Measurements Of Pollution In The Troposphere Data Research Articles

Differences in MOPITT surface level CO retrievals and trends from Level 2 and Level 3 products in coastal grid boxes

Abstract. Users of MOPITT (Measurement of Pollution in the Troposphere) data are advised to discard retrievals performed over water from analyses. This is because MOPITT retrievals are more sensitive to near-surface CO when performed over land than water, meaning that they have a greater measurement component and are less tied to the a priori CO concentrations (which are taken from a model climatology) that are necessarily used in their retrieval. MOPITT Level 3 (L3) products are a 1∘ × 1∘ gridded average of finer-resolution (∼ 22 × 22 km) Level 2 (L2) retrievals. In the case of coastal L3 grid boxes, L2 retrievals performed over both land and water may be averaged together to create the L3 product, with L2 retrievals over land not contributing to the average at all in certain situations. This conflicts with data usage recommendations. The aim of this paper is to highlight the consequences that this has on surface level retrievals and their temporal trends in “as-downloaded” L3 data (L3O), by comparing them to those obtained if only the L2 retrievals performed over land are averaged to create the L3 product (L3L), for all identified coastal L3 MOPITT grid boxes. First, the difference between surface level retrievals in L3L and the corresponding L2 retrievals performed over water (L3W) is established for days when they are averaged together to create the L3O product for coastal grid boxes (yielding an L3O surface index of “mixed”, L3OM). Mean retrieved volume mixing ratios (VMRs) in L3L differ by over 10 ppbv from those in L3W, and temporal trends detected in L3L are between 0.28 and 0.43 ppbv yr−1 stronger than in L3W, on average. These L3L − L3W differences are clearly linked to retrieval sensitivity differences, with L3W being more heavily tied to the a priori CO profiles used in the retrieval, which are a model-derived monthly mean climatology that, by definition, has no trend year to year. VMRs in the resulting L3OM are significantly different to L3L for 45 % of all coastal grid boxes, corresponding to 75 % of grid boxes where the L3L − L3W difference is also significant. Just under half of the grid boxes that featured a significant L3L − L3W trend difference also see trends differing significantly between L3L and L3OM. Factors that determine whether L3OM and L3L differ significantly include the proportion of the surface covered by land/water and the magnitude of land–water contrast in retrieval sensitivity. Comparing the full L3O dataset to L3L, it is shown that if L3O is filtered so that only retrievals over land (L3OL) are analysed – as recommended – there is a huge loss of days with data for coastal grid boxes. This is because L2 retrievals over land are routinely discarded during the L3O creation process for these grid boxes. There is less data loss if L3OM retrievals are also retained, but the resulting L3O “land or mixed” (L3OLM) subset still has fewer data days than L3L for 61 % of coastal grid boxes. As shown, these additional days with data feature some influence from retrievals made over water, demonstrably affecting mean VMRs and their trends. Coastal L3 grid boxes contain 33 of the 100 largest coastal cities in the world, by population. Focusing on the L3 grid boxes containing these cities, it is shown that mean VMRs in L3OL and L3L differ significantly for 11 of the 27 grid boxes that can be compared (there are no L3OL data for 6 of the grid boxes studied), with 9 of the 18 grid boxes where temporal trend analysis can be performed in L3OL featuring a trend that is significantly different to that in L3L. These differences are a direct result of the data loss in L3OL – data that are available in L2 data (and are incorporated into the L3L product created for this study). The L3L − L3OLM mean VMR difference exceeds 10 (22) ppbv for 11 (3) of these 33 grid boxes, significant in 13 cases, with significant temporal trend differences in 5 cases. It is concluded that an L3 product based only on L2 retrievals over land – the L3L product analysed in this paper, available for public download – could be of benefit to MOPITT data users.

