scholarly journals Impact of surface emissions to the zonal variability of tropical tropospheric ozone and carbon monoxide for november 2004

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.

2009 ◽  
Vol 9 (11) ◽  
pp. 3563-3582 ◽  
Author(s):  
K. W. Bowman ◽  
D. B. A. Jones ◽  
J. A. Logan ◽  
H. Worden ◽  
F. Boersma ◽  
...  

Abstract. The impact of surface emissions on the zonal structure of tropical tropospheric ozone and carbon monoxide is investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions.Vertical ozone profiles from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show elevated concentrations of ozone over Indonesia and Australia (60–70 ppb) in the lower troposphere against the backdrop of the well-known zonal "wave-one" pattern with ozone concentrations of (70–80 ppb) centered over the Atlantic . 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., 2009). 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% over Indonesia. The response of the free tropospheric chemical state to the changes in these emissions is investigated for ozone, CO, NOx, and PAN. Model simulations indicate that ozone over Indonesian/Australian is sensitive to regional changes in surface emissions of NOx but relatively insensitive to lightning NOx. Over sub-equatorial Africa and South America, free tropospheric NOx was reduced in response to increased surface emissions potentially muting ozone production.


2015 ◽  
Vol 8 (1) ◽  
pp. 385-398 ◽  
Author(s):  
G. M. Miles ◽  
R. Siddans ◽  
B. J. Kerridge ◽  
B. G. Latter ◽  
N. A. D. Richards

Abstract. This paper describes and assesses the performance of the RAL (Rutherford Appleton Laboratory) ozone profile retrieval scheme for the Global Ozone Monitoring Experiment 2 (GOME-2) with a focus on tropospheric ozone. Developments to the scheme since its application to GOME-1 measurements are outlined. These include the approaches developed to account sufficiently for UV radiometric degradation in the Hartley band and for inadequacies in knowledge of instrumental parameters in the Huggins bands to achieve the high-precision spectral fit required to extract information on tropospheric ozone. The assessment includes a validation against ozonesondes (sondes) sampled worldwide over 2 years (2007–2008). Standard deviations of the ensemble with respect to the sondes are considerably lower for the retrieved profiles than for the a priori, with the exception of the lowest subcolumn. Once retrieval vertical smoothing (averaging kernels) has been applied to the sonde profiles there is a retrieval bias of 6% (1.5 DU) in the lower troposphere, with smaller biases in the subcolumns above. The bias in the troposphere varies with latitude. The retrieval underestimates lower tropospheric ozone in the Southern Hemisphere (SH) (15–20% or ~ 1–3 DU) and overestimates it in the Northern Hemisphere (NH) (10% or 2 DU). The ability of the retrieval to reflect the geographical distribution of lower tropospheric ozone, globally (rather than just ozonesonde launch sites) is demonstrated by comparison with the chemistry transport model TOMCAT. For a monthly mean of cloud-cleared GOME-2 pixels, a correlation of 0.66 is found between the retrieval and TOMCAT sampled accordingly, with a bias of 0.7 Dobson Units. GOME-2 estimates higher concentrations in NH pollution centres but lower ozone in the Southern Ocean and South Pacific, which is consistent with the comparison to ozonesondes.


2006 ◽  
Vol 6 (6) ◽  
pp. 11465-11520 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.


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.


2014 ◽  
Vol 7 (7) ◽  
pp. 7923-7962 ◽  
Author(s):  
G. M. Miles ◽  
R. Siddans ◽  
B. J. Kerridge ◽  
B. G. Latter ◽  
N. A. D. Richards

Abstract. This paper describes and assesses the performance of the RAL (Rutherford Appleton Laboratory) ozone profile retrieval scheme for the Global Ozone Monitoring Experiment 2 (GOME-2) with a~focus on tropospheric ozone. Developments to the scheme since its application to GOME-1 measurements are outlined. These include the approaches developed to account sufficiently for UV radiometric degradation in the Hartley band and for inadequacies in knowledge of instrumental parameters in the Huggins bands to achieve the high precision spectral fit required to extract information on tropospheric ozone. The assessment includes a validation against ozonesondes (sondes) sampled worldwide over two years (2007–2008). Standard deviations of the ensemble with respect to the sondes are considerably lower for the retrieved profiles than for the a priori, with the exception of the lowest sub-column. Once retrieval vertical smoothing (averaging kernels) has been applied to the sonde profiles there is a retrieval bias of 6% (1.5 DU) in the lower troposphere, with smaller biases in the sub-columns above. The bias in the troposphere varies with latitude. The retrieval underestimates lower tropospheric ozone in the Southern Hemisphere (SH) (15–20% or ~ 1–3 DU) and overestimates it in the Northern Hemisphere (NH) (10% or 2 DU). The ability of the retrieval to represent the geographical distribution of lower tropospheric ozone, globally (rather than just ozonesonde launch sites) is demonstrated through agreement with the chemistry transport model TOMCAT. For a monthly mean of cloud-cleared GOME-2 pixels, a correlation of 0.66 is found between the retrieval and TOMCAT sampled accordingly, with a bias of 0.7 Dobson Units. GOME-2 estimates higher concentrations in NH pollution centres but lower ozone in the Southern Ocean and South Pacific, which is consistent with the comparison to ozonesondes.


2010 ◽  
Vol 10 (10) ◽  
pp. 4725-4739 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  

Abstract. We analyze the theoretical basis of 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 from 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. We apply the three methods to a full year (2006) of TES and OMI data. Comparison with in situ data from ozonesondes 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. 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 further allows for CTM evaluation using both satellite observations. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics due to possible underestimates of biomass burning, soil, and lightning emissions. It overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx of ozone.


