Measurements Of Pollution In The Troposphere Research Articles

Nonlinear and Non‐Gaussian Ensemble Assimilation of MOPITT CO

AbstractSatellite retrievals of carbon monoxide (CO) are routinely assimilated in atmospheric chemistry models to improve air quality forecasts, produce reanalyzes and to estimate emissions. This study applies the quantile‐conserving ensemble filter framework, a novel assimilation algorithm that can deal with non‐Gaussian and modestly nonlinear distributions. Instead of assuming normal distributions like the Ensemble Adjustments Kalman Filter (EAKF), we now apply a bounded normal rank histogram (BNRH) distribution for the prior. The goal is to efficiently estimate bounded quantities such as CO atmospheric mixing ratios and emission fluxes while maintaining the good performance achieved by the EAKF. We contrast assimilating meteorological and MOPITT (Measurement of Pollution in the Troposphere) observations for May 2018. We evaluate the results with the fourth deployment of the NASA Atmospheric Tomography Mission (ATom‐4) airborne field campaign. We also compare simulations with CO tropospheric columns from the network for the detection of atmospheric composition change and surface in‐situ observations from NOAA carbon cycle greenhouse gases. While the differences remain small, the BNRH approach clearly works better than the EAKF in comparison to all observation data sets.

Diagnosing uncertainties in global biomass burning emission inventories and their impact on modeled air pollutants

Abstract. Large uncertainties persist within current biomass burning (BB) inventories, and the choice of these inventories can substantially impact model results when assessing the influence of BB aerosols on weather and climate. We evaluated discrepancies among BB emission inventories by comparing carbon monoxide (CO) and organic carbon (OC) emissions from seven major BB regions globally between 2013 and 2016. Mainstream bottom-up inventories, including the Fire INventory from NCAR 1.5 (FINN1.5) and Global Fire Emissions Database version 4s (GFED4s), along with the top-down inventories Quick Fire Emissions Dataset 2.5 (QFED2.5) and Visible Infrared Imaging Radiometer (VIIRS-)based Fire Emission Inventory version 0 (VFEI0), were selected for this study. Global CO emissions range from 252 to 336 Tg, with regional disparities reaching up to a 6-fold difference. Dry matter is the primary contributor to the regional variation in CO emissions (50 %–80 %), with emission factors accounting for the remaining 20 %–50 %. Uncertainties in dry matter often arise from biases in calculating bottom fuel consumption and burned area, influenced by vegetation classification methods and fire detection products. In the tropics, peatlands contribute more fuel loads and higher emission factors than grasslands. At high latitudes, increased cloud fraction amplifies the discrepancy in estimated burned area (or fire radiative power) by 20 %. The global OC emissions range from 14.9 to 42.9 Tg, exhibiting higher variability than CO emissions due to the corrected emission factors in QFED2.5, with regional disparities reaching a factor of 8.7. Additionally, we applied these BB emission inventories to the Community Atmosphere Model version 6 (CAM6) and assessed the model performance against observations. Our results suggest that the simulations based on the GFED4s agree best with the Measurements of Pollution in the Troposphere (MOPITT-)retrieved CO. While comparing the simulation with the Moderate Resolution Imaging Spectroradiometer (MODIS) and AErosol RObotic NETwork (AERONET) aerosol optical depth (AOD), our results reveal that there is no global optimal choice for BB inventories. In the high latitudes of the Northern Hemisphere, using GFED4s and QFED2.5 can better capture the AOD magnitude and diurnal variation. In equatorial Asia, GFED4s outperforms other models in representing day-to-day changes, particularly during intense burning. In Southeast Asia, we recommend using the OC emission magnitude from FINN1.5 combined with daily variability from QFED2.5. In the Southern Hemisphere, the latest VFEI0 has performed relatively well. This study has implications for reducing the uncertainties in emissions and improving BB emission inventories in further studies.