A comparison of carbon monoxide retrievals between the MOPITT satellite and Canadian high-Arctic ground-based NDACC and TCCON FTIR measurements

Abstract. Measurements of Pollution In The Troposphere (MOPITT) is an instrument on NASA's Terra satellite that has measured tropospheric carbon monoxide (CO) from early 2000 to the present day. Validation of data from satellite instruments like MOPITT is often conducted using ground-based measurements to ensure the continued accuracy of the space-based instrument's measurements and its scientific results. Previous MOPITT validation studies generally found a larger bias in the MOPITT data poleward of 60∘ N. In this study, we use data from 2006 to 2019 from the Bruker IFS 125HR Fourier Transform Infrared spectrometer (FTIR) located at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut, Canada, to validate the MOPITT version 8 (V8) retrievals. These comparisons utilize mid- and near-infrared FTIR measurements made as part of the Network for the Detection for Atmospheric Composition Change (NDACC) and the Total Carbon Column Observing Network (TCCON), respectively. All MOPITT version 8 retrievals within a radius of 110 km (1∘) from the PEARL Ridge Laboratory and within a 24 h time interval are used in this validation study. MOPITT retrieval products include those from the near-infrared (NIR) channel, the thermal infrared (TIR) channel, and a joint product from the thermal and near-infrared (TIR–NIR) channels. Each channel's detector has 4 pixels. We calculated the MOPITT pixel-to-pixel biases for each pixel, which were found to vary based on the season and surface type (land or water). The systematic bias for pixel 1 over land is larger than that for other pixels, which can reach up to 20 ppb. We use a small-region approximation method to find filtering criteria. We then apply the filters to the MOPITT dataset to minimize the MOPITT pixel bias and the number of outliers in the dataset. The sensitivity of each MOPITT pixel and each product is examined over the Canadian high Arctic. We then follow the methodologies recommended by NDACC and TCCON for the comparison between the FTIR and satellite total column retrievals. MOPITT averaging kernels are used to weight the NDACC and TCCON retrievals and take into account the different vertical sensitivities between the satellite and PEARL FTIR measurements. We use a modified Taylor diagram to present the comparison results from each pixel for each product over land and water with NDACC and TCCON measurements. Our results show overall consistency between MOPITT and the NDACC and TCCON measurements. When compared to the FTIR, the NIR MOPITT retrievals have a positive bias of 3 %–10 % depending on the pixel. The bias values are negative for the TIR product, with values between −5 % and 0 %. The joint TIR–NIR products show differences of −4 % to 7 %. The drift in MOPITT biases (in units of % yr−1) relative to NDACC and TCCON varies by MOPITT data product. In the NIR, drifts vs. TCCON are smaller than those vs. NDACC; however, this scenario is reversed for the MOPITT TIR and joint TIR–NIR products. Overall, this study aims to provide detailed validation for MOPITT version 8 measurements in the Canadian high Arctic.

Assimilation of S5P/TROPOMI carbon monoxide data with the global CAMS near-real-time system

Abstract. The Tropospheric Monitoring Instrument (TROPOMI) on the Copernicus Sentinel 5 Precursor (S5P) satellite, launched in October 2017, provides a wealth of atmospheric composition data, including total columns of carbon monoxide (TCCO) at high horizontal resolution (5.5 km × 7 km). Near-real-time TROPOMI TCCO data have been monitored in the global data assimilation system of the Copernicus Atmosphere Monitoring Service (CAMS) since November 2018 to assess the quality of the data. The CAMS system already routinely assimilates TCCO data from the Measurement of Pollution in the Troposphere (MOPITT) instrument and the Infrared Atmospheric Sounding Interferometer (IASI) outside the polar regions. The assimilation of TROPOMI TCCO data in the CAMS system was tested for the period 6 July to 31 December 2021, i.e. after the TROPOMI algorithm update to version 02.02.00 in July 2021. By assimilating TROPOMI TCCO observations, the CAMS CO columns increase by on average 8 %, resulting in an improved fit to independent observations (IAGOS aircraft profiles and NDACC Fourier transform infrared (FTIR) tropospheric and total-column CO data) compared to a version of the CAMS system where only TCCO from MOPITT and IASI is assimilated. The largest absolute and relative changes from the assimilation of TROPOMI CO are found in the lower and middle troposphere, i.e. that part of the atmosphere that is not already well constrained by the assimilated TIR MOPITT and IASI data. The largest impact near the surface comes from clear-sky TROPOMI data over land, and additional vertical information comes from the retrievals of measurements in cloudy conditions. July and August 2021 saw record numbers of boreal wildfires over North America and Russia, leading to large amounts of CO being released into the atmosphere. The paper assesses the impact of TROPOMI CO assimilation on selected CO plumes more closely. While the CO column can be well constrained by the assimilation of TROPOMI CO data, and the fit to individual IAGOS CO profiles in the lower and middle troposphere is considerably improved, the TROPOMI CO columns do not provide further constraints on individual plumes that are transported across continents and oceans at altitudes above 500 hPa.

