Transport Model Errors Research Articles

Greenhouse gas emissions and their trends over the last 3 decades across Africa

Abstract. A key goal of the Paris Agreement (PA) is to reach net-zero greenhouse gas (GHG) emissions by 2050 globally, which requires mitigation efforts from all countries. Africa's rapidly growing population and gross domestic product (GDP) make this continent important for GHG emission trends. In this paper, we study the emissions of carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) in Africa over 3 decades (1990–2018). We compare bottom-up (BU) approaches, including United Nations Convention Framework on Climate Change (UNFCCC) national inventories, FAO, PRIMAP-hist, process-based ecosystem models for CO2 fluxes in the land use, land use change and forestry (LULUCF) sector and global atmospheric inversions. For inversions, we applied different methods to separate anthropogenic CH4 emissions. The BU inventories show that, over the decade 2010–2018, fewer than 10 countries represented more than 75 % of African fossil CO2 emissions. With a mean of 1373 Mt CO2 yr−1, total African fossil CO2 emissions over 2010–2018 represent only 4 % of global fossil emissions. However, these emissions grew by +34 % from 1990–1999 to 2000–2009 and by +31 % from 2000–2009 to 2010–2018, which represents more than a doubling in 30 years. This growth rate is more than 2 times faster than the global growth rate of fossil CO2 emissions. The anthropogenic emissions of CH4 grew by 5 % from 1990–1999 to 2000–2009 and by 14.8 % from 2000–2009 to 2010–2018. The N2O emissions grew by 19.5 % from 1990–1999 to 2000–2009 and by 20.8 % from 2000–2009 to 2010–2018. When using the mean of the estimates from UNFCCC reports (including the land use sector) with corrections from outliers, Africa was a mean source of greenhouse gases of 262221863239 Mt CO2 eq. yr−1 from all BU estimates (the subscript and superscript indicate min–max range uncertainties) and of +263717615873 Mt CO2 eq. yr−1 from top-down (TD) methods during their overlap period from 2001 to 2017. Although the mean values are consistent, the range of TD estimates is larger than the one of the BU estimates, indicating that sparse atmospheric observations and transport model errors do not allow us to use inversions to reduce the uncertainty in BU estimates. The main source of uncertainty comes from CO2 fluxes in the LULUCF sector, for which the spread across inversions is larger than 50 %, especially in central Africa. Moreover, estimates from national UNFCCC communications differ widely depending on whether the large sinks in a few countries are corrected to more plausible values using more recent national sources following the methodology of Grassi et al. (2022). The medians of CH4 emissions from inversions based on satellite retrievals and surface station networks are consistent with each other within 2 % at the continental scale. The inversion ensemble also provides consistent estimates of anthropogenic CH4 emissions with BU inventories such as PRIMAP-hist. For N2O, inversions systematically show higher emissions than inventories, on average about 4.5 times more than PRIMAP-hist, either because natural N2O sources cannot be separated accurately from anthropogenic ones in inversions or because BU estimates ignore indirect emissions and underestimate emission factors. Future improvements can be expected thanks to a denser network of monitoring atmospheric concentrations. This study helps to introduce methods to enhance the scope of use of various published datasets and allows us to compute budgets thanks to recombinations of those data products. Our results allow us to understand uncertainty and trends in emissions and removals in a region of the world where few observations exist and where most inventories are based on default IPCC guideline values. The results can therefore serve as a support tool for the Global Stocktake (GST) of the Paris Agreement. The referenced datasets related to the figures are available at https://doi.org/10.5281/zenodo.7347077 (Mostefaoui et al., 2022).

Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions

Abstract. Inverse modeling is a widely used top-down method to infer greenhouse gas (GHG) emissions and their spatial distribution based on atmospheric observations. The errors associated with inverse modeling have multiple sources, such as observations and a priori emission estimates, but they are often dominated by the transport model error. Here, we utilize the Lagrangian particle dispersion model (LPDM) FLEXPART (FLEXible PARTicle Dispersion Model), driven by the meteorological fields of the regional numerical weather prediction model COSMO. The main sources of errors in LPDMs are the turbulence diffusion parameterization and the meteorological fields. The latter are outputs of an Eulerian model. Recently, we introduced an improved parameterization scheme of the turbulence diffusion in FLEXPART, which significantly improves FLEXPART-COSMO simulations at 1 km resolution. We exploit F-gas measurements from two extended field campaigns on the Swiss Plateau (in Beromünster and Sottens), and we conduct both high-resolution (1 km) and low-resolution (7 km) FLEXPART transport simulations that are then used in a Bayesian analytical inversion to estimate spatial emission distributions. Our results for four F-gases (HFC-134a, HFC-125, HFC-32, SF6) indicate that both high-resolution inversions and a dense measurement network significantly improve the ability to estimate spatial distribution of the emissions. Furthermore, the total emission estimates from the high-resolution inversions (351 ± 44 Mg yr−1 for HFC-134a, 101 ± 21 Mg yr−1 for HFC-125, 50 ± 8 Mg yr−1 for HFC-32, 9.0 ± 1.1 Mg yr−1 for SF6) are significantly higher compared to the low-resolution inversions (20 %–40 % increase) and result in total a posteriori emission estimates that are closer to national inventory values as reported to the UNFCCC (10 %–20 % difference between high-resolution inversion estimates and inventory values compared to 30 %–40 % difference between the low-resolution inversion estimates and inventory values). Specifically, we attribute these improvements to a better representation of the atmospheric flow in complex terrain in the high-resolution model, partly induced by the more realistic topography. We further conduct numerous sensitivity inversions, varying different parameters and variables of our Bayesian inversion framework to explore the whole range of uncertainty in the inversion errors (e.g., inversion grid, spatial distribution of a priori emissions, covariance parameters like baseline uncertainty and spatial correlation length, temporal resolution of the assimilated observations, observation network, seasonality of emissions). From the abovementioned parameters, we find that the uncertainty of the mole fraction baseline and the spatial distribution of the a priori emissions have the largest impact on the a posteriori total emission estimates and their spatial distribution. This study is a step towards mitigating the errors associated with the transport models and better characterizing the uncertainty inherent in the inversion error. Improvements in the latter will facilitate the validation and standardization of national GHG emission inventories and support policymakers.

How well can inverse analyses of high-resolution satellite data resolve heterogeneous methane fluxes? Observing system simulation experiments with the GEOS-Chem adjoint model (v35)

Abstract. We perform observing system simulation experiments (OSSEs) with the GEOS-Chem adjoint model to test how well methane emissions over North America can be resolved using measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and similar high-resolution satellite sensors. We focus analysis on the impacts of (i) spatial errors in the prior emissions and (ii) model transport errors. Along with a standard scale factor (SF) optimization we conduct a set of inversions using alternative formalisms that aim to overcome limitations in the SF-based approach that arise for missing sources. We show that 4D-Var analysis of the TROPOMI data can improve monthly emission estimates at 25 km even with a spatially biased prior or model transport errors (42 %–93 % domain-wide bias reduction; R increases from 0.51 up to 0.73). However, when both errors are present, no single inversion framework can successfully improve both the overall bias and spatial distribution of fluxes relative to the prior on the 25 km model grid. In that case, the ensemble-mean optimized fluxes have a domain-wide bias of 77 Gg d−1 (comparable to that in the prior), with spurious source adjustments compensating for the transport errors. Increasing observational coverage through longer-timeframe inversions does not significantly change this picture. An inversion formalism that optimizes emission enhancements rather than scale factors exhibits the best performance for identifying missing sources, while an approach combining a uniform background emission with the prior inventory yields the best performance in terms of overall spatial fidelity – even in the presence of model transport errors. However, the standard SF optimization outperforms both of these for the magnitude of the domain-wide flux. For the common scenario in which prior errors are non-random, approximate posterior error reduction calculations (derived via gradient-based randomization) for the inversions reflect the sensitivity to observations but have no spatial correlation with the actual emission improvements. This demonstrates that such information content analysis can be used for general observing system characterization but does not describe the spatial accuracy of the posterior emissions or of the actual emission improvements. Findings here highlight the need for careful evaluation of potential missing sources in prior emission datasets and for robust accounting of model transport errors in inverse analyses of the methane budget.