TROPESS-CrIS CO single-pixel vertical profiles: intercomparisons with MOPITT and model simulations for 2020 western US wildfires

Abstract. The new TROPESS (TRopospheric Ozone and its Precursors from Earth System Sounding) profile retrievals of carbon monoxide (CO) from the Cross-track Infrared Sounder (CrIS) are evaluated against Measurement of Pollution in the Troposphere (MOPITT) CO version 9 data. Comparison results that were adjusted to common a priori constraints in the retrieval processes have improved agreement between the two data sets over direct comparisons. TROPESS-CrIS CO profiles are within 5 % of MOPITT but have higher concentrations in the lower troposphere and lower concentrations in the upper troposphere. For the intense western US wildfire events in September 2020, we compare CO fields simulated by the GISS climate model to the two satellite CO observations. We show intermediate steps of the comparison process to illustrate the evaluation of model simulations by deriving the “retrieved” model CO profiles as they would be observed by the satellite. This includes the application of satellite level-2 data along with their corresponding diagnostic operators provided in the TROPESS-CrIS and MOPITT products. The process allows a diagnosis of potential model improvements in modeling fire emissions and pollution transport.

CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data

CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data

Identifying episodic carbon monoxide emission events in the MOPITT measurement dataset

Abstract. The Measurements Of Pollution In The Troposphere (MOPITT) instrument aboard NASA's Terra satellite has been measuring upwelling radiance in a nadir-viewing mode since March 2000. These radiance measurements are inverted to yield estimates of carbon monoxide (CO) profiles and total columns, providing the longest satellite record of this trace gas to date. The CO measurements from MOPITT have been used in a variety of ways, including trend analyses and the construction of CO budgets. However, their use is complicated by the influence of episodic emission events, which release large quantities of CO into the atmosphere with irregular timing, such as large sporadic wildfires of natural or anthropogenic origin. The chaotic nature of these events is a large source of variability in CO budgets and models, requiring that these events be well characterized in order to develop an improved understanding of the role they have in influencing tropospheric CO. This study describes the development of a multistep algorithm that is used to identify large episodic emission events using daily mean Level 2 (L2) MOPITT total column measurements gridded to a 0.5 by 0.5° spatial resolution. The core component of this procedure involves empirically determining the expectation density function (EDF) that describes the departure of daily-mean CO observations from the baseline behaviour of CO, as described by its periodic components and trends. The EDFs employed are not assumed to be symmetric but instead are constructed from a pair of superimposed normal distributions. Enhancement flag files are produced following this methodology, identifying the episodic events that show strong enhancement of CO outside of the range of expected CO behaviour and are now made available for the period 3 March 2000 to 31 July 2022. The distribution and frequency of these flagged measurements over this 22-year period are analyzed in order to illustrate the robustness of this method.

Advantages of assimilating multispectral satellite retrievals of atmospheric composition: a demonstration using MOPITT carbon monoxide products

Abstract. The Measurements Of Pollution In The Troposphere (MOPITT) is an ideal instrument to understand the impact of (1) assimilating multispectral and joint retrievals versus single spectral products, (2) assimilating satellite profile products versus column products, and (3) assimilating multispectral and joint retrievals versus assimilating individual products separately. We use the Community Atmosphere Model with chemistry with the Data Assimilation Research Testbed (CAM-chem+DART) to assimilate different MOPITT carbon monoxide (CO) products to address these three questions. Both anthropogenic and fire CO emissions are optimized in the data assimilation experiments. The results are compared with independent CO observations from TROPOspheric Monitoring Instrument (TROPOMI), the Total Carbon Column Observing Network (TCCON), NOAA Carbon Cycle Greenhouse Gases (CCGG) sites, In-service Aircraft for a Global Observing System (IAGOS), and Western wildfire Experiment for Cloud chemistry, Aerosol absorption and Nitrogen (WE-CAN). We find that (1) assimilating the MOPITT joint (multispectral; near-IR and thermal IR) column product leads to better model–observation agreement at and near the surface than assimilating the MOPITT thermal-IR-only column retrieval. (2) Assimilating column products has a larger impact and improvement for background and large-scale CO compared to assimilating profile products due to vertical localization in profile assimilation. However, profile assimilation can outperform column assimilations in fire-impacted regions and near the surface. (3) Assimilating multispectral and joint products results in similar or slightly better agreement with observations compared to assimilating the single spectral products separately.

