Comment on gmd-2023-4

Scaling relationship between CO pollution and population size over major US metropolitan statistical areas

Long-term trend analysis of CO in the Yongsan district of Seoul, Korea, between the years 1987 and 2013

Abstract. The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument has been measuring global tropospheric carbon monoxide (CO) since March 2000, providing the longest nearly continuous record of CO from space. During its long mission, the data processing algorithms have been updated to improve the quality of CO retrievals and the sensitivity to the lower troposphere. Currently, MOPITT retrievals are only performed for clear-sky observations or over low clouds for ocean scenes. The cloud detection scheme was modified in the new V9 product, resulting in an improvement in observational coverage, especially over land. Comparison of the spatial and seasonal variations of the data coverage in V9 and V8 shows differences with significant geographical and temporal variability, with some regions such as Canada and the Amazon exhibiting a doubling of data in winter. Here we conducted an analysis of Moderate Resolution Imaging Spectroradiometer (MODIS) cloud heights and cloud mask products along with MOPITT retrieval cloud flag descriptors to understand the impact of cloud conditions on the MOPITT observational coverage, with a particular focus on observations over Canada. The MOPITT CO total column (TC) data were modified by turning off the cloud detection scheme to allow for a CO retrieval result, regardless of their cloud status. Analyses of the standard V8 CO TC product (cloud filtered) and non-standard product (non-cloud-masked) were conducted for selected days. Results showed some coherent structures that were observed frequently in the non-masked CO product that was not present in the V8 product and could potentially be actual CO features. Many times, these CO plumes were also seen in the Infrared Atmospheric Sounding Interferometer (IASI) CO TC product. The MODIS cloud height analysis revealed that a significant number of low-cloud CO retrievals were discarded in the V8 product. Most of the missed CO plumes in the V8 product are now detected in the new V9 product as a result of the dependence of the MOPITT radiance ratio (MRT) test over land. Comparisons of the MRT and MODIS cloud height data indicate a remarkable negative correlation. As a result of the modified V9 cloud detection algorithm, a significant portion of the low-cloud CO retrievals is now incorporated in the new V9 MOPITT product. Consequently, the observational coverage over Canada is significantly improved, which benefits analyses of regional CO variability, especially during extreme pollution events. We also conducted a comparison of MOPITT and IASI CO TC and found generally good agreement, with about a 5 %–10 % positive bias that is more pronounced in highly polluted scenes.

Abstract. Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL (Geophysical Fluid Dynamics Laboratory) standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100 yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern midlatitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.

Fire emissions are a major contributor to atmospheric composition, affecting atmospheric oxidizing capacity and air quality. Transported amounts from Northern Hemisphere boreal fires can reach the pristine Arctic atmosphere as well as impact air quality in populated regions. Carbon monoxide (CO) is a useful trace gas emitted from fires that can be used to link extreme fire events with climate variability. We use our recently developed statistical tool to investigate the climate drivers of satellite measured CO variability in two Northern Hemisphere boreal fire regions: northwest Canada and Siberia. Our focus is on quantifying the ability of climate mode indices for the Pacific, Atlantic, Indian and Arctic Oceans in predicting CO amounts in these regions. Climate mode indices El Niño Southern Oscillation (ENSO), Tropical North Atlantic (TNA), the Dipole Mode Index (DMI) and the Arctic Oscillation (AO) are used to develop statistical models of column CO interannual variability from the Measurements of Pollution In The Troposphere (MOPITT) satellite instrument, for the time period covering 2001-2017. In addition, we assess the ability of fire emission inventories to reproduce CO, including the Fire Inventory from NCAR (FINN), the NASA Quick Fire Emissions Dataset (QFED) and the Copernicus Atmosphere Monitoring Service (CAMS) Global Fire Assimilation System (GFAS). These are implemented in the NCAR Community Atmosphere Model with chemistry (CAM-chem) and subsequently evaluated against MOPITT CO observations. Emission uncertainty contribution to inter-inventory differences are quantified, and the modeled contribution of fires to CO interannual variability is determined.

