Atlantic is associated with negative dO3/dCO in the observations; this feature is reproduced in GEOS-Chem and supports a dominant contribution from lightning to the ozone maximum. A~major model discrepancy is found over the Northeast Pacific in summer-fall where dO3/dCO is positive in the observations but negative in the model, for all ozone sources. We suggest that this reflects a model overestimate of lightning at northern mid-latitudes combined with an underestimate of the East Asian CO source.


2013 ◽  
Vol 13 (8) ◽  
pp. 21455-21505
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.


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.


2018 ◽  
Vol 184 ◽  
pp. 244-253 ◽  
Author(s):  
Sachiko Hayashida ◽  
Mizuo Kajino ◽  
Makoto Deushi ◽  
Tsuyoshi Thomas Sekiyama ◽  
Xiong Liu

2017 ◽  
Vol 17 (9) ◽  
pp. 5829-5849 ◽  
Author(s):  
Theano Drosoglou ◽  
Alkiviadis F. Bais ◽  
Irene Zyrichidou ◽  
Natalia Kouremeti ◽  
Anastasia Poupkou ◽  
...  

Abstract. One of the main issues arising from the comparison of ground-based and satellite measurements is the difference in spatial representativeness, which for locations with inhomogeneous spatial distribution of pollutants may lead to significant differences between the two data sets. In order to investigate the spatial variability of tropospheric NO2 within a sub-satellite pixel, a campaign which lasted for about 6 months was held in the greater area of Thessaloniki, Greece. Three multi-axial differential optical absorption spectroscopy (MAX-DOAS) systems performed measurements of tropospheric NO2 columns at different sites representative of urban, suburban and rural conditions. The direct comparison of these ground-based measurements with corresponding products from the Ozone Monitoring Instrument onboard NASA's Aura satellite (OMI/Aura) showed good agreement over the rural and suburban areas, while the comparison with the Global Ozone Monitoring Experiment-2 (GOME-2) onboard EUMETSAT's Meteorological Operational satellites' (MetOp-A and MetOp-B) observations is good only over the rural area. GOME-2A and GOME-2B sensors show an average underestimation of tropospheric NO2 over the urban area of about 10.51 ± 8.32  ×  1015 and 10.21 ± 8.87  × 1015 molecules cm−2, respectively. The mean difference between ground-based and OMI observations is significantly lower (6.60 ± 5.71  ×  1015 molecules cm−2). The differences found in the comparisons of MAX-DOAS data with the different satellite sensors can be attributed to the higher spatial resolution of OMI, as well as the different overpass times and NO2 retrieval algorithms of the satellites. OMI data were adjusted using factors calculated by an air quality modeling tool, consisting of the Weather Research and Forecasting (WRF) mesoscale meteorological model and the Comprehensive Air Quality Model with Extensions (CAMx) multiscale photochemical transport model. This approach resulted in significant improvement of the comparisons over the urban monitoring site. The average difference of OMI observations from MAX-DOAS measurements was reduced to −1.68 ± 5.01  ×  1015 molecules cm−2.


2010 ◽  
Vol 10 (1) ◽  
pp. 1417-1456 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  

Abstract. We analyze three different methods to validate and intercompare satellite measurements of atmospheric composition, and apply them to tropospheric ozone retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI). The first method (in situ method) uses in situ vertical profiles for absolute instrument validation; it is limited by the sparseness of in situ data. The second method (CTM method) uses a chemical transport model (CTM) as an intercomparison platform; it provides a globally complete intercomparison with relatively small noise added by model error. The third method (averaging kernel smoothing method) involves smoothing the retrieved profile from one instrument with the averaging kernel matrix of the other; it also provides a global intercomparison but dampens the actual difference between instruments and adds noise from the a priori. Application to a full year (2006) of TES and OMI data shows mean positive biases of 5.3 parts per billion volume (ppbv) (10%) for TES and 2.8 ppbv (5%) for OMI at 500 hPa relative to in situ data from ozonesondes. We show that the CTM method (using the GEOS-Chem CTM) closely approximates results from the in situ method while providing global coverage. It reveals that differences between TES and OMI are generally less than 10 ppbv (18%), except at northern mid-latitudes in summer and over tropical continents. The CTM method allows for well-constrained CTM evaluation in places where the satellite observations are consistent. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics, reflecting a combination of possible factors, and overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx.


2008 ◽  
Vol 8 (1) ◽  
pp. 1505-1548 ◽  
Author(s):  
K. W. Bowman ◽  
D. Jones ◽  
J. Logan ◽  
H. Worden ◽  
F. Boersma ◽  
...  

Abstract. The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so-called zonal "wave-one" pattern, which is characterized by peak ozone concentrations (70–80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60–70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30–40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.


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