Temporal variability of atmospheric columnar CO2, CH4, CO and N2O concentrations using ground-based remote sensing FTIR Spectrometer

Solar absorption spectra collected using a ground-based Fourier Transform Infrared (FTIR) Spectrometer were used to retrieve the column-averaged concentrations (X) of CO2, CH4, CO, and N2O during the years 2016–2019 in the Suburban region of Shadnagar, Telangana, India. For the research period, the diurnal mean amplitudes of XCO2, XCH4, XCO, and XN2O are ∼ 13 ppmv, ∼50 ppbv, ∼13 ppbv, and ∼ 19 ppbv respectively. Strong seasonality at the study site is indicated by the seasonal variations of XCO2 and XCO of 18.3 ppmv and 39.2 ppbv, respectively. Additionally, we compared FTIR data to XCO2 detected by Orbiting Carbon Observatory-2 (OCO-2) and CO columns from Measurements of Pollution in the Troposphere (MOPITT). For the XCO2 and CO columns, the comparison research shows a mean relative bias between FTIR data and satellite data of 0.92 % and 0.71 %, respectively. The FTIR and satellite data show a Pearson correlation coefficient (r) of 0.71 (XCO2, N = 26 co-located) and 0.60 (CO columns, N = 44), respectively. The findings demonstrate a good agreement between our data and satellite data.

The capabilities of the adjoint of GEOS-Chem model to support HEMCO emission inventories and MERRA-2 meteorological data

Abstract. The adjoint of the GEOS-Chem (Goddard Earth Observing System with Chemistry) model has been widely used to constrain the sources of atmospheric compositions. Here, we designed a new framework to facilitate emission inventory updates in the adjoint of the GEOS-Chem model. The major advantage of this new framework is good readability and extensibility, which allows us to support Harmonized Emissions Component (HEMCO) emission inventories conveniently and to easily add more emission inventories following future updates in GEOS-Chem forward simulations. Furthermore, we developed new modules to support MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) meteorological data, which allows us to perform long-term analyses with consistent meteorological data for the period 1979–present. The performances of the developed capabilities were evaluated with the following steps: (1) diagnostic outputs of carbon monoxide (CO) sources and sinks to ensure the correct reading and use of emission inventories, (2) forward simulations to compare the modeled surface and column CO concentrations among various model versions, (3) backward simulations to compare adjoint gradients of global CO concentrations to CO emissions with finite-difference gradients, and (4) observing system simulation experiments (OSSEs) to evaluate the model performance in 4D variational (4D-Var) assimilations. Finally, an example application of 4D-Var assimilation was presented to constrain anthropogenic CO emissions in 2015 by assimilating Measurement of Pollution in the Troposphere (MOPITT) CO observations. The capabilities developed in this work are important for better applications of the adjoint of the GEOS-Chem model in the future. These capabilities will be submitted to the standard GEOS-Chem adjoint code base for better development of the community of the adjoint of the GEOS-Chem model.

Application of the Multi-Scale Infrastructure for Chemistry and Aerosols version 0 (MUSICAv0) for air quality research in Africa

Abstract. The Multi-Scale Infrastructure for Chemistry and Aerosols Version 0 (MUSICAv0) is a new community modeling infrastructure that enables the study of atmospheric composition and chemistry across all relevant scales. We develop a MUSICAv0 grid with Africa refinement (∼ 28 km × 28 km over Africa). We evaluate the MUSICAv0 simulation for 2017 with in situ observations and compare the model results to satellite products over Africa. A simulation from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), a regional model that is widely used in Africa studies, is also included in the analyses as a reference. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Both models underestimate carbon monoxide (CO) compared to in situ observations and satellite CO column retrievals from the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument. MUSICAv0 tends to overestimate ozone (O3), likely due to overestimated stratosphere-to-troposphere flux of ozone. Both models significantly underestimate fine particulate matter (PM2.5) at two surface sites in East Africa. The MUSICAv0 simulation agrees better with aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric nitrogen dioxide (NO2) column retrievals from the Ozone Monitoring Instrument (OMI) than WRF-Chem. MUSICAv0 has a consistently lower tropospheric formaldehyde (HCHO) column than OMI retrievals. Based on model–satellite discrepancies between MUSICAv0 and WRF-Chem and MOPITT CO, MODIS AOD, and OMI tropospheric NO2, we find that future field campaign(s) and more in situ observations in the East African region (5∘ S–5∘ N, 30–45∘ E) could substantially improve the predictive skill of atmospheric chemistry model(s). This suggested focus region exhibits the largest model–in situ observation discrepancies, as well as targets for high population density, land cover variability, and anthropogenic pollution sources.