Satellite-Observed Variations and Trends in Carbon Monoxide over Asia and Their Sensitivities to Biomass Burning

As the carbon monoxide (CO) total column over Asia is among the highest in the world, it is important to characterize its variations in space and time. Using Measurements of Pollution in the Troposphere (MOPITT) and Atmospheric InfraRed Sounder (AIRS) satellite data, the variations and trends in CO total column over Asia and its seven subregions during 2003–2017 are investigated in this study. The CO total column in Asia is higher in spring and winter than in summer and autumn. The seasonal maximum and minimum are in spring and summer respectively in the regional mean over Asia, varying between land and oceans, as well as among the subregions. The CO total column in Asia shows strong interannual variation, with a regional mean coefficient of variation of 5.8% in MOPITT data. From 2003 to 2017, the annual mean of CO total column over Asia decreased significantly at a rate of (0.58 ± 0.15)% per year (or −(0.11 ± 0.03) × 1017 molecules cm−2 per year) in MOPITT data, resulting from significant CO decreases in winter, summer, and spring. In most of the subregions, significant decreasing trends in CO total column are also observed, more obviously over areas with high CO total column, including eastern regions of China and the Sichuan Basin. The regional decreasing trends in these areas are over 1% per year. Over the entire Asia, and in fire-prone subregions including South Siberia, Indo-China Peninsula, and Indonesia, we found significant correlations between the MOPITT CO total column and the fire counts from the Moderate Resolution Imaging Spectroradiometer (MODIS). The variations in MODIS fire counts may explain 58%, 60%, 36%, and 71% of the interannual variation in CO total column in Asia and these three subregions, respectively. Over different land cover types, the variations in biomass burning may explain 62%, 52%, and 31% of the interannual variation in CO total column, respectively, over the forest, grassland, and shrubland in Asia. Extremes in CO total column in Asia can be largely explained by the extreme fire events, such as the fires over Siberia in 2003 and 2012 and over Indonesia in 2006 and 2015. The significant decreasing trends in MODIS fire counts inside and outside Asia suggest that global biomass burning may be a driver for the decreasing trend in CO total column in Asia, especially in spring. In general, the variations and trends in CO total column over Asia detected by AIRS are similar to but smaller than those by MOPITT. The two datasets show similar spatial and temporal variations in CO total column over Asia, with correlation coefficients of 0.86–0.98 in the annual means. This study shows that the interannual variation in atmospheric CO in Asia is sensitive to biomass burning, while the decreasing trend in atmospheric CO over Asia coincides with the decreasing trend in MODIS fire counts from 2003 to 2017.

