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A data set containing more than 6 years (February 2009 to present) of radiance spectra for carbon dioxide (CO2) and methane (CH4) observations has been acquired by the Greenhouse gases Observing SATellite (GOSAT, available at http://data.gosat.nies.go.jp/GosatUserInterfaceGateway/guig/GuigPage/open.do), nicknamed “Ibuki”, Thermal And Near infrared Sensor for carbon Observation Fourier Transform Spectrometer (TANSO-FTS). This paper provides updates on the performance of the satellite and TANSO-FTS sensor and describes important changes to the data product, which has recently been made available to users. With these changes the typical accuracy of retrieved column-averaged dry air mole fractions of CO2 and CH4 (XCO2 and XCH4, respectively) are 2 ppm or 0.5 % and 13 ppb or 0.7 %, respectively. Three major anomalies of the satellite system affecting TANSO-FTS are reported: a failure of one of the two solar paddles in May 2014, a switch to the secondary pointing system in January 2015, and most recently a cryocooler shutdown and restart in August 2015. The Level 1A (L1A) (raw interferogram) and the Level 1B (L1B) (radiance spectra) of version V201 described here have long-term uniform quality and provide consistent retrieval accuracy even after the satellite system anomalies. In addition, we discuss the unique observation abilities of GOSAT made possible by an agile pointing mechanism, which allows for optimization of global sampling patterns.

Knowledge of surface pressure is essential for calculating column-averaged dry-air mole fractions of trace gases, such as CO2 (XCO2). In the NASA Orbiting Carbon Observatory 2 (OCO-2) Atmospheric Carbon Observations from Space (ACOS) retrieval algorithm, the retrieved surface pressures have been found to have unacceptable errors, warranting a parametric bias correction. This correction depends on the difference between retrieved and a priori surface pressures, which are derived from a meteorological model that is hypsometrically adjusted to the surface elevation using a digital elevation model (DEM). As a result, the effectiveness of the OCO-2 bias correction is contingent upon the accuracy of the referenced DEM. Here, we investigate several different DEM datasets for use in the OCO-2 ACOS retrieval algorithm: the OCODEM used in ACOS v10 and previous versions, the NASADEM+ (a composite of SRTMv4, ASTER GDEMv3, GIMP, and RAMPv2 DEMs) used in ACOS v11, the Copernicus GLO-90 DEM (GLO-90 DEM), and two polar regional DEMs (ArcticDEM and REMA). We find that the NASADEM+ (ASTER GDEMv3) has a persistent negative bias on the order of 10 to 20 m across most regions north of 60° N latitude, relative to all the other DEMs considered (OCODEM, ArcticDEM, and GLO-90 DEM). Variations of 10 m in DEM elevations lead to variations in XCO2 of approximately 0.4 ppm, meaning that the XCO2 from OCO-2 ACOS v11 retrievals tends to be 0.4 to 0.8 ppm lower across regions north of 60° N than XCO2 from OCO-2 ACOS v10. Our analysis also suggests that the GLO-90 DEM has superior global continuity and accuracy compared to the other DEMs, motivating a post-processing update from OCO-2 v11 Lite files (which used NASADEM+) to OCO-2 v11.1 by substituting the GLO-90 DEM globally. We find that OCO-2 v11.1 improves accuracy and spatial continuity in the bias-corrected XCO2 product relative to both v10 and v11 in high-latitude regions while resulting in marginal or no change in most regions within ± 60° latitude. In addition, OCO-2 v11.1 provides increased data throughput after quality control filtering in most regions, partly due to the change in DEM but mostly due to other corrections to quality control parameters. Given large-scale differences north of 60° N between the OCODEM and NASADEM+, we find that replacing the OCODEM with NASADEM+ yields a ∼ 100 TgC shift in inferred carbon uptake for the zones spanning 30 to 60° N and 60 to 90° N, which is on the order of 5 % to 7 % of the estimated pan-Arctic land sink. Changes in inferred fluxes from replacing the OCODEM with the GLO-90 DEM are smaller, and given the evidence for improved accuracies from this DEM, this suggests that large changes in inferred fluxes from the NASADEM+ are likely erroneous.

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97∘ N, 4.93∘ E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation.The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions.The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.