Global Scale Inversions from MOPITT CO and MODIS AOD

Top-down observational constraints on emissions flux estimates from satellite observations of chemical composition are subject to biases and errors stemming from transport, chemistry and prior emissions estimates. In this context, we developed an ensemble data assimilation system to optimize the initial conditions for carbon monoxide (CO) and aerosols, while also quantifying the respective emission fluxes with a distinct attribution of anthropogenic and wildfire sources. We present the separate assimilation of CO profile v9 retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument and Aerosol Optical Depth (AOD), collection 6.1, from the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. This assimilation system is built on the Data Assimilation Research Testbed (DART) and includes a meteorological ensemble to assimilate weather observations within the online Community Atmosphere Model with Chemistry (CAM-chem). Inversions indicate an underestimation of CO emissions in CAMS-GLOB-ANT_v5.1 in China for 2015 and an overestimation of CO emissions in the Fire INventory from NCAR (FINN) version 2.2, especially in the tropics. These emissions increments are consistent between the MODIS AOD and the MOPITT CO-based inversions. Additional simulations and comparison with in situ observations from the NASA Atmospheric Tomography Mission (ATom) show that biases in hydroxyl radical (OH) chemistry dominate the CO errors.

Adoption of cleaner technologies and reduction in fire events in the hotspots lead to global decline in carbon monoxide

Carbon Monoxide (CO) is not a greenhouse gas (GHG), but has the capacity to change atmospheric chemistry of other GHGs such as methane and ozone, and therefore indirectly affects Earth's radiative forcing of the GHGs and surface temperature. Here, we use the CO mixing ratio at 850 hPa from the Tropospheric Emission Spectrometer (TES) reanalysis and the Measurement of Pollution in the Troposphere (MOPITT) satellite measurements for the period 2005–2019 to examine the spatio-temporal changes in CO across the latitudes. We find a substantial decrease in global CO, about −0.21 ± 0.09 ppb/yr (−0.23 ± 0.12%/yr) with the TES data and about −0.36 ± 0.07 ppb/yr (−0.45 ± 0.08%/yr) with the MOPITT satellite measurements during the study period. The highest CO decreasing trend is observed in Eastern China (−2.7 ± 0.37 ppb/yr) followed by Myanmar (−2.142 ± 0.59 ppb/yr) and South America (−1.08 ± 0.82 ppb/yr). This negative trend in CO is primarily due to the decrease in biomass burning and stringent environmental regulations in the respective regions and countries. The sources including road transport, which account for about 33.6% of CO emissions, followed by industries (18.3%) and agricultural waste burning (8.8%), might also be responsible for the reduction in CO due to the adaptation of improved emission control technology and regulations in the past decades from 2005 to 2019. Therefore, the study provides new insights on the current trends of global CO distribution and reasons for recent reduction in global CO emissions, which would be useful for future decision-making process to control air pollution.

Anomalies of O3, CO, C2H2, H2CO, and C2H6 detected with multiple ground-based Fourier-transform infrared spectrometers and assessed with model simulation in 2020: COVID-19 lockdowns versus natural variability