Examining CO2 Model Observation Residuals Using ACT‐America Data

AbstractAtmospheric inversion typically relies on the specification of prior flux and atmospheric model transport errors, which have large uncertainties. Here, we used ACT‐America airborne observations to compare model observation mismatch in the eastern U.S. and during four climatological seasons for the mesoscale WRF(‐Chem) and global scale CarbonTracker/TM5 (CT) models. Models used identical surface carbon fluxes, and CT was used as boundary condition for WRF. Both models showed reasonable agreement with observations, and residuals follow near symmetric peaked (i.e., non‐Gaussian) distribution with near‐zero bias of both models (CT: ppm; WRF: ppm). We also found large magnitude residuals at the tails of the distribution that contribute considerably to overall bias. Atmospheric boundary‐layer biases (1–10 ppm) were much larger than free tropospheric biases (0.5–1 ppm) and were of same magnitude as model‐model differences, whereas free tropospheric biases were mostly governed by background conditions. Results revealed systematic differences in atmospheric transport, most pronounced in the warm and cold sectors of synoptic systems, highlighting the importance of transport for residuals. While CT could reproduce the principal dynamics associated with synoptic systems, WRF showed a clearer distinction for differences across fronts. Variograms were used to quantify spatial correlation of residuals and showed characteristic residual length scales of approximately 100–300 km. Our findings suggest that inclusion of synoptic weather‐dependent and non‐Gaussian error structure may benefit inversion systems.

Accounting for Transport Error in Inversions: An Urban Synthetic Data Experiment.

We present and discuss the use of a high‐dimensional computational method for atmospheric inversions that incorporates the space‐time structure of transport and dispersion errors. In urban environments, transport and dispersion errors are largely the result of our inability to capture the true underlying transport of greenhouse gas (GHG) emissions to observational sites. Motivated by the impact of transport model error on estimates of fluxes of GHGs using in situ tower‐based mole‐fraction observations, we specifically address the need to characterize transport error structures in high‐resolution large‐scale inversion models. We do this using parametric covariance functions combined with shrinkage‐based regularization methods within an Ensemble Transform Kalman Filter inversion setup. We devise a synthetic data experiment to compare the impact of transport and dispersion error component of the model‐data mismatch covariance choices on flux retrievals and study the robustness of the method with respect to fewer observational constraints. We demonstrate the analysis in the context of inferring CO2 fluxes starting with a hypothesized prior in the Washington D.C. /Baltimore area constrained by a synthetic set of tower‐based CO2 measurements within an observing system simulation experiment framework. This study demonstrates the ability of these simple covariance structures to substantially improve the estimation of fluxes over standard covariance models in flux estimation from urban regions.

Regional CO<sub>2</sub> inversions with LUMIA, the Lund University Modular Inversion Algorithm, v1.0

Abstract. Atmospheric inversions are used to derive constraints on the net sources and sinks of CO2 and other stable atmospheric tracers from their observed concentrations. The resolution and accuracy that the fluxes can be estimated with depends, among other factors, on the quality and density of the observational coverage, on the precision and accuracy of the transport model used by the inversion to relate fluxes to observations, and on the adaptation of the statistical approach to the problem studied. In recent years, there has been an increasing demand from stakeholders for inversions at higher spatial resolution (country scale), in particular in the framework of the Paris agreement. This step up in resolution is in theory enabled by the growing availability of observations from surface in situ networks (such as ICOS in Europe) and from remote sensing products (OCO-2, GOSAT-2). The increase in the resolution of inversions is also a necessary step to provide efficient feedback to the bottom-up modeling community (vegetation models, fossil fuel emission inventories, etc.). However, it calls for new developments in the inverse models: diversification of the inversion approaches, shift from global to regional inversions, and improvement in the computational efficiency. In this context, we developed LUMIA, the Lund University Modular Inversion Algorithm. LUMIA is a Python library for inverse modeling built around the central idea of modularity: it aims to be a platform that enables users to construct and experiment with new inverse modeling setups while remaining easy to use and maintain. It is in particular designed to be transport-model-agnostic, which should facilitate isolating the transport model errors from those introduced by the inversion setup itself. We have constructed a first regional inversion setup using the LUMIA framework to conduct regional CO2 inversions in Europe using in situ data from surface and tall-tower observation sites. The inversions rely on a new offline coupling between the regional high-resolution FLEXPART Lagrangian particle dispersion model and the global coarse-resolution TM5 transport model. This test setup is intended both as a demonstration and as a reference for comparison with future LUMIA developments. The aims of this paper are to present the LUMIA framework (motivations for building it, development principles and future prospects) and to describe and test this first implementation of regional CO2 inversions in LUMIA.