The multi‐year retrievals of carbon monoxide (CO) by the MOPITT (Measurements Of Pollution In The Troposphere) instrument onboard the NASA Terra satellite provide an opportunity for the first time to study quantitatively the transport and sources of pollution in the mid‐troposphere. This paper presents the assimilation of the Phase I (March 3, 2000–May 6, 2001) MOPITT retrievals with optimized CO emissions constrained by monthly MOPITT CO data. The observed‐minus‐forecast (OmF) CO distributions illustrate improvement of this data analysis compared with the assimilation that employs climatological surface fluxes.

Carbon monoxide (CO) plays an important role in both air quality and climate. Photochemical oxidation of CO produces ozone (O3) and carbon dioxide (CO2) while also affecting the lifetime of methane (CH4) through reactions with the hydroxyl radical (OH). Because CO2, CH4 and O3 are greenhouse gases, emissions of CO have an indirect radiative forcing, estimated at 0.22 W/m2. Ground-level O3 and CO are also air pollutants that affect human and ecosystem health. Quantifying trends in carbon monoxide is essential for understanding trends in tropospheric ozone, especially in background regions. Using the 22-year data record from MOPITT (Measurements of Pollution In The Troposphere), we show global and regional trends from satellite observations of atmospheric CO. We also examine trends in CO emissions based on model inversions for CO emitted by biomass burning (BB) and fossil fuels (FF) and from chemical production from emissions of biogenic (BG) VOCs (volatile organic compounds). We find that CO concentrations and CO emissions from BB and FF have been mostly decreasing globally, with some notable regional exceptions.

Abstract. East Asia has experienced rapid development with increasing carbon monoxide (CO) emission in the past decades. Therefore, uplifting CO from the boundary layer to the free troposphere in East Asia can have great implications on regional air quality around the world. It can also influence global climate due to the longer lifetime of CO at higher altitudes. In this study, three cases of high CO episodes in the East China Sea and the Sea of Japan from 2003 to 2005 are examined with spaceborne Measurements of Pollution in the Troposphere (MOPITT) data, in combination with aircraft measurements from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. High CO abundances of 300–550 ppbv are observed in MOZAIC data in the free troposphere during these episodes. These are among the highest CO abundances documented at these altitudes. On average, such episodes with CO over 400 ppbv (in the 2003 and 2004 cases) and between 200 and 300 ppbv (in the 2005 case) may occur 2–5 and 10–20% in time, respectively, in the respective altitudes over the region. Correspondingly, elevated CO is shown in MOPITT daytime data in the middle to upper troposphere in the 2003 case, in the lower to middle troposphere in the 2004 case, and in the upper troposphere in the 2005 case. Through analyses of the simulations from a chemical transport model GEOS-Chem and a trajectory dispersion model FLEXPART, we found different CO signatures in the elevated CO and distinct transport pathways and mechanisms for these cases. In the 2003 case, emissions from large forest fires near Lake Baikal dominated the elevated CO, which had been rapidly transported upward by a frontal system from the fire plumes. In the 2004 case, anthropogenic CO from the North China Plain experienced frontal lifting and mostly reached ~ 700 hPa near the East China Sea, while CO from biomass burning over Indochina experienced orographic lifting, lee-side-trough-induced convection, and frontal lifting through two separate transport pathways, leading to two distinct CO enhancements around 700 and 300 hPa. In the 2005 case, the observed CO of ~ 300 ppbv around 300 hPa originated from anthropogenic sources over the Sichuan Basin and the North China Plain and from forest fires over Indochina. The high CO was transported to such altitudes through strong frontal lifting, interacting with convection and orographic lifting. These cases show that topography affects vertical transport of CO in East Asia via different ways, including orographic uplifting over the Hengduan Mountains, assisting frontal lifting in the North China Plain, and facilitating convection in the Sichuan Basin. In particular, topography-induced lee-side troughs over Indochina led to strong convection that assisted CO uplifting to the upper troposphere. This study shows that the new daytime MOPITT near-infrared (NIR) and thermal-infrared (TIR) data (version 5 or above) have enhanced vertical sensitivity in the free troposphere and may help qualitative diagnosis of vertical transport processes in East Asia.