Anomalies of tropospheric columns of ozone (O3), carbon monoxide (CO), acetylene (C2H2), formaldehyde (H2CO), and ethane (C2H6) are quantified during the 2020 stringent COVID-19 world-wide lockdown using multiple ground-based Fourier-transform infrared spectrometers covering urban and remote conditions. We applied an exponential smoothing forecasting approach to the data sets to estimate business-as-usual values for 2020, which are then contrasted with actual observations. The Community Atmosphere Model with chemistry (CAM-chem) is used to simulate the same gases using lockdown-adjusted and business-as-usual emissions. The role of meteorology, or natural variability, is assessed with additional CAM-chem simulations. The tropospheric column of O3 declined between March and May 2020 for most sites with a mean decrease of 9.2% ± 4.7%. Simulations reproduce these anomalies, especially under background conditions where natural variability explains up to 80% of the decline for sites in the Northern Hemisphere. While urban sites show a reduction between 1% and 12% in tropospheric CO, the remote sites do not show a significant change. Overall, CAM-chem simulations capture the magnitude of the anomalies and in many cases natural variability and lockdowns have opposite effects. We further used the long-term record of the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument to capture global anomalies of CO. Reductions of CO vary highly across regions but North America and Europe registered lower values in March 2020. The absence of CO reduction in April and May, concomitant with reductions of anthropogenic emissions, is explained by a negative anomaly in the hydroxyl radical (OH) found with CAM-chem. The implications of these findings are discussed for methane (CH4), which shows a positive lifetime anomaly during the COVID-19 lockdown period. The fossil fuel combustion by-product tracer C2H2 shows a mean drop of 13.6% ± 8.3% in urban Northern Hemisphere sites due to the reduction in emissions and in some sites exacerbated by natural variability. For some sites with anthropogenic influence there is a decrease in C2H6. The simulations capture the anomalies but the main cause may be related to natural variability. H2CO declined during the stringent 2020 lockdown in all urban sites explained by reductions in emissions of precursors.

Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model

Abstract. We explore the sensitivity of modeled tropospheric hydroxyl (OH) concentration trends to meteorology and near-term climate forcers (NTCFs), namely methane (CH4) nitrogen oxides (NOx=NO2+NO) carbon monoxide (CO), non-methane volatile organic compounds (NMVOCs) and ozone-depleting substances (ODSs), using the Geophysical Fluid Dynamics Laboratory (GFDL)'s atmospheric chemistry–climate model, the Atmospheric Model version 4.1 (AM4.1), driven by emissions inventories developed for the Sixth Coupled Model Intercomparison Project (CMIP6) and forced by observed sea surface temperatures and sea ice prepared in support of the CMIP6 Atmospheric Model Intercomparison Project (AMIP) simulations. We find that the modeled tropospheric air-mass-weighted mean [OH] has increased by ∼5 % globally from 1980 to 2014. We find that NOx emissions and CH4 concentrations dominate the modeled global trend, while CO emissions and meteorology were also important in driving regional trends. Modeled tropospheric NO2 column trends are largely consistent with those retrieved from the Ozone Monitoring Instrument (OMI) satellite, but simulated CO column trends generally overestimate those retrieved from the Measurements of Pollution in The Troposphere (MOPITT) satellite, possibly reflecting biases in input anthropogenic emission inventories, especially over China and South Asia.

Transport pathways of carbon monoxide from Indonesian fire pollution to a subtropical high-altitude mountain site in the western North Pacific

Abstract. Dry conditions associated with the El Niño–Southern Oscillation (ENSO) and a positive Indian Ocean Dipole (IOD) are known to have caused major fire pollution events and intense carbon emissions over a vast spatial expanse of Indonesia in October 2006 and 2015. During these two events, a substantial increase in the carbon monoxide (CO) mixing ratio was detected by in situ measurements at Lulin Atmospheric Background Station (LABS; 23.47∘ N 120.87∘ E; 2862 ma.s.l.) in Taiwan, which is the only background station in the subtropical western North Pacific region. Compared to the long-term October mean (2006–2021), CO was elevated by ∼ 47.2 ppb (parts per billion; 37.2 %) and ∼ 36.7 ppb (28.9 %) in October 2006 and 2015, respectively. This study delineates plausible pathways for the CO transport from Indonesia to LABS using Measurement of Pollution in the Troposphere (MOPITT) CO observations and Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis products (winds and geopotential height – GpH). Two simultaneously occurring transport pathways were identified, namely (i) horizontal transport in the free troposphere and (ii) vertical transport through the Hadley circulation (HC). The GpH analysis of both events revealed the presence of a high-pressure anticyclone over the northern part of the South China Sea (SCS), which played an important role in the free-tropospheric horizontal transport of CO. In this scenario, CO in the free troposphere is transported on the western edge of the high-pressure system and then driven by subtropical westerlies to LABS. Simultaneously, uplifted CO over Indonesia can enter the HC and be transferred to subtropical locations such as LABS. The vertical cross section of the MOPITT CO and MERRA-2 vertical pressure velocity supported the transport of CO through the HC. Furthermore, the results revealed a distinct HC strength in two events (higher in 2006 compared to 2015) due to the different ENSO conditions. Overall, the present findings can provide some insights into understanding the regional transport of pollution over Southeast Asia and the role of climate conditions on transport pathways.