On the model uncertainties in Bayesian source reconstruction using an ensemble of weather predictions, the emission inverse modelling system FREAR v1.0, and the Lagrangian transport and dispersion model Flexpart v9.0.2

Abstract. Bayesian source reconstruction is a powerful tool for determining atmospheric releases. It can be used, amongst other applications, to identify a point source releasing radioactive particles into the atmosphere. This is relevant for applications such as emergency response in case of a nuclear accident or Comprehensive Nuclear-Test-Ban treaty verification. The method involves solving an inverse problem using environmental radioactivity observations and atmospheric transport models. The Bayesian approach has the advantage of providing an uncertainty quantification on the inferred source parameters. However, it requires the specification of the inference input errors, such as the observation error and model error. The latter is particularly hard to provide as there is no straightforward way to determine the atmospheric transport and dispersion model error. Here, the importance of model error is illustrated for Bayesian source reconstruction using a recent and unique case where radionuclides were detected on several continents. A numerical weather prediction ensemble is used to create an ensemble of atmospheric transport and dispersion simulations, and a method is proposed to determine the model error.

Model Error Estimation for the Simplified PN Radiation Transport Equations

The Simplified () approximation is often used to model radiation transport phenomena, but it converges to the true solution of the transport equation only in one-dimensional slab geometry. In all other geometries, it incurs a model error that needs to be quantified. In this paper, we estimate the radiation transport model error due to the approximation and employ transport solutions (with high order) as reference transport solutions. Because the solution does not contain the full angular information of the transport solution, an angular intensity must be reconstructed from the solution in order to compute the model error. We propose two such reconstruction schemes. Model error estimates are given for various quantities of interests, i.e., scalar radiation intensity, radiation flux, and boundary leakage. An adjoint-based approach is proposed to evaluate the model error and is compared against forward and residual techniques. Two-dimensional numerical experiments are presented.

Representing model uncertainty for global atmospheric CO<sub>2</sub> flux inversions using ECMWF-IFS-46R1

Abstract. Atmospheric flux inversions use observations of atmospheric CO2 to provide anthropogenic and biogenic CO2 flux estimates at a range of spatio-temporal scales. Inversions require prior flux, a forward model and observation errors to estimate posterior fluxes and uncertainties. Here, we investigate the forward transport error and the associated biogenic feedback in an Earth system model (ESM) context. These errors can occur from uncertainty in the initial meteorology, the analysis fields used, or the advection schemes and physical parameterisation of the model. We also explore the spatio-temporal variability and flow-dependent error covariances. We then compare the error with the atmospheric response to uncertainty in the prior anthropogenic emissions. Although transport errors are variable, average total-column CO2 (XCO2) transport errors over anthropogenic emission hotspots (0.1–0.8 ppm) are comparable to, and often exceed, prior monthly anthropogenic flux uncertainties projected onto the same space (0.1–1.4 ppm). Average near-surface transport errors at three sites (Paris, Caltech and Tsukuba) range from 1.7 to 7.2 ppm. The global average XCO2 transport error standard deviation plateaus at ∼0.1 ppm after 2–3 d, after which atmospheric mixing significantly dampens the concentration gradients. Error correlations are found to be highly flow dependent, with XCO2 spatio-temporal correlation length scales ranging from 0 to 700 km and 0 to 260 min. Globally, the average model error caused by the biogenic response to atmospheric meteorological uncertainties is small (<0.01 ppm); however, this increases over high flux regions and is seasonally dependent (e.g. the Amazon; January and July: 0.24±0.18 ppm and 0.13±0.07 ppm). In general, flux hotspots are well-correlated with model transport errors. Our model error estimates, combined with the atmospheric response to anthropogenic flux uncertainty, are validated against three Total Carbon Observing Network (TCCON) XCO2 sites. Results indicate that our model and flux uncertainty account for 21 %–65 % of the total uncertainty. The remaining uncertainty originates from additional sources, such as observation, numerical and representation errors, as well as structural errors in the biogenic model. An underrepresentation of transport and flux uncertainties could also contribute to the remaining uncertainty. Our quantification of CO2 transport error can be used to help derive accurate posterior fluxes and error reductions in future inversion systems. The model uncertainty diagnosed here can be used with varying degrees of complexity and with different modelling techniques by the inversion community.