Multi-axis differential optical absorption spectroscopy (MAX-DOAS) and direct sun NO2 vertical column network data are used to investigate the accuracy of tropospheric NO2 column measurements of the GOME-2 instrument on the MetOp-A satellite platform and the OMI instrument on Aura. The study is based on 23 MAX-DOAS and 16 direct sun instruments at stations distributed worldwide. A method to quantify and correct for horizontal dilution effects in heterogeneous NO2 field conditions is proposed. After systematic application of this correction to urban sites, satellite measurements are found to present smaller biases compared to ground-based reference data in almost all cases. We investigate the seasonal dependence of the validation results as well as the impact of using different approaches to select satellite ground pixels in coincidence with ground-based data. In optimal comparison conditions (satellite pixels containing the station) the median bias between satellite tropospheric NO2 column measurements and the ensemble of MAX-DOAS and direct sun measurements is found to be significant and equal to -34 % for GOME-2A and -24 % for OMI. These biases are further reduced to-24 % and -18 % respectively, after application of the dilution correction. Comparisons with the QA4ECV satellite product for both GOME-2A and OMI are also performed, showing less scatter but also a slightly larger median tropospheric NO2 column bias with respect to the ensemble of MAX-DOAS and direct sun measurements.

Long-term measurements of atmospheric mass concentrations of black carbon (BC) are needed to investigate changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including particle soot absorption photometers (PSAPs), continuous light absorption photometers (CLAPs), Aethalometers, and multi-angle absorption photometers (MAAPs). The measured babs can be converted to mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC; MBC= babs/ MAC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2), and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC and long-term stability of the regression slope, which is denoted as MACcor (MAC derived from the correlation). In general, babs–MBC (COSMOS) correlations were high (r2= 0.76–0.95 for hourly data) at Alert in Canada, Ny-Ålesund in Svalbard, Barrow (NOAA Barrow Observatory) in Alaska, Pallastunturi in Finland, and Fukue in Japan and stable for up to 10 years. We successfully estimated MACcor values (10.8–15.1 m2 g−1 at a wavelength of 550 nm for hourly data) for these instruments, and these MACcor values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC at these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation in MBC in the Arctic and to evaluation of the performance of numerical model calculations.

Observations from the new Japanese geostationary satellite Himawari-8 permit quasi-real-time estimation of global shortwave radiation at an unprecedented temporal resolution. However, accurate comparisons with ground-truthing observations are essential to assess their uncertainty. In this study, we evaluated the Himawari-8 global radiation product AMATERASS using observations recorded at four SKYNET stations in Japan and, for certain analyses, from the surface network of the Japanese Meteorological Agency in 2016. We found that the spatiotemporal variability of the satellite estimates was smaller than that of the ground observations; variability decreased with increases in the time step and spatial domain. Cloud variability was the main source of uncertainty in the satellite radiation estimates, followed by direct effects caused by aerosols and bright albedo. Under all-sky conditions, good agreement was found between satellite and ground-based data, with a mean bias in the range of 20–30 W m−2 (i.e., AMATERASS overestimated ground observations) and a root mean square error (RMSE) of approximately 70–80 W m−2. However, results depended on the time step used in the validation exercise, on the spatial domain, and on the different climatological regions. In particular, the validation performed at 2.5 min showed largest deviations and RMSE values ranging from about 110 W m−2 for the mainland to a maximum of 150 W m−2 in the subtropical region. We also detected a limited overestimation in the number of clear-sky episodes, particularly at the pixel level. Overall, satellite-based estimates were higher under overcast conditions, whereas frequent episodes of cloud-induced enhanced surface radiation (i.e., measured radiation was greater than expected clear-sky radiation) tended to reduce this difference. Finally, the total mean bias was approximately 10–15 W m−2 under clear-sky conditions, mainly because of overall instantaneous direct aerosol forcing efficiency in the range of 120–150 W m−2 per unit of aerosol optical depth (AOD). A seasonal anticorrelation between AOD and global radiation differences was evident at all stations and was also observed within the diurnal cycle.

