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We developed a high-resolution surface flux inversion system based on the global Lagrangian–Eulerian coupled tracer transport model composed of National Institute for Environmental Studies Transport Model (NIES-TM) and FLEXible PARTicle dispersion model (FLEXPART). The inversion system is named NTFVAR (NIES-TM-FLEXPART-variational) as it applies variational optimisation to estimate surface fluxes. We tested the system by estimating optimized corrections to natural surface CO2 fluxes to achieve best fit to atmospheric CO2 data collected by the global in-situ network, as a necessary step towards capability of estimating anthropogenic CO2 emissions. We employ the Lagrangian particle dispersion model (LPDM) FLEXPART to calculate the surface flux footprints of CO2 observations at a 0.1° × 0.1° spatial resolution. The LPDM is coupled to a global atmospheric tracer transport model (NIES-TM). Our inversion technique uses an adjoint of the coupled transport model in an iterative optimization procedure. The flux error covariance operator is being implemented via implicit diffusion. Biweekly flux corrections to prior flux fields were estimated for the years 2010–2012 from in-situ CO2 data included in the Observation Package (ObsPack) dataset. High-resolution prior flux fields were prepared using Open-Data Inventory for Anthropogenic Carbon dioxide (ODIAC) for fossil fuel combustion, Global Fire Assimilation System (GFAS) for biomass burning, the Vegetation Integrative SImulator for Trace gases (VISIT) model for terrestrial biosphere exchange and Ocean Tracer Transport Model (OTTM) for oceanic exchange. The terrestrial biospheric flux field was constructed using a vegetation mosaic map and separate simulation of CO2 fluxes at daily time step by the VISIT model for each vegetation type. The prior flux uncertainty for terrestrial biosphere was scaled proportionally to the monthly mean Gross Primary Production (GPP) by the Moderate Resolution Imaging Spectroradiometer (MODIS) MOD17 product. The inverse system calculates flux corrections to the prior fluxes in the form of a relatively smooth field multiplied by high-resolution patterns of the prior flux uncertainties for land and ocean, following the coastlines and vegetation productivity gradients. The resulting flux estimates improve fit to the observations at continuous observations sites, reproducing both the seasonal variation and short-term concentration variability, including high CO2 concentration events associated with anthropogenic emissions. The use of high-resolution atmospheric transport in global CO2 flux inversion has the advantage of better resolving the transport from the mix of the anthropogenic and biospheric sources in densely populated continental regions and shows potential for better separation between fluxes from terrestrial ecosystems and strong localised sources such as anthropogenic emissions and forest fires. Further improvements in the modelling system are needed as the posterior fit is better than that by the National Oceanic and Atmospheric Administration (NOAA) CarbonTracker only for a fraction of the monitoring sites, mostly at coastal and island locations experiencing mix of background and local flux signals.

The Total Carbon Column Observing Network (TCCON) is a network of ground-based Fourier transform spectrometers (FTSs) that record near-infrared (NIR) spectra of the sun. From these spectra, accurate and precise observations of CO2 column-averaged dry-air mole fractions (denoted XCO2) are retrieved. TCCON FTS observations have previously been used to validate satellite estimations of XCO2; however, our knowledge of the short-term spatial and temporal variations in XCO2 surrounding the TCCON sites is limited. In this work, we use the National Institute for Environmental Studies (NIES) Eulerian three-dimensional transport model and the FLEXPART (FLEXible PARTicle dispersion model) Lagrangian particle dispersion model (LPDM) to determine the footprints of short-term variations in XCO2 observed by operational, past, future and possible TCCON sites. We propose a footprint-based method for the collocation of satellite and TCCON XCO2 observations and estimate the performance of the method using the NIES model and five GOSAT (Greenhouse Gases Observing Satellite) XCO2 product data sets. Comparison of the proposed approach with a standard geographic method shows a higher number of collocation points and an average bias reduction up to 0.15 ppm for a subset of 16 stations for the period from January 2010 to January 2014. Case studies of the Darwin and Reunion Island sites reveal that when the footprint area is rather curved, non-uniform and significantly different from a geographical rectangular area, the differences between these approaches are more noticeable. This emphasises that the collocation is sensitive to local meteorological conditions and flux distributions.

