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This study investigated the spatiotemporal variabilities in nitrogen dioxide (NO 2), formaldehyde (HCHO), ozone (O 3), and light-absorbing aerosols within the Greater Tokyo Area, Japan, which is the most populous metropolitan area in the world. The analysis is based on total tropospheric column, partial tropospheric column (within the boundary layer), and in situ observations retrieved from multiple platforms as well as additional information obtained from reanalysis and box model simulations. This study mainly covers the 2013–2020 period, focusing on 2020 when air quality was influenced by the coronavirus 2019 (COVID-19) pandemic. Although total and partial tropospheric NO 2 columns were reduced by an average of about 10 % in 2020, reductions exceeding 40 % occurred in some areas during the pandemic state of emergency. Light-absorbing aerosol levels within the boundary layer were also reduced for most of 2020, while smaller fluctuations in HCHO and O 3 were observed. The significantly enhanced degree of weekly cycling of NO 2 , HCHO, and light-absorbing aerosol found in urban areas during 2020 suggests that, in contrast to other countries, mobility in Japan also dropped on weekends. We conclude that, despite the lack of strict mobility restrictions in Japan, widespread adherence to recommendations designed to limit the COVID-19 spread resulted in unique air quality improvements. [ABSTRACT FROM AUTHOR]

We developed a high-resolution surface flux inversion system based on the global Eulerian–Lagrangian coupled tracer transport model composed of the National Institute for Environmental Studies (NIES) transport model (TM; collectively NIES-TM) and the FLEXible PARTicle dispersion model (FLEXPART). The inversion system is named NTFVAR (NIES-TM–FLEXPART-variational) as it applies a variational optimization to estimate surface fluxes. We tested the system by estimating optimized corrections to natural surface CO2 fluxes to achieve the best fit to atmospheric CO2 data collected by the global in situ network as a necessary step towards the capability of estimating anthropogenic CO2 emissions. We employed the Lagrangian particle dispersion model (LPDM) FLEXPART to calculate surface flux footprints of CO2 observations at a spatial resolution of 0.1∘×0.1∘. The LPDM is coupled with 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 was 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) data set. High-resolution prior flux fields were prepared using the Open-Data Inventory for Anthropogenic Carbon dioxide (ODIAC) for fossil fuel combustion, the Global Fire Assimilation System (GFAS) for biomass burning, the Vegetation Integrative SImulator for Trace gases (VISIT) model for terrestrial biosphere exchange, and the Ocean Tracer Transport Model (OTTM) for oceanic exchange. The terrestrial biospheric flux field was constructed using a vegetation mosaic map and a separate simulation of CO2 fluxes at a daily time step by the VISIT model for each vegetation type. The prior flux uncertainty for the 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 fine-scale vegetation productivity gradients. The resulting flux estimates improved the fit to the observations taken at continuous observation sites, reproducing both the seasonal and short-term concentration variabilities including high CO2 concentration events associated with anthropogenic emissions. The use of a high-resolution atmospheric transport in global CO2 flux inversions has the advantage of better resolving the transported mixed signals from the anthropogenic and biospheric sources in densely populated continental regions. Thus, it has the potential to achieve better separation between fluxes from terrestrial ecosystems and strong localized sources, such as anthropogenic emissions and forest fires. Further improvements in the modelling system are needed as our posterior fit was better than that of the National Oceanic and Atmospheric Administration (NOAA)'s CarbonTracker for only a fraction of the monitoring sites, i.e. mostly at coastal and island locations where background and local flux signals are mixed. [ABSTRACT FROM AUTHOR]

A three-dimensional simulation of gravitational separation, defined as the process of atmospheric molecule separation under gravity according to their molar masses, is performed for the first time in the upper troposphere and lower stratosphere. We analyze distributions of two isotopes with a small difference in molecular mass (13C16O2 (Mi=45) and 12C16O2 (Mi=44)) simulated by the National Institute for Environmental Studies (NIES) chemical transport model (TM) with a parameterization of molecular diffusion. The NIES model employs global reanalysis and an isentropic vertical coordinate and uses optimized CO2 fluxes. The applicability of the NIES TM to the modeling of gravitational separation is demonstrated by a comparison with measurements recorded by high-precision cryogenic balloon-borne samplers in the lower stratosphere. We investigate the processes affecting the seasonality of gravitational separation and examine the age of air derived from the tracer distributions modeled by the NIES TM. We find a strong relationship between age of air and gravitational separation for the main climatic zones. The advantages and limitations of using age of air and gravitational separation as indicators of the variability in the stratosphere circulation are discussed. [ABSTRACT FROM AUTHOR]

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 ap- proach 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. [ABSTRACT FROM AUTHOR]

Extremely high levels of column-averaged dryair mole fractions of atmospheric methane (XCH4) were detected in August and September 2013 over northeast Asia (~20 ppb above the averaged summertime XCH4 over 2009-2012, after removing a long-term trend), as being retrieved from the Short-Wavelength InfraRed (SWIR) spectral data observed with the Thermal And Near-infrared Sensor for carbon Observation - Fourier Transform Spectrometer (TANSO-FTS) onboard Greenhouse Gases Observing Satellite (GOSAT). Similar enhancements of XCH4 were also observed by the ground-based measurements at two Total Carbon Column Observing Network (TCCON) sites in Japan. The analysis of surface CH4 concentrations observed at three monitoring sites around the Japan archipelago suggest that the extreme increase of XCH4 has occurred in a limited area. The model analysis was conducted to investigate this anomalously high XCH4 event, using an atmospheric transport model. The results indicate that the extreme increase of XCH4 is attributed to the anomalous atmospheric pressure pattern over East Asia during the summer of 2013, which effectively transported the CH4-rich air to Japan from the strong CH4 source areas in east China. The two Japanese TCCON sites, ~1000 km east-west apart each other, coincidentally located along the substantially CH4-rich air flow from east China. This analysis demonstrates the capability of GOSAT to monitor an XCH4 event on a synoptic scale. We anticipate that the synoptic information of XCH4 from GOSAT data contributes to improve our understanding of regional carbon cycle and the regional flux estimation. [ABSTRACT FROM AUTHOR]