A cloud identification and profiling algorithm is being developed for the multi-spectral imager (MSI), which is one of the four instruments that the Earth Clouds, Aerosols, and Radiation Explorer (EarthCARE) spacecraft will feature. During recent work, we noticed that the MSI response function could shift substantially among some wavelengths (0.67 and 1.65 µm bands) owing to the spectral misalignment (SMILE), in which a shift in the center wavelength appears as a distortion in the spectral image. We evaluated how SMILE affects the cloud retrieval product qualitatively and quantitatively. We chose four detector pixels from bands 1 and 3 with the nadir pixel as the reference to elucidate how the SMILE error affects the cloud optical thickness (τ) and effective cloud droplet radius (re) by simulating the MSI forward radiation with Comprehensive Analysis Program for Cloud Optical Measurement (CAPCOM). We also evaluated the error in simulated scenes from a global cloud system-resolving model and a satellite simulator to measure the effect on actual observation scenes. For typical shallow warm clouds (τ = 8, re = 8 µm), the SMILE error on the cloud retrieval was not significant in most cases (up to 6 % error). For typical deep convective clouds (τ = 8, re = 40 µm), the SMILE error on the cloud retrieval was even less significant in most cases (up to 4 % error). Moreover, our results from two oceanic scenes using the synthetic MSI data agreed well with the forward radiation simulation, indicating that the SMILE error was generally within 10 %. Generally, this negligible impact of the SMILE is true for water surfaces, but it still needs to be investigated further for land surfaces in future works.

We examined potential interferences from water vapor and atmospheric background gases (N2 , O2 , and Ar), and biases by isotopologues of target species, on accurate measurement of atmospheric CO2 and CH4 by means of wavelength-scanned cavity ring-down spectroscopy (WS-CRDS). Changes of the background gas mole fractions in the sample air substantially impacted the CO2 and CH4 measurements: variation of CO2 and CH4 due to relative increase of each background gas increased as Ar < O2 < N2 , suggesting similar relation for the pressure-broadening effects (PBEs) among the background gas. The pressure-broadening coefficients due to variations in O2 and Ar for CO2 and CH4 are empirically determined from these experimental results. Calculated PBEs using the pressure-broadening coefficients are linearly correlated with the differences between the mole fractions of O2 and Ar and their ambient abundances. Although the PBEs calculation showed that impact of natural variation of O2 is negligible on the CO2 and CH4 measurements, significant bias was inferred for the measurement of synthetic standard gases. For gas standards balanced with purified air, the PBEs were estimated to be marginal (up to 0.05 ppm for CO2 and 0.01 ppb for CH4 ) although the PBEs were substantial (up to 0.87 ppm for CO2 and 1.4 ppb for CH4 ) for standards balanced with synthetic air. For isotopic biases on CO2 measurements, we compared experimental results and theoretical calculations, which showed excellent agreement within their uncertainty. We derived instrument-specific water correction functions empirically for three WS-CRDS instruments (Picarro EnviroSense 3000i, G-1301, and G-2301), and evaluated the transferability of the water correction function from G-1301 among these instruments. Although the transferability was not proven, no significant difference was found in the water vapor correction function for the investigated WS-CRDS instruments as well as the instruments reported in the past studies within the typical analytical precision at sufficiently low water concentrations (<0.7% for CO2 and <0.6% for CH4 ). For accurate measurements of CO2 and CH4 in ambient air, we concluded that WS-CRDS measurements should be performed under complete dehumidification of air samples, or moderate dehumidification followed by application of a water vapor correction function, along with calibration by natural air-based standard gases or purified air-balanced synthetic standard gases with the isotopic correction.

In response to the need for an up-to-date emissions inventory and the recent achievement of geostationary observations afforded by the Geostationary Environment Monitoring Spectrometer (GEMS) and its sister instruments, this study aims to establish a top-down approach for adjusting aerosol precursor emissions over East Asia. This study involves a series of the TROPOspheric Monitoring Instrument (TROPOMI) NO2 product, the GEMS aerosol optical depth (AOD) data fusion product and its proxy product, and chemical transport model (CTM)-based inverse modeling techniques. We begin by sequentially adjusting bottom-up estimates of nitrogen oxides (NOx) and primary particulate matter (PM) emissions, both of which significantly contribute to aerosol loadings over East Asia to reduce model biases in AOD simulations during the year 2019. While the model initially underestimates AOD by 50.73 % on average, the sequential emissions adjustments that led to overall increases in the amounts ofNOx emissions by 122.79 % and of primary PM emissions by 76.68 % and 114.63 % (single- and multiple-instrument-derived emissions adjustments, respectively) reduce the extents of AOD underestimation to 33.84 % and 19.60 %, respectively. We consider the outperformance of the model using the emissions constrained by the data fusion product to be the result of the improvement in the quantity of available data. Taking advantage of the data fusion product, we perform sequential emissions adjustments during the spring of 2022, the period during which the substantial reductions in anthropogenic emissions took place