In situ observation of the atmospheric CO2, CH4, and CO mixing ratios at Hateruma Island (HAT, 24.05° N, 123.80° E) often show synoptic-scale variations with correlative elevations during winter, associated with air transport from the East Asian countries. We examine winter (November– March) trends in ΔCH4 / ΔCO2, ΔCO / ΔCO2, and ΔCO / ΔCH4 observed at Hateruma over the period 1999 to 2010. To investigate the relationship between the East Asian emissions and the short-term variations in the atmospheric mixing ratios, we use the FLEXPART Lagrangian particle dispersion model (LPDM). The observed ratios ΔCH4 / ΔCO2 and ΔCO / ΔCO2 both show an overall gradual decrease over the study period due to a recent rapid increase in fossil fuel consumption in China. We note, however, that the decreasing rates of ΔCH4 / ΔCO2 and ΔCO / ΔCO2 show gradual decrease and increase, respectively, during the entire observation periods used in this study. The ΔCO / ΔCH4 slope, on the other hand, shows an increasing trend during 1999–2004 but a decrease during 2005–2010. Calculation of the concentration footprint for the atmospheric observation at HAT by using the FLEXPART LPDM indicates that most of the short-term variations are caused by emission variations from northern and eastern China. Combined with a set of reported emission maps, we have estimated the temporal changes in the annual CH4 and CO emissions from China under the assumption that the estimate of the fossil-fuel-derived CO2 emissions based on the energy statistics are accurate. The estimated annual CH4 emissions, corresponding to nonseasonal sources or anthropogenic sources without rice fields, show a nearly constant value of 39 ± 7 TgCH4 yr−1 during 1998–2002, and then gradually increase to 46 ± 8 TgCH4 yr−1 in 2009/2010. The estimated annual CO emissions increase from 134 ± 32 TgCO yr−1 in 1998/1999 to 182 ± 42 TgCO yr−1 in 2004/2005, level off after 2005, and then slightly decrease to less than 160 TgCO yr−1 in 2008–2010.

The Total Carbon Column Observing Network (TCCON) is a network of ground-based Fourier Transform Spectrometers (FTS) that record near-infrared (NIR) spectra of the Sun. From these spectra, accurate and precise observations of CO2 column-averaged dry-air mole fraction (denoted XCO2) are retrieved. TCCON FTS observations have previously been used to validate satellite estimations of XCO2; however, our knowledge of the short-term spatial and temporal variations in XCO2 surrounding the TCCON sites is limited. In this work, we use the National Institute for Environmental Studies (NIES) Eulerian three-dimensional transport model and the FLEXPART (FLEXible PARTicle) Lagrangian Particle Dispersion Model (LPDM) to determine the footprints of short-term variations in XCO2 observed by operational, past, future, and possible TCCON sites. We propose a footprint-based method for the colocation of satellite and TCCON XCO2 observations, and estimate the performance of the method using the NIES model and five GOSAT XCO2 product datasets. Comparison of the proposed approach with a standard geographic method shows higher number of colocation points and average bias reduction up to 0.15 ppm for a subset of 16 stations for the period from January 2010 to January 2014. Case studies of the Darwin and La Réunion sites reveal that when the footprint area is rather curved, non-uniform and significantly different from a geographical rectangular area, the differences between these approaches are more noticeable. This emphasizes that the colocation is sensitive to local meteorological conditions and flux distributions.

