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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.

Abstract. The applications of novel deep learning (DL) techniques in atmospheric science are rising quickly. Here we build a hybrid DL model (hyDL-CO), based on convolutional neural networks (CNNs) and long short-term memory (LSTM) neural networks, to provide a comparative analysis between DL and Kalman filter (KF) to predict carbon monoxide (CO) concentrations in China in 2015–2020. We find the performance of DL model is better than KF in the training period (2015–2018): the mean bias and correlation coefficients are 9.6 ppb and 0.98 over eastern China and are −12.5 ppb and 0.96 over grids with independent observations (i.e., grids with CO observations that are not used in DL training and KF assimilation). By contrast, the assimilated CO concentrations by KF exhibit comparable correlation coefficients but larger negative biases. Furthermore, the DL model demonstrates good temporal extensibility in the test period (2019–2020): the mean bias and correlation coefficients are 95.7 ppb and 0.93 over eastern China and 81.0 ppb and 0.91 over grids with independent observations, while CO observations are not fed into the DL model as an input variable. Despite these advantages, we find a weaker prediction capability of the DL model than KF in the test period, and a noticeable underestimation of CO concentrations at extreme pollution events in the DL model. This work demonstrates the advantages and disadvantages of DL models to predict atmospheric compositions with respect to traditional data assimilation, which is helpful for better applications of this novel technique in future studies.

Abstract. Nitrogen dioxide (NO2) column density measurements from satellites have been widely used in constraining emissions of nitrogen oxides (NOx = NO + NO2). However, the utility of these measurements is impacted by reduced observational coverage due to cloud cover and their reduced sensitivity toward the surface. Combining the information from satellites with surface observations of NO2 will provide greater constraints on emission estimates of NOx. We have developed a deep-learning (DL) model to integrate satellite data and in situ observations of surface NO2 to estimate NOx emissions in China. A priori information for the DL model was obtained from satellite-derived emissions from the Tropospheric Chemistry Reanalysis (TCR-2). A two-stage training strategy was used to integrate in situ measurements from the China Ministry of Ecology and Environment (MEE) observation network with the TCR-2 data. The DL model is trained from 2005 to 2018 and evaluated for 2019 and 2020. The DL model estimated a source of 19.4 Tg NO for total Chinese NOx emissions in 2019, which is consistent with the TCR-2 estimate of 18.5 ± 3.9 Tg NO and the 20.9 Tg NO suggested by the Multi-resolution Emission Inventory for China (MEIC). Combining the MEE data with TCR-2, the DL model suggested higher NOx emissions in some of the less-densely populated provinces, such as Shaanxi and Sichuan, where the MEE data indicated higher surface NO2 concentrations than TCR-2. The DL model also suggested a faster recovery of NOx emissions than TCR-2 after the Chinese New Year (CNY) holiday in 2019, with a recovery time scale that is consistent with Baidu “Qianxi” mobility data. In 2020, the DL-based analysis estimated about a 30 % reduction in NOx emissions in eastern China during the COVID-19 lockdown period, relative to pre-lockdown levels. In particular, the maximum emission reductions were 42 % and 30 % for the Jing-Jin-Ji (JJJ) and the Yangtze River Delta (YRD) mega-regions, respectively. Our results illustrate the potential utility of the DL model as a complementary tool for conventional data-assimilation approaches for air quality applications.

Uptake of atmospheric carbon by the ocean, especially at high latitudes, plays an important role in offsetting anthropogenic emissions. At the surface of the Southern Ocean south of 30∘S, the ocean carbon uptake, which had been weakening in 1990s, strengthened in the 2000s. However, sparseness of in-situ measurements in the ocean interior make it difficult to compute changes in carbon storage below the surface. Here we develop a machine-learning model, which can estimate concentrations of dissolved inorganic carbon (DIC) in the Southern Ocean up to 4 km depth only using data available at the ocean surface. Our model is fast and computationally inexpensive. We apply it to calculate trends in DIC concentrations over the past three decades and find that DIC decreased in the 1990s and 2000s, but has increased, in particular in the upper ocean since the 2010s. However, the particular circulation dynamics that drove these changes may have differed across zonal sectors of the Southern Ocean. While the near-surface decrease in DIC concentrations would enhance atmospheric CO2 uptake continuing the previously-found trends, weakened connectivity between surface and deep layers and build-up of DIC in deep waters could reduce the ocean’s carbon storage potential.

Air pollution is a major cause of mortality globally (Cohen et al., 2017). In this context, tropospheric ozone is a key pollutant that is produced photochemically by the oxidation of hydrocarbons in the presence of nitrogen oxides (NO x = NO + NO 2 ). Air pollution regulations have resulted in dramatic reductions in emissions of NO x . However, Jiang et al. (2018) suggested that NO x emission estimates inferred from satellite observations (referred to as top-down estimates) indicate that there has been a slowdown in the reduction rate since 2009, compared to the bottom-up emission inventory reported by the US Environmental Protection Agency (EPA) National Emission Inventory (NEI). In contrast, it has been suggested that the slowdown in the reduction rate in the satellite-derived emission estimates does not indicate a discrepancy with the NEI inventory, but instead is due to the increasing relative influence of nonanthropogenic NO x emissions on atmospheric NO x as captured by the satellite measurements (Silvern et al., 2019). It has also been reported by J. Li and Wang (2019) that the satellite-derived trends are consistent with the trends in surface observations of NO 2 in high emission regions and that the discrepancy between the top-down and bottom-up trends are due to nonlinearity in the relationship between NO x emissions and the satellite observations of NO 2 in low emission "rural" regions. Here, we use a data-driven deep learning (DL) model that predicts surface ozone abundances across the US, which allows us to assess the consistency of the inferred 2005-2014 trends in NO x emissions with observed surface ozone.

Abstract. In this study, we present the development of a new coupled weather and greenhouse gas (GHG) data assimilation system based on Environment and Climate Change Canada's (ECCC's) operational Ensemble Kalman Filter (EnKF). The estimated meteorological state is augmented to include three chemical constituents: CO2, CO and CH4. Variable localization is used to prevent the direct update of meteorology by the observations of the constituents and vice versa. Physical localization is used to damp spurious analysis increments far from a given observation. Perturbed flux fields are used to account for the uncertainty in CO due to error in the fluxes. The system is demonstrated for the estimation of 3-dimensional CO states using simulated observations from a variety of networks. First, a hypothetically dense uniformly distributed observation network is used to demonstrate that the system is working. More realistic observation networks based on surface hourly observations, and space-based observations provide a demonstration of the complementarity of the different networks and further confirm the reasonable behaviour of the coupled assimilation system. Having demonstrated the ability to estimate CO distributions, this system will be extended to estimate surface fluxes in the future.

Abstract. In this study, we present the development of a new coupled weather and carbon monoxide (CO) data assimilation system based on the Environment and Climate Change Canada (ECCC) operational ensemble Kalman filter (EnKF). The estimated meteorological state is augmented to include CO. Variable localization is used to prevent the direct update of meteorology by the observations of the constituents and vice versa. Physical localization is used to damp spurious analysis increments far from a given observation. Perturbed surface flux fields are used to account for the uncertainty in CO due to errors in the surface fluxes. The system is demonstrated for the estimation of three-dimensional CO states using simulated observations from a variety of networks. First, a hypothetically dense, uniformly distributed observation network is used to demonstrate that the system is working. More realistic observation networks, based on surface hourly observations, and space-based observations provide a demonstration of the complementarity of the different networks and further confirm the reasonable behavior of the coupled assimilation system. Having demonstrated the ability to estimate CO distributions, this system will be extended to estimate surface fluxes in the future.