Evaluation of MOPITT Version 7 joint TIR–NIR X<sub>CO</sub> retrievals with TCCON

Abstract. Observations of carbon monoxide (CO) from the Measurements Of Pollution In The Troposphere (MOPITT) instrument aboard the Terra spacecraft were expected to have an accuracy of 10 % prior to the launch in 1999. Here we evaluate MOPITT Version 7 joint (V7J) thermal-infrared and near-infrared (TIR–NIR) retrieval accuracy and precision and suggest ways to further improve the accuracy of the observations. We take five steps involving filtering or bias corrections to reduce scatter and bias in the data relative to other MOPITT soundings and ground-based measurements. (1) We apply a preliminary filtering scheme in which measurements over snow and ice are removed. (2) We find a systematic pairwise bias among the four MOPITT along-track detectors (pixels) on the order of 3–4 ppb with a small temporal trend, which we remove on a global scale using a temporally trended bias correction. (3) Using a small-region approximation (SRA), a new filtering scheme is developed and applied based on additional quality indicators such as the signal-to-noise ratio (SNR). After applying these new filters, the root-mean-squared error computed using the local median from the SRA over 16 years of global observations decreases from 3.84 to 2.55 ppb. (4) We also use the SRA to find variability in MOPITT retrieval anomalies that relates to retrieval parameters. We apply a bias correction to one parameter from this analysis. (5) After applying the previous bias corrections and filtering, we compare the MOPITT results with the GGG2014 ground-based Total Carbon Column Observing Network (TCCON) observations to obtain an overall global bias correction. These comparisons show that MOPITT V7J is biased high by about 6 %–8 %, which is similar to past studies using independent validation datasets on V6J. When using TCCON spectrometric column retrievals without the standard airmass correction or scaling to aircraft (WMO scale), the ground- and satellite-based observations overall agree to better than 0.5 %. GEOS-Chem data assimilations are used to estimate the influence of filtering and scaling to TCCON on global CO and tend to pull concentrations away from the prior fluxes and closer to the truth. We conclude with suggestions for further improving the MOPITT data products.

Quantifying Emissions of CO and NOx Using Observations From MOPITT, OMI, TES, and OSIRIS

AbstractWe use the GEOS‐Chem four‐dimensional variational data assimilation system to estimate emissions of carbon monoxide (CO) and nitrogen oxides (NOx) in November 2009 and July 2010. We assimilated CO retrievals from The Measurements of Pollution In The Troposphere (MOPITT), ozone (O3) retrievals from the Tropospheric Emission Spectrometer (TES) and the Optical Spectrograph and InfraRed Imager System (OSIRIS), and NO2 columns from the Ozone Monitoring Instrument (OMI). By assimilating data for multiple chemical species with the four‐dimensional variational scheme we obtain a consistent chemical state over the assimilation period. The modeled O3 bias was reduced to less than 3.5 ppbv everywhere, relative to independent aircraft O3 data, except in the high‐latitude upper troposphere and lower stratosphere. We found that in November, the CO and NOx emission estimates obtained with the multiple species assimilation were generally comparable to those inferred from assimilating only MOPITT or OMI data, respectively, whereas in July the differences were larger. For the main anthropogenic source regions, the inferred North American and European emissions responded most strongly to the multispecies information in the assimilation. In July, North American and European CO emission estimates differed by 31% and 65% relative to the MOPITT‐only estimates, respectively. We also found large differences for the North American and European NOx emission estimates, which differed by 27% and 16% relative to the OMI‐only estimates, respectively. Our results highlight the potential benefit of exploiting the additional constraints offered by multispecies chemical data assimilation.

A 15-year record of CO emissions constrained by MOPITT CO observations

Abstract. Long-term measurements from satellites and surface stations have demonstrated a decreasing trend of tropospheric carbon monoxide (CO) in the Northern Hemisphere over the past decade. Likely explanations for this decrease include changes in anthropogenic, fires, and/or biogenic emissions or changes in the primary chemical sink hydroxyl radical (OH). Using remotely sensed CO measurements from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument, in situ methyl chloroform (MCF) measurements from the World Data Centre for Greenhouse Gases (WDCGG) and the adjoint of the GEOS-Chem model, we estimate the change in global CO emissions from 2001 to 2015. We show that the loss rate of MCF varied by 0.2 % in the past 15 years, indicating that changes in global OH distributions do not explain the recent decrease in CO. Our two-step inversion approach for estimating CO emissions is intended to mitigate the effect of bias errors in the MOPITT data as well as model errors in transport and chemistry, which are the primary factors contributing to the uncertainties when quantifying CO emissions using these remotely sensed data. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, and unchanged anthropogenic CO emissions from Europe since 2008. We find decreasing trends of biomass burning CO emissions from boreal North America, boreal Asia and South America, but little change over Africa. In contrast to prior results, we find that a positive trend in CO emissions is likely for India and southeast Asia.