Diagnosing spatial error structures in CO<sub>2</sub> mole fractions and XCO<sub>2</sub> column mole fractions from atmospheric transport

Abstract. Atmospheric inversions inform us about the magnitude and variations of greenhouse gas (GHG) sources and sinks from global to local scales. Deployment of observing systems such as spaceborne sensors and ground-based instruments distributed around the globe has started to offer an unprecedented amount of information to estimate surface exchanges of GHG at finer spatial and temporal scales. However, all inversion methods still rely on imperfect atmospheric transport models whose error structures directly affect the inverse estimates of GHG fluxes. The impact of spatial error structures on the retrieved fluxes increase concurrently with the density of the available measurements. In this study, we diagnose the spatial structures due to transport model errors affecting modeled in situ carbon dioxide (CO2) mole fractions and total-column dry air mole fractions of CO2 (XCO2). We implement a cost-effective filtering technique recently developed in the meteorological data assimilation community to describe spatial error structures using a small-size ensemble. This technique can enable ensemble-based error analysis for multiyear inversions of sources and sinks. The removal of noisy structures due to sampling errors in our small-size ensembles is evaluated by comparison with larger-size ensembles. A second filtering approach for error covariances is proposed (Wiener filter), producing similar results over the 1-month simulation period compared to a Schur filter. Based on a comparison to a reference 25-member calibrated ensemble, we demonstrate that error variances and spatial error correlation structures are recoverable from small-size ensembles of about 8 to 10 members, improving the representation of transport errors in mesoscale inversions of CO2 fluxes. Moreover, error variances of in situ near-surface and free-tropospheric CO2 mole fractions differ significantly from total-column XCO2 error variances. We conclude that error variances for remote-sensing observations need to be quantified independently of in situ CO2 mole fractions due to the complexity of spatial error structures at different altitudes. However, we show the potential use of meteorological error structures such as the mean horizontal wind speed, directly available from ensemble prediction systems, to approximate spatial error correlations of in situ CO2 mole fractions, with similarities in seasonal variations and characteristic error length scales.

Comparative analysis of low-Earth orbit (TROPOMI) and geostationary (GeoCARB, GEO-CAPE) satellite instruments for constraining methane emissions on fine regional scales: application to the Southeast US

Abstract. We conduct Observing System Simulation Experiments (OSSEs) to compare the ability of future satellite measurements of atmospheric methane columns (TROPOMI, GeoCARB, GEO-CAPE) for constraining methane emissions down to the 25 km scale through inverse analyses. The OSSE uses the GEOS-Chem chemical transport model (0.25∘×0.3125∘ grid resolution) in a 1-week simulation for the Southeast US with 216 emission elements to be optimized through inversion of synthetic satellite observations. Clouds contaminate 73 %–91 % of the viewing scenes depending on pixel size. Comparison of GEOS-Chem to Total Carbon Column Observing Network (TCCON) surface-based methane column observations indicates a model transport error standard deviation of 12 ppb, larger than the instrument errors when aggregated on the 25 km model grid scale, and with a temporal error correlation of 6 h. We find that TROPOMI (7×7 km2 pixels, daily return time) can provide a coarse regional optimization of methane emissions, comparable to results from an aircraft campaign (SEAC4RS), and is highly sensitive to cloud cover. The geostationary instruments can do much better and are less sensitive to cloud cover, reflecting both their finer pixel resolution and more frequent observations. The information content from GeoCARB toward constraining methane emissions increases by 20 %–25 % for each doubling of the GeoCARB measurement frequency. Temporal error correlation in the transport model moderates but does not cancel the benefit of more frequent measurements for geostationary instruments. We find that GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission preformulated by NASA in response to the Decadal Survey of the US National Research Council.