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.

Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data

Abstract. Column mixing ratio of carbon dioxide (CO2) data alone do not provide enough information for source attribution. Carbon monoxide (CO) is a product of inefficient combustion often co-emitted with CO2. CO data can then provide a powerful constraint on fire emissions, supporting more accurate estimation of biospheric CO2 fluxes. In this framework and using the chemistry transport model TM5, a CO inversion using Measurements of Pollution in The Troposphere (MOPITT) v8 data is performed to estimate fire emissions which are then converted into CO2 fire emissions (called FIREMo) through the use of the emission ratio. These optimized CO2 fire emissions are used to rebalance the CO2 net ecosystem exchange (NEEMo) and respiration (RhMo) with the global CO2 growth rate. Subsequently, in a second step, these rebalanced fluxes are used as priors for a CO2 inversion to derive the NEE and ocean fluxes constrained either by the Orbiting Carbon Observatory 2 (OCO-2) v9 or by in situ (IS) CO2 data. For comparison purpose, we also balanced the respiration using fire emissions from the Global Fire Emissions Database (GFED) version 3 (GFED3) and version 4.1s (GFED4.1s). We hence study the impact of CO fire emissions in our CO2 inversions at global, latitudinal, and regional scales over the period 2015–2018 and compare our results to the two other similar approaches using GFED3 (FIRE3) and GFED4.1s (FIRE4) fires, as well as with an inversion using both Carnegie–Ames–Stanford Approach (CASA)-GFED3 NEE and GFED3 fire priors (priorCMS). After comparison at the different scales, the inversions are evaluated against Total Carbon Column Observing Network (TCCON) data. Comparison of the flux estimates shows that at the global scale posterior net flux estimates are more robust than the different prior flux estimates. However, at the regional scale, we can observe differences in fire emissions among the priors, resulting in differences among the NEE prior emissions. The derived NEE prior emissions are rebalanced in concert with the fires. Consequently, the differences observed in the NEE posterior emissions are a result of the balancing with fires and the constraints provided by CO2 observations. Tropical net flux estimates from in situ inversions are highly sensitive to the prior flux assumed, of which fires are a significant component. Slightly larger net CO2 sources are derived with posterior fire emissions using either FIRE4 or FIREMo in the OCO-2 inversion, in particular for most tropical regions during the 2015 El Niño year. Similarly, larger net CO2 sources are also derived with posterior fire emissions in the in situ data inversion for Tropical Asia. Evaluation with CO2 TCCON data shows lower biases with the three rebalanced priors than with the prior using CASA-GFED3. However, posteriors have average bias and scatter very close each other, making it difficult to conclude which simulation performs better than the other. We observe that the assimilated CO2 data have a strong influence on the global net fluxes among the different inversions. Inversions using OCO-2 (or IS) data have similar emissions, mostly as a result of the observational constraints and to a lesser extent because of the fire prior used. But results in the tropical regions suggest net flux sensitivity to the fire prior for both the IS and OCO-2 inversions. Further work is needed to improve prior fluxes in tropical regions where fires are a significant component. Finally, even if the inversions using the FIREMo prior did enhance the biases over some TCCON sites, it is not the case for the majority of TCCON sites. This study consequently pushes forward the development of a CO–CO2 joint inversion with multi-observations for a possible stronger constraint on posterior CO2 fire and biospheric emissions.

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.