The MOPITT Version 6 product: algorithm enhancements and validation

Abstract. The Measurements of Pollution in the Troposphere (MOPITT) Version 6 (V6) product for carbon monoxide (CO) incorporates several enhancements which will benefit many users of MOPITT data. V6 algorithm improvements are described in detail, and V6 validation results are presented. First, a geolocation bias related to the orientation of the MOPITT instrument relative to the TERRA platform was characterized and eliminated. Second, the variable a priori for CO concentrations for V6 is based on simulations performed with the chemical transport model Community Atmosphere Model with Chemistry (CAM-chem) for the years 2000–2009 instead of the model-derived climatology for 1997–2004 used for V5. Third, meteorological fields required for V6 retrieval processing are extracted from the MERRA (Modern-Era Retrospective Analysis For Research And Applications) reanalysis. Finally, a significant latitude-dependent retrieval bias in the upper troposphere in Version 5 products has been substantially reduced.

Technical Note: Temporal change in averaging kernels as a source of uncertainty in trend estimates of carbon monoxide retrieved from MOPITT

Abstract. It has become possible to retrieve the global, long-term trends of trace gases that are important to atmospheric chemistry, climate, and air quality from satellite data records that span more than a decade. However, many of the satellite remote sensing techniques produce measurements that have variable sensitivity to the vertical profiles of atmospheric gases. In the case of constrained retrievals like optimal estimation, this leads to a varying amount of a priori information in the retrieval and is represented by an averaging kernel (AK). In this study, we investigate to what extent the estimation of trends from retrieved data can be biased by temporal changes of averaging kernels used in the retrieval algorithm. In particular, the surface carbon monoxide data retrieved from the Measurements Of Pollution In The Troposphere (MOPITT) instrument from 2001 to 2010 were analyzed. As a practical example based on the MOPITT data, we show that if the true atmospheric mixing ratio is continuously 50% higher or lower than the a priori state, the temporal change of the averaging kernel at the surface level gives rise to an artificial trend in retrieved surface carbon monoxide, ranging from −10.71 to +13.21 ppbv yr−1 (−5.68 to +8.84 % yr−1) depending on location. Therefore, in the case of surface (or near-surface level) CO derived from MOPITT, the AKs trends multiplied by the difference between true and a priori states must be quantified in order to estimate trend biases.

Study of the impact of wildfire emissions, through MOPITT total CO column, at different spatial scales

The estimation of total carbon monoxide (CO) column has been identified as essential to improve our understanding of its role in the global climate system. The Earth Observing System (EOS) Science Steering Committee and the World Meteorological Organization (WMO) has suggested that a satellite-borne CO sensor, which would operate for extended periods, would be useful for that task. Measurements of Pollution in the Troposphere (MOPITT), on board the Terra spacecraft, is a correlation radiometer for estimating CO vertical profiles and total CO column in the lower atmosphere, through the thermal radiance received in the 4.7 μm spectral region. One of the main sources of CO in the atmosphere is the fires and global biomass-burning emissions that are produced when combustion is not complete, especially in the smouldering phase. This article presents a methodology based on a Fourier technique and spatial analysis in order to estimate the total CO column contribution of wildfires at three different spatial scales. First, in a seasonal study, a Mediterranean country (Spain) is selected, and the main regions affected by fire during four years in the summer season are analysed. Second, in order to estimate CO emissions at a local scale, a large fire (in Spain) and a cluster of fires (in North China) are selected. Third, for a global study at large scale and for comparing with CO and carbon dioxide (CO2) data from Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY), locations in North China, equatorial Africa, and Amazonia are selected. Results obtained show that MOPITT data are suitable to assess and to discriminate CO emissions at local spatial scales. Finally, a qualitative agreement between CO behaviour obtained by MOPITT and CO and CO2 obtained by SCIAMACHY is found.