Inverse modeling can provide valuable insights into the sources of atmospheric tracers based on observations and a set of boundary conditions. However, biases in these boundary conditions can lead to biases in the optimized emissions. In this study, we present a series of global inversion experiments of carbon monoxide (CO) emissions using the TM5-4dvar inverse modeling suit constrained by satellite data from the TROPOspheric Monitoring Instrument (TROPOMI) and surface flask measurements from NOAA. These experiments are designed to systematically assess the impact of different boundary conditions, with a particular focus on hydroxyl radical (OH) distributions, a key determinant of both the sources and sinks of CO.Methyl chloroform (MCF) measurements are commonly used to constrain global atmospheric OH climatological fields. We find that our OH fields that are modeled with global atmospheric chemistry calculations are biased high. Despite this bias, these OH fields often provide more realistic lateral distributions than climatological OH fields, particularly in the tropical boundary layer. Another critical boundary condition for inverse modeling of CO is its secondary production from Volatile Organic Compounds (VOCs) and methane. Due to the challenges of directly measuring secondary CO production, model-based estimates are used instead.Our results show that combining modeled secondary CO production estimates with modeled OH fields leads to a closed budget, reducing aliasing across emission categories and enhancing confidence in the optimized anthropogenic and biomass burning emissions. Although the individual budget terms of both the secondary production and the chemical loss of CO may be overestimated, their combined effect yields realistic steady-state CO mixing ratios, as validated by TROPOMI CO observations. This study emphasizes the critical need for improved OH fields to accurately estimate CO emissions, and advances the understanding of potential biases in future inversions.

<strong class="journal-contentHeaderColor">Abstract.</strong> 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 &times; 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 (PM_2.5) 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 an East African region (30&deg; E &ndash; 45&deg; E, 5&deg; S &ndash; 5&deg; N) 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.

Analysis of carbon monoxide budget in North China

Air pollution trends measured from Terra: CO and AOD over industrial, fire-prone, and background regions

Abstract. The MOPITT (Measurements of Pollution in the Troposphere) satellite instrument has been making nearly continuous observations of atmospheric carbon monoxide (CO) since 2000. Satellite observations of CO are routinely used to analyze emissions from fossil fuels and biomass burning, as well as the atmospheric transport of those emissions. Recent enhancements to the MOPITT retrieval algorithm have resulted in the release of the version 8 (V8) product. V8 products benefit from updated spectroscopic data for water vapor and nitrogen used to develop the operational radiative transfer model and exploit a new method for minimizing retrieval biases through parameterized radiance bias correction. In situ datasets used for algorithm development and validation include the NOAA (National Oceanic and Atmospheric Administration) and HIPPO (HIAPER Pole-to-Pole Observations) datasets used for earlier MOPITT validation work in addition to measurements from the ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems – Cloud processes of the main precipitation systems in Brazil: A contribution to cloud resolving modeling and to the GPM (Global Precipitation Measurement)), KORUS-AQ (The Korea-United States Air Quality Study), and ATom (The Atmospheric Tomography Mission) programs. Validation results illustrate clear improvements with respect to long-term bias drift and geographically variable retrieval bias. For example, whereas bias drift for the V7 thermal-infrared (TIR)-only product exceeded 0.5 % yr−1 for levels in the upper troposphere (e.g., at 300 hPa), bias drift for the V8 TIR-only product is found to be less than 0.1 % yr−1 at all levels. Also, whereas upper-tropospheric (300 hPa) retrieval bias in the V7 TIR-only product exceeded 10 % in the tropics, corresponding V8 biases are less than 5 % (in terms of absolute value) at all latitudes and do not exhibit a clear latitudinal dependence.