Evaluation of WRF-chem simulations of NO2 and CO from biomass burning over East Africa and its surrounding regions

In East Africa, biomass burning in the savanna region emits nitrogen dioxide (NO2), carbon monoxide (CO), and aerosols among other species. These emissions are dangerous air pollutants which pose a health risk to the population. They also affect the radiation budget. Currently, limited academic research has been done to study their spatial and temporal distribution over this region by means of numerical modeling. This study therefore used the Weather Research and Forecasting model coupled with chemistry (WRF-chem) to simulate, for the first time, the distribution of NO2 during the year 2012 and CO during the period June 2015 to May 2016 over this region. These periods had the highest atmospheric abundances of these species. The model’s performance was evaluated against satellite observations from the Ozone Monitoring Instrument (OMI) and the Measurement of Pollution in the Troposphere (MOPITT). Three evaluation metrics were used, these were, the normalized mean bias (NMB), the root mean square error (RMSE) and Pearson’s correlation coefficient (R). Further, an attempt was made to reduce the bias shown by WRF-chem by applying a deep convolutional autoencoder (WRF-DCA) algorithm and linear scaling (WRF-LS). The results showed that WRF-chem simulated the seasonality of the gases but made below adequate estimates of the gas abundances. It overestimated NO2 and underestimated CO throughout all the seasons. Overall, for NO2, WRF-chem had an average NMB of 3.51, RMSE of 2 × 1015 molecules/cm2 and R of 0.44 while for CO, it had an average NMB of − 0.063, RMSE of 0.65 × 1018 molecules/cm2 and R of 0.13. Furthermore, even though both WRF-DCA and WRF-LS successfully reduced the bias in WRF-chem’s NO2 estimates, WRF-DCA had a superior performance compared to WRF-LS. It reduced the NMB by an average of 3.2 (90.2%). Finally, this study has shown that deep learning has a strong ability to improve the estimates of numerical models, and this can be a cue to incorporate this approach along other stages of the numerical modeling process.

Evaluation of MOPITT and TROPOMI carbon monoxide retrievals using AirCore in situ vertical profiles

Abstract. AirCore in situ vertical profiles sample the atmosphere from near the surface to the lower stratosphere, making them ideal for the validation of satellite tropospheric trace gas data. Here we present intercomparison results of AirCore carbon monoxide (CO) measurements with respect to retrievals from MOPITT (Measurements of Pollution In The Troposphere; version 8) and TROPOMI (TROPOspheric Monitoring Instrument), on board the NASA Terra and ESA Sentinel 5-Precursor satellites, respectively. Mean MOPITT/AirCore total column bias values and their standard deviation (0.4 ± 5.5, 1.7 ± 5.6, and 0.7 ± 6.0 for MOPITT thermal-infrared, near-infrared, and multispectral retrievals, respectively; all in %) are similar to results obtained in MOPITT/NOAA aircraft flask data comparisons from this study and from previous validation efforts. MOPITT CO retrievals are systematically validated using in situ vertical profiles from a variety of aircraft campaigns. Because most aircraft vertical profiles do not sample the troposphere's entire vertical extent, they must be extended upwards in order to be usable in validation. Here we quantify, for the first time, the error introduced in MOPITT CO validation by the use of shorter aircraft vertical profiles extended upwards by analyzing validation results of MOPITT with respect to full and truncated AirCore CO vertical profiles. Our results indicate that the error is small, affects mostly upper tropospheric retrievals (at 300 hPa: ∼ 2.6, 0.8, and 3.2 percent points for MOPITT thermal-infrared, near-infrared, and multispectral, respectively), and may have resulted in the overestimation of MOPITT retrieval biases in that region. TROPOMI can retrieve CO under both clear and cloudy conditions. The latter is achieved by quantifying interfering trace gases and parameters describing the cloud contamination of the measurements together with the CO column; then, the reference CO profiles used in the retrieval are scaled based on estimated above-cloud CO rather than on estimated total CO. We use AirCore measurements as the reference to evaluate the error introduced by this approach in cloudy TROPOMI retrievals over land after accounting for TROPOMI's vertical sensitivity to CO (relative bias and its standard deviation = 2.02 % ± 11.13 %). We also quantify the null-space error, which accounts for differences between the shape of TROPOMI reference profiles and that of AirCore measured profiles (for TROPOMI cloudy enull=0.98 % ± 2.32 %).