Impact of physical parameterizations and initial conditions on simulated atmospheric transport and CO<sub>2</sub> mole fractions in the US Midwest

Abstract. Atmospheric transport model errors are one of the main contributors to the uncertainty affecting CO2 inverse flux estimates. In this study, we determine the leading causes of transport errors over the US upper Midwest with a large set of simulations generated with the Weather Research and Forecasting (WRF) mesoscale model. The various WRF simulations are performed using different meteorological driver datasets and physical parameterizations including planetary boundary layer (PBL) schemes, land surface models (LSMs), cumulus parameterizations and microphysics parameterizations. All the different model configurations were coupled to CO2 fluxes and lateral boundary conditions from the CarbonTracker inversion system to simulate atmospheric CO2 mole fractions. PBL height, wind speed, wind direction, and atmospheric CO2 mole fractions are compared to observations during a month in the summer of 2008, and statistical analyses were performed to evaluate the impact of both physics parameterizations and meteorological datasets on these variables. All of the physical parameterizations and the meteorological initial and boundary conditions contribute 3 to 4 ppm to the model-to-model variability in daytime PBL CO2 except for the microphysics parameterization which has a smaller contribution. PBL height varies across ensemble members by 300 to 400 m, and this variability is controlled by the same physics parameterizations. Daily PBL CO2 mole fraction errors are correlated with errors in the PBL height. We show that specific model configurations systematically overestimate or underestimate the PBL height averaged across the region with biases closely correlated with the choice of LSM, PBL scheme, and cumulus parameterization (CP). Domain average PBL wind speed is overestimated in nearly every model configuration. Both planetary boundary layer height (PBLH) and PBL wind speed biases show coherent spatial variations across the Midwest, with PBLH overestimated averaged across configurations by 300–400 m in the west, and PBL winds overestimated by about 1 m s−1 on average in the east. We find model configurations with lower biases averaged across the domain, but no single configuration is optimal across the entire region and for all meteorological variables. We conclude that model ensembles that include multiple physics parameterizations and meteorological initial conditions are likely to be necessary to encompass the atmospheric conditions most important to the transport of CO2 in the PBL, but that construction of such an ensemble will be challenging due to ensemble biases that vary across the region.

Quantifying the vertical transport of CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub> over the western Pacific

Abstract. We use the GEOS-Chem global 3-D atmospheric chemistry transport model to interpret atmospheric observations of bromoform (CHBr3) and dibromomethane (CH2Br2) collected during the CAST and CONTRAST aircraft measurement campaigns over the western Pacific, January–February 2014. We use a new linearized, tagged version of CHBr3 and CH2Br2, allowing us to study the influence of emissions from specific geographical regions on observed atmospheric variations. The model describes 32 %–37 % of CHBr3 and 15 %–45 % of CH2Br2 observed variability during CAST and CONTRAST, reflecting model errors in vertical transport. The model has a mean positive bias of 30 % that is larger near the surface, reflecting errors in the poorly constrained prior emission estimates. We find using the model that observed variability of CHBr3 and CH2Br2 is driven by open ocean emissions where there is deep convection. Atmospheric variability above 6 km includes a significant contribution from coastal oceans, but it is still dominated by emissions from the open ocean and by older air masses that originate upwind. In the absence of reliable ocean emission estimates, we use a new physical age-of-air simulation to determine the relative abundance of halogens delivered by CHBr3 and CH2Br2 to the tropical transition layer (TTL). We find that 76 % (92 %) of air masses that originate from the ocean reach the TTL within two (three) atmospheric e-folding lifetimes of CHBr3 and almost all of them reach the TTL within one e-folding lifetime of CH2Br2. Over the duration of CAST and CONTRAST, and over our study region, oceans delivered a mean (range) CHBr3 and CH2Br2 mole fraction of 0.46 (0.13–0.72) and 0.88 (0.71–1.01) pptv, respectively, to the TTL, and a mean (range) Bry mole fraction of 3.14 (1.81–4.18) pptv from source gases to the upper troposphere.