We designed a method to simulate atmospheric CO2 concentrations at several continuous observation sites around the globe using surface fluxes at a very high spatial resolution. The simulations presented in this study were performed using the Global Eulerian-Lagrangian Coupled Atmospheric model (GELCA), comprising a Lagrangian particle dispersion model coupled to a global atmospheric tracer transport model with prescribed global surface CO2 flux maps at a 1 × 1 km resolution. The surface fluxes used in the simulations were prepared by assembling the individual components of terrestrial, oceanic and fossil fuel CO2 fluxes. This experimental setup (i.e. a transport model running at a medium resolution, coupled to a high-resolution Lagrangian particle dispersion model together with global surface fluxes at a very high resolution), which was designed to represent high-frequency variations in atmospheric CO2 concentration, has not been reported at a global scale previously. Two sensitivity experiments were performed: (a) using the global transport model without coupling to the Lagrangian dispersion model, and (b) using the coupled model with a reduced resolution of surface fluxes, in order to evaluate the performance of Eulerian-Lagrangian coupling and the role of high-resolution fluxes in simulating high-frequency variations in atmospheric CO2 concentrations. A correlation analysis between observed and simulated atmospheric CO2 concentrations at selected locations revealed that the inclusion of both Eulerian-Lagrangian coupling and high-resolution fluxes improves the high-frequency simulations of the model. The results highlight the potential of a coupled Eulerian-Lagrangian model in simulating high-frequency atmospheric CO2 concentrations at many locations worldwide. The model performs well in representing observations of atmospheric CO2 concentrations at high spatial and temporal resolutions, especially for coastal sites and sites located close to sources of large anthropogenic emissions. While this study focused on simulations of CO2 concentrations, the model could be used for other atmospheric compounds with known estimated emissions.

We present the development of the Adjoint of the Global Eulerian–Lagrangian Coupled Atmospheric (A-GELCA) model that consists of the National Institute for Environmental Studies (NIES) model as an Eulerian three-dimensional transport model (TM), and FLEXPART (FLEXible PARTicle dispersion model) as the Lagrangian plume diffusion model (LPDM). The tangent and adjoint components of the Eulerian model were constructed directly from the original NIES TM code using an automatic differentiation tool known as TAF (Transformation of Algorithms in Fortran; http://www.FastOpt.com), with additional manual pre- and post-processing aimed at improving the performance of the computing, including MPI (Message Passing Interface). As results, the adjoint of Eulerian model is discrete. Construction of the adjoint of the Lagrangian component did not require any code modification, as LPDMs are able to track a significant number of particles back in time and thereby calculate the sensitivity of observations to the neighboring emissions areas. Eulerian and Lagrangian adjoint components were coupled at the time boundary in the global domain.The results are verified using a series of test experiments. The forward simulation shown the coupled model is effective in reproducing the seasonal cycle and short-term variability of CO2 even in the case of multiple limiting factors, such as high uncertainty of fluxes and the low resolution of the Eulerian model. The adjoint model demonstrates the high accuracy compared to direct forward sensitivity calculations and fast performance. The developed adjoint of the coupled model combines the flux conservation and stability of an Eulerian discrete adjoint formulation with the flexibility, accuracy, and high resolution of a Lagrangian backward trajectory formulation.

We designed a method to simulate atmospheric CO2 concentrations at several continuous observation sites around the globe using surface fluxes at a very high spatial resolution. The simulations presented in this study were performed using a Lagrangian particle dispersion model coupled to a global atmospheric tracer transport model with prescribed global surface CO2 flux maps at a 1 × 1 km resolution. The surface fluxes used in the simulations were prepared by assembling the individual components of terrestrial, oceanic and fossil fuel CO2 fluxes. This experimental setup (i.e., a transport model running at a medium resolution, coupled to a high-resolution Lagrangian particle dispersion model together with global surface fluxes at a very high resolution), which was designed to represent high-frequency variations in atmospheric CO2 concentration, has not been reported at a global scale previously. Two sensitivity experiments were performed: (a) using the global transport model without coupling to the Lagrangian dispersion model, and (b) using the coupled model with a reduced resolution of surface fluxes, in order to evaluate the performance of Eulerian-Lagrangian coupling and the role of high-resolution fluxes in simulating high-frequency variations in atmospheric CO2 concentrations. A correlation analysis between observed and simulated atmospheric CO2 concentrations at selected locations revealed that the inclusion of both Eulerian-Lagrangian coupling and high-resolution fluxes improves the high-frequency simulations of the model. The results highlight the potential of a coupled Eulerian-Lagrangian model in simulating high-frequency atmospheric CO2 concentrations at many locations worldwide. The model performs well in representing observations of atmospheric CO2 concentrations at high spatial and temporal resolutions, especially for coastal sites and sites located close to sources of large anthropogenic emissions. While this study focused on simulations of CO2 concentrations, the model could be used for other atmospheric compounds with known estimated emissions.