Regional CO pollution over the Indian-subcontinent and various transport pathways as observed by MOPITT

We used day-side Measurement of Pollution in the Troposphere (MOPITT) carbon monoxide (CO) retrievals (2000–2007) to examine the regional CO emission and its transport pathways during the summer/winter monsoon, with a specific focus on the Indian-subcontinent. It is observed that MOPITT CO retrievals at 850 hPa level in general show large scale features of CO emission in India, as reflected in the bottom-up inventory. In particular, high CO mixing ratios over the eastern north-eastern part of India, along the Indo-Gangetic (IG) region, and low CO mixing ratios over central India are generally captured from the MOPITT data. A strong plume with enhanced CO mixing ratios at 350 hPa is observed during the summer monsoon, demonstrating large scale vertical transport of the boundary layer CO from the Indian region into the upper troposphere. During winter outflow CO from the Indian region is found to be transported over the Arabian Sea and Bay of Bengal and reaches up to Saudi Arabia and north-eastern Africa. It is observed that emissions from Southeast Asia and the eastern north-eastern Indian region have the greatest impact over the Bay of Bengal and the eastern Indian Ocean, while emissions from the rest of India dominate over the Arabian Sea and the western Indian Ocean.

Bayesian statistical modeling of spatially correlated error structure in atmospheric tracer inverse analysis

Abstract. We present and discuss the use of Bayesian modeling and computational methods for atmospheric chemistry inverse analyses that incorporate evaluation of spatial structure in model-data residuals. Motivated by problems of refining bottom-up estimates of source/sink fluxes of trace gas and aerosols based on satellite retrievals of atmospheric chemical concentrations, we address the need for formal modeling of spatial residual error structure in global scale inversion models. We do this using analytically and computationally tractable conditional autoregressive (CAR) spatial models as components of a global inversion framework. We develop Markov chain Monte Carlo methods to explore and fit these spatial structures in an overall statistical framework that simultaneously estimates source fluxes. Additional aspects of the study extend the statistical framework to utilize priors on source fluxes in a physically realistic manner, and to formally address and deal with missing data in satellite retrievals. We demonstrate the analysis in the context of inferring carbon monoxide (CO) sources constrained by satellite retrievals of column CO from the Measurement of Pollution in the Troposphere (MOPITT) instrument on the TERRA satellite, paying special attention to evaluating performance of the inverse approach using various statistical diagnostic metrics. This is developed using synthetic data generated to resemble MOPITT data to define a proof-of-concept and model assessment, and then in analysis of real MOPITT data. These studies demonstrate the ability of these simple spatial models to substantially improve over standard non-spatial models in terms of statistical fit, ability to recover sources in synthetic examples, and predictive match with real data.

A comparison of OEM CO retrievals from the IASI and MOPITT instruments

Abstract. Observations of atmospheric carbon monoxide (CO) can only be made on continental and global scales by remote sensing instruments situated in space. One such instrument is the Infrared Atmospheric Sounding Interferometer (IASI), producing spectrally resolved, top-of-atmosphere radiance measurements from which CO vertical layers and total columns can be retrieved. This paper presents a technique for intercomparisons of satellite data with low vertical resolution. The example in the paper also generates the first intercomparison between an IASI CO data set, in this case that produced by the University of Leicester IASI Retrieval Scheme (ULIRS), and the V3 and V4 operationally retrieved CO products from the Measurements Of Pollution In The Troposphere (MOPITT) instrument. The comparison is performed for a localised region of Africa, primarily for an ocean day-time configuration, in order to develop the technique for instrument intercomparison in a region with well defined a priori. By comparing both the standard data and a special version of MOPITT data retrieved using the ULIRS a priori for CO, it is shown that standard intercomparisons of CO are strongly affected by the differing a priori data of the retrievals, and by the differing sensitivities of the two instruments. In particular, the differing a priori profiles for MOPITT V3 and V4 data result in systematic retrieved profile changes as expected. An application of averaging kernels is used to derive a difference quantity which is much less affected by smoothing error, and hence more sensitive to systematic error. These conclusions are confirmed by simulations with model profiles for the same region. This technique is used to show that for the data that has been processed the systematic bias between MOPITT V4 and ULIRS IASI data, at MOPITT vertical resolution, is less than 7 % for the comparison data set, and on average appears to be less than 4 %. The results of this study indicate that intercomparisons of satellite data sets with low vertical resolution should ideally be performed with: retrievals using a common a priori appropriate to the geographic region studied; the application of averaging kernels to compute difference quantities with reduced a priori influence; and a comparison with simulated differences using model profiles for the target gas in the region.