Reducing errors in aircraft atmospheric inversion estimates of point-source emissions: the Aliso Canyon natural gas leak as a natural tracer experiment

Urban greenhouse gas (GHG) flux estimation with atmospheric measurements and modeling, i.e. the ‘top-down’ approach, can potentially support GHG emission reduction policies by assessing trends in surface fluxes and detecting anomalies from bottom-up inventories. Aircraft-collected GHG observations also have the potential to help quantify point-source emissions that may not be adequately sampled by fixed surface tower-based atmospheric observing systems. Here, we estimate CH4 emissions from a known point source, the Aliso Canyon natural gas leak in Los Angeles, CA from October 2015–February 2016, using atmospheric inverse models with airborne CH4 observations from twelve flights ≈4 km downwind of the leak and surface sensitivities from a mesoscale atmospheric transport model. This leak event has been well-quantified previously using various methods by the California Air Resources Board, thereby providing high confidence in the mass-balance leak rate estimates of (Conley et al ), used here for comparison to inversion results. Inversions with an optimal setup are shown to provide estimates of the leak magnitude, on average, within a third of the mass balance values, with remaining errors in estimated leak rates predominantly explained by modeled wind speed errors of up to 10 m s−1, quantified by comparing airborne meteorological observations with modeled values along the flight track. An inversion setup using scaled observational wind speed errors in the model-data mismatch covariance matrix is shown to significantly reduce the influence of transport model errors on spatial patterns and estimated leak rates from the inversions. In sum, this study takes advantage of a natural tracer release experiment (i.e. the Aliso Canyon natural gas leak) to identify effective approaches for reducing the influence of transport model error on atmospheric inversions of point-source emissions, while suggesting future potential for integrating surface tower and aircraft atmospheric GHG observations in top-down urban emission monitoring systems.

The constraint of CO<sub>2</sub> measurements made onboard passenger aircraft on surface–atmosphere fluxes: the impact of transport model errors in vertical mixing

Abstract. Inaccurate representation of atmospheric processes by transport models is a dominant source of uncertainty in inverse analyses and can lead to large discrepancies in the retrieved flux estimates. We investigate the impact of uncertainties in vertical transport as simulated by atmospheric transport models on fluxes retrieved using vertical profiles from aircraft as an observational constraint. Our numerical experiments are based on synthetic data with realistic spatial and temporal sampling of aircraft measurements. The impact of such uncertainties on the flux retrieved using the ground-based network and those retrieved using the aircraft profiles are compared. We find that the posterior flux retrieved using aircraft profiles is less susceptible to errors in boundary layer height, compared to the ground-based network. This finding highlights a benefit of utilizing atmospheric observations made onboard aircraft over surface measurements for flux estimation using inverse methods. We further use synthetic vertical profiles of CO2 in an inversion to estimate the potential of these measurements, which will be made available through the IAGOS (In-service Aircraft for a Global Observing System) project in the future, in constraining the regional carbon budget. Our results show that the regions of tropical Africa and temperate Eurasia, that are under-constrained by the existing surface-based network, will benefit the most from these measurements, with a reduction of posterior flux uncertainty of about 7 to 10 %.