2013 ◽  
Vol 6 (2) ◽  
pp. 239-249 ◽  
Author(s):  
J. Bak ◽  
J. H. Kim ◽  
X. Liu ◽  
K. Chance ◽  
J. Kim

Abstract. South Korea is planning to launch the GEMS (Geostationary Environment Monitoring Spectrometer) instrument into the GeoKOMPSAT (Geostationary Korea Multi-Purpose SATellite) platform in 2018 to monitor tropospheric air pollutants on an hourly basis over East Asia. GEMS will measure backscattered UV radiances covering the 300–500 nm wavelength range with a spectral resolution of 0.6 nm. The main objective of this study is to evaluate ozone profiles and stratospheric column ozone amounts retrieved from simulated GEMS measurements. Ozone Monitoring Instrument (OMI) Level 1B radiances, which have the spectral range 270–500 nm at spectral resolution of 0.42–0.63 nm, are used to simulate the GEMS radiances. An optimal estimation-based ozone profile algorithm is used to retrieve ozone profiles from simulated GEMS radiances. Firstly, we compare the retrieval characteristics (including averaging kernels, degrees of freedom for signal, and retrieval error) derived from the 270–330 nm (OMI) and 300–330 nm (GEMS) wavelength ranges. This comparison shows that the effect of not using measurements below 300 nm on retrieval characteristics in the troposphere is insignificant. However, the stratospheric ozone information in terms of DFS decreases greatly from OMI to GEMS, by a factor of ∼2. The number of the independent pieces of information available from GEMS measurements is estimated to 3 on average in the stratosphere, with associated retrieval errors of ~1% in stratospheric column ozone. The difference between OMI and GEMS retrieval characteristics is apparent for retrieving ozone layers above ~20 km, with a reduction in the sensitivity and an increase in the retrieval errors for GEMS. We further investigate whether GEMS can resolve the stratospheric ozone variation observed from high vertical resolution Earth Observing System (EOS) Microwave Limb Sounder (MLS). The differences in stratospheric ozone profiles between GEMS and MLS are comparable to those between OMI and MLS below ~3 hPa (~40 km), except with slightly larger biases and larger standard deviations by up to 5%. At pressure altitudes above ~3 hPa, GEMS retrievals show strong influence of a priori and large differences with MLS, which, however, can be sufficiently improved by using better a priori information. The GEMS-MLS differences show negative biases of less than 4% for stratospheric column ozone, with standard deviations of 1–3%, while OMI retrievals show similar agreements with MLS except for 1% smaller biases at middle and high latitudes. Based on the comparisons, we conclude that GEMS will measure tropospheric ozone and stratospheric ozone columns with accuracy comparable to that of OMI and ozone profiles with slightly worse performance than that of OMI below ~3 hPa.


2010 ◽  
Vol 10 (24) ◽  
pp. 12273-12283 ◽  
Author(s):  
J. Kar ◽  
M. N. Deeter ◽  
J. Fishman ◽  
Z. Liu ◽  
A. Omar ◽  
...  

Abstract. A large wintertime increase in pollutants has been observed over the eastern parts of the Indo Gangetic Plains. We use improved version 4 carbon monoxide (CO) retrievals from the Measurements of Pollution in the Troposphere (MOPITT) along with latest version 3 aerosol data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) lidar instrument and the tropospheric ozone residual products to characterize this pollution pool. The feature is seen primarily in the lower troposphere from about November to February with strong concomitant increases in CO and aerosol optical depth (AOD). The signature of the feature is also observed in tropospheric ozone column data. The height resolved aerosol data from CALIPSO confirm the trapping of the pollution pool at the lowest altitudes. The observations indicate that MOPITT can capture this low altitude phenomenon even in winter conditions as indicated by the averaging kernels.


2019 ◽  
Vol 19 (21) ◽  
pp. 13569-13579 ◽  
Author(s):  
Helen M. Worden ◽  
A. Anthony Bloom ◽  
John R. Worden ◽  
Zhe Jiang ◽  
Eloise A. Marais ◽  
...  

Abstract. Biogenic non-methane volatile organic compounds (NMVOCs) emitted from vegetation are a primary source for the chemical production of carbon monoxide (CO) in the atmosphere, and these biogenic emissions account for about 18 % of the global CO burden. Partitioning CO fluxes to different source types in top-down inversion methods is challenging; typically a simple scaling of the posterior flux to prior flux values for fossil fuel, biogenic and biomass burning sources is used. Here we show top-down estimates of biogenic CO fluxes using a Bayesian inference approach, which explicitly accounts for both posterior and a priori CO flux uncertainties. This approach re-partitions CO fluxes following inversion of Measurements Of Pollution In The Troposphere (MOPITT) CO observations with the GEOS-Chem model, a global chemical transport model driven by assimilated meteorology from the NASA Goddard Earth Observing System (GEOS). We compare these results to the prior information for CO used to represent biogenic NMVOCs from GEOS-Chem, which uses the Model of Emissions of Gases and Aerosols from Nature (MEGAN) for biogenic emissions. We evaluate the a posteriori biogenic CO fluxes against top-down estimates of isoprene fluxes using Ozone Monitoring Instrument (OMI) formaldehyde observations. We find similar seasonality and spatial consistency in the posterior CO and top-down isoprene estimates globally. For the African savanna region, both top-down CO and isoprene seasonality vary significantly from the MEGAN a priori inventory. This method for estimating biogenic sources of CO will provide an independent constraint on modeled biogenic emissions and has the potential for diagnosing decadal-scale changes in emissions due to land-use change and climate variability.


2014 ◽  
Vol 14 (17) ◽  
pp. 9249-9258 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  

Abstract. High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 ± 0.04 and 0.7 ± 0.02 mW m−2 in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1σ) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.


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