Seasonal cycle of emissions of CO inferred from MOPITT profiles of CO: Sensitivity to pyroconvection and profile retrieval assumptions

[1] We estimate monthly continental-scale CO emissions for 2006 by optimally fitting prior emissions used by the GEOS-Chem chemistry transport model to retrieved profile measurements of CO from the Measurement Of Pollution In The Troposphere (MOPITT) satellite instrument. We focus on the range of emission estimates obtained by using different versions of the MOPITT profile data, and by better describing enhanced vertical mixing of emissions from wildfires. We find that annual posterior CO emissions estimates for 2006 range from 1003 to 1180 Tg CO, within the range of prior estimates (1243 ± 617 Tg CO). We generally find larger differences in posterior CO emissions from using different versions of the MOPITT data than from improving the description of wildfires, with the exception of fires over Indonesia. Posterior emissions over regions with wildfires have a large seasonal cycle, as expected, which can be substantially different from prior emission estimates. We find GFEDv2 prior emissions underestimate the duration of the biomass burning season for North Africa by as much as 1 month. We also find posterior emissions over Indonesia are a factor of 2 higher than prior emissions (83 ± 42 Tg CO) in 2006 due to widespread fires during July–December. Posterior emissions over Canada during 2006 are a factor of 2–3 higher than prior emissions (9 ± 4.6 Tg CO). We also find a seasonal cycle of CO emissions over North America and Europe, in agreement with previous studies, which is not described by prior emissions.

Wintertime pollution over the Eastern Indo-Gangetic Plains as observed from MOPITT, CALIPSO and tropospheric ozone residual data

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.

Observations of near‐surface carbon monoxide from space using MOPITT multispectral retrievals

Using both thermal infrared (TIR) and near infrared (NIR) channels of MOPITT (Measurements of Pollution in the Troposphere) on EOS‐Terra, we demonstrate the first coincident multispectral retrievals of carbon monoxide (CO) from space. Exploiting both TIR and NIR channels has been possible due to recent progress in characterizing NIR channel radiance errors. This has allowed us to trade off sensitivity to near surface CO for larger random errors in the combined retrieval. By examining retrieval diagnostics such as DFS (degrees of freedom for signal) and averaging kernels for the multispectral retrieval (TIR + NIR) as compared to the TIR‐only retrieval, we find that adding the NIR channel to the retrieval significantly increases sensitivity to CO, especially near the surface, but with high spatial variability due to surface albedo variations. The cases with the largest increases in DFS are over regions with low thermal contrast between the surface and lower atmosphere. In the tropics (23.4°S–23.4°N), the fraction of daytime land cases with at least 0.4 DFS in the surface layer (surface to 800 hPa) is 20% for TIR‐only retrievals compared to 59% for multispectral retrievals. Vertical resolution for the surface layer is also improved, in some cases from around 6 km for TIR‐only to roughly 1 km for TIR + NIR. Since we apply a single a priori CO profile (unlike MOPITT V4) and error covariance in all the retrievals reported here, these increases are due solely to the addition of the NIR channel. Enhanced sensitivity to near surface CO is especially evident in a case study for central/east Asia where source regions for urban areas with high population density are clearly identifiable. Although these retrievals are still a research product and require further validation and scientific evaluation, they demonstrate the increased sensitivity to CO in the lowermost troposphere that can be obtained from multispectral MOPITT data.