Lower-tropospheric CO<sub>2</sub> from near-infrared ACOS-GOSAT observations

Abstract. We present two new products from near-infrared Greenhouse Gases Observing Satellite (GOSAT) observations: lowermost tropospheric (LMT, from 0 to 2.5 km) and upper tropospheric–stratospheric (U, above 2.5 km) carbon dioxide partial column mixing ratios. We compare these new products to aircraft profiles and remote surface flask measurements and find that the seasonal and year-to-year variations in the new partial column mixing ratios significantly improve upon the Atmospheric CO2 Observations from Space (ACOS) and GOSAT (ACOS-GOSAT) initial guess and/or a priori, with distinct patterns in the LMT and U seasonal cycles that match validation data. For land monthly averages, we find errors of 1.9, 0.7, and 0.8 ppm for retrieved GOSAT LMT, U, and XCO2; for ocean monthly averages, we find errors of 0.7, 0.5, and 0.5 ppm for retrieved GOSAT LMT, U, and XCO2. In the southern hemispheric biomass burning season, the new partial columns show similar patterns to MODIS fire maps and MOPITT multispectral CO for both vertical levels, despite a flat ACOS-GOSAT prior, and a CO–CO2 emission factor comparable to published values. The difference of LMT and U, useful for evaluation of model transport error, has also been validated with a monthly average error of 0.8 (1.4) ppm for ocean (land). LMT is more locally influenced than U, meaning that local fluxes can now be better separated from CO2 transported from far away.

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.

Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide

Abstract. Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m−3). For such plumes, the ER is found to increase almost 2-fold on the scale of ∼ 10 h of daytime aerosol evolution (after a few first hours of the evolution that are not resolved in our analysis). The robustness of this finding is corroborated by sensitivity tests and Monte Carlo experiments. Furthermore, a simulation using the volatility basis set framework suggests that a large part of the increase in the ER can be explained by atmospheric processing of semi-volatile organic compounds. Our results are consistent with findings of a number of earlier studies reporting considerable underestimation of AOD by CTMs in which BB aerosol aging processes have either been disregarded or simulated in a highly simplified way. In general, this study demonstrates the feasibility of using satellite measurements of AOD in biomass burning plumes in combination with aerosol tracer simulations for the investigation of BB aerosol evolution and validation of BB aerosol aging schemes in atmospheric models.

Greenhouse gas simulations with a coupled meteorological and transport model: the predictability of CO<sub>2</sub>

Abstract. A new model for greenhouse gas transport has been developed based on Environment and Climate Change Canada's operational weather and environmental prediction models. When provided with realistic posterior fluxes for CO2, the CO2 simulations compare well to NOAA's CarbonTracker fields and to near-surface continuous measurements, columns from the Total Carbon Column Observing Network (TCCON) and NOAA aircraft profiles. This coupled meteorological and tracer transport model is used to study the predictability of CO2. Predictability concerns the quantification of model forecast errors and thus of transport model errors. CO2 predictions are used to compute model–data mismatches when solving flux inversion problems and the quality of such predictions is a major concern. Here, the loss of meteorological predictability due to uncertain meteorological initial conditions is shown to impact CO2 predictability. The predictability of CO2 is shorter than that of the temperature field and increases near the surface and in the lower stratosphere. When broken down into spatial scales, CO2 predictability at the very largest scales is mainly due to surface fluxes but there is also some sensitivity to the land and ocean surface forcing of meteorological fields. The predictability due to the land and ocean surface is most evident in boreal summer when biospheric uptake produces large spatial gradients in the CO2 field. This is a newly identified source of uncertainty in CO2 predictions but it is expected to be much less significant than uncertainties in fluxes. However, it serves as an upper limit for the more important source of transport error and loss of predictability, which is due to uncertain meteorological analyses. By isolating this component of transport error, it is demonstrated that CO2 can only be defined on large spatial scales due to the presence of meteorological uncertainty. Thus, for a given model, there is a spatial scale below which fluxes cannot be inferred simply due to the fact that meteorological analyses are imperfect. These unresolved spatial scales correspond to small scales near the surface but increase with altitude. By isolating other components of transport error, the largest or limiting error can be identified. For example, a model error due to the lack of convective tracer transport was found to impact transport error on the very largest (wavenumbers less than 5) spatial scales. Thus for wavenumbers greater than 5, transport model error due to meteorological analysis uncertainty is more important for our model than the lack of convective tracer transport.

Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.