Abstract. We analyse the carbon monoxide (CO), ethane (C2H6) and hydrogen cyanide (HCN) partial columns (from the ground to 12 km) derived from measurements by ground-based solar Fourier Transform Spectroscopy at Lauder, New Zealand (45° S, 170° E), and at Arrival Heights, Antarctica (78° S, 167° E), from 1997 to 2009. Significant negative trends are calculated for all species at both locations, based on the daily-mean observed time series, namely CO (−0.94 ± 0.47% yr−1), C2H6 (−2.37 ± 1.18% yr−1) and HCN (−0.93 ± 0.47% yr−1) at Lauder and CO (−0.92 ± 0.46% yr−1), C2H6 (−2.82 ± 1.37% yr−1) and HCN (−1.41 ± 0.71% yr−1) at Arrival Heights. The uncertainties reflect the 95% confidence limits. However, the magnitudes of the trends are influenced by the anomaly associated with the 1997–1998 El Niño Southern Oscillation event at the beginning of the time series reported. We calculate trends for each month from 1997 to 2009 and find negative trends for all months. The largest monthly trends of CO and C2H6 at Lauder, and to a lesser degree at Arrival Heights, occur during austral spring during the Southern Hemisphere tropical and subtropical biomass burning period. For HCN, the largest monthly trends occur in July and August at Lauder and around November at Arrival Heights. The correlations between CO and C2H6 and between CO and HCN at Lauder in September to November, when the biomass burning maximizes, are significantly larger that those in other seasons. A tropospheric chemistry-climate model is used to simulate CO, C2H6, and HCN partial columns for the period of 1997–2009, using interannually varying biomass burning emissions from GFED3 and annually periodic but seasonally varying emissions from both biogenic and anthropogenic sources. The model-simulated partial columns of these species compare well with the measured partial columns and the model accurately reproduces seasonal cycles of all three species at both locations. However, while the model satisfactorily captures both the seasonality and trends in HCN, it is not able to reproduce the negative trends in either C2H6 or CO. A further simulation assuming a 35% decline of C2H6 and a 26% decline of CO emissions from the industrial sources from 1997 to 2009 largely captures the observed trends of C2H6 and CO partial columns at both locations. Here we attribute trends in HCN exclusively to changes in biomass burning and thereby isolate the influence of anthropogenic emissions as responsible for the long-term decline in CO and C2H6. This analysis shows that biomass burning emissions are the main factors in controlling the interannual and seasonal variations of these species. We also demonstrate contributions of biomass burning emission from different southern tropical and sub-tropical regions to seasonal and interannual variations of CO at Lauder; it shows that long-range transport of biomass burning emissions from southern Africa and South America have consistently larger year-to-year contributions to the background seasonality of CO at Lauder than those from other regions (e.g. Australia and South-East Asia). However, large interannual anomalies are triggered by variations in biomass burning emissions associated with large-scale El Niño Southern Oscillation and prolonged biomass burning events, e.g. the Australian bush fires.

Satellite estimates of burned area, associated carbon monoxide (CO) emission estimates, and CO column retrievals do not agree on the peak fire month in Africa, evident in both Northern and Southern Africa though distinct in the burning seasonality. Here we analyze this long‐standing problem using (1) a top‐down Bayesian inversion of Measurements Of Pollution In The Troposphere CO columns during 2005–2016 into surface CO emissions and (2) the bottom‐up Global Fire Emissions Database 4.1 s. We show that Global Fire Emissions Database 4.1 s underestimates CO emissions by 12–62% in the late fire season and hypothesize that this is partly because it assumes seasonally static emission factors. However, the degree to which emission factors would have to vary through the season to bring top‐down and bottom‐up in agreement cannot be confirmed by past field‐based measurements. Improved observational constraint on the seasonality of burned area, fuel combustion, and emission factors would further reduce the discrepancy between bottom‐up and top‐down emission estimates.