Spatial distribution of near-surface CO over bay of Bengal during winter: role of transport

As part of Integrated Campaign for Aerosols, gases and Radiation Budget (ICARB), cruise-based measurements of near-surface CO were carried out over Bay of Bengal (BoB) covering the latitude–longitude sector 3.5°N–21.0°N and 76.0°E–98.0°E, during winter months of December 2008 to January 2009. These in-situ measured CO mixing ratio varied in the range of 80–480 ppbv over this marine environment with the distinct spatial pattern. The highest mixing ratios were measured over southeast-BoB with mean value of 379±58 ppbv. CO mixing ratios were high over north-BoB compared to southern BoB. These in-situ measurements were compared with the satellite-measured surface CO obtained from Measurements of Pollution in the Troposphere (MOPITT) onboard TERRA and found to be in good agreement over most of the regions, except at southeast-BoB. Surface CO and column CO from MOPITT data showed a similar spatial pattern. Based on the analysis of airmass back-trajectories, satellite-based spatial map of CO distribution over Asian region and Potential Source Contribution Function analysis, different pathways of transport of CO were identified. Transport from northern landmass as well as from south-east Asia has a significant influence in the spatial variation of CO over BoB. Winter-time mixing ratio of CO was found to be higher compared to those measured during other campaigns conducted during February–March 1999, 2001 (pre-monsoon) and September–October, 2002 (post-monsoon).

Variability of springtime transpacific pollution transport during 2000–2006: the INTEX-B mission in the context of previous years

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.

On the capability of IASI measurements to inform about CO surface emissions

Abstract. Between July and November 2008, simultaneous observations were conducted by several orbiting instruments that monitor carbon monoxide in the atmosphere, among them the Infrared Atmospheric Sounding Instrument (IASI) and Measurements Of Pollution In The Troposphere (MOPITT). In this paper, the concentration retrievals at about 700 hPa from these two instruments are successively used in a variational Bayesian system to infer the global distribution of CO emissions. Starting from a global emission budget of 479 Tg for the considered period, the posterior estimate of CO emissions using IASI retrievals gives a total of 643 Tg, which is in close agreement with the budget calculated with version 3 of the MOPITT data (649 Tg). The regional totals are also broadly consistent between the two inversions. Even though our theoretical error budget indicates that IASI constrains the emissions slightly less than MOPITT, because of lesser sensitivity in the lower troposphere, these first results indicate that IASI may play a major role in the quantification of the emissions of CO.

Retrieval of Carbon monoxide profiles over Indian region using MOPITT data

Vertical profiles of carbon monoxide (CO) over the Indian region have scarcely been monitored. Satellite sensor, Measurement Of Pollution In The Troposphere (MOPITT) provides profiles of CO using a global retrieval scheme, which converts measured radiances to CO mixing ratios. In this study we have developed a regional retrieval scheme, valid over the Indian region, which employs Line-By-Line (LBL) calculations over a tropical model atmosphere to generate a Look-Up-Table (LUT) forward model function and uses a regional a priori dataset of CO along with seasonally variable emissivity to invert the MOPITT radiances to CO profiles. This baseline study provides an approach to optimizing retrievals for specific regional applications. A case study was carried out over a forest fire prone region in Northern India from February to April 2005 to validate the retrieval algorithm. The results are in agreement with the fire maps generated from MODerate resolution Imaging Spectro-radiometer (MODIS). The shape of the CO profiles over the region matches quite well with the vertical structure of CO during the INDOEX campaign, especially during the polluted month of April. Inter-comparisons with the MOPITT data product indicate some discrepancies in the lower troposphere, especially during the forest fire season. Future studies with in-situ measurements may be able to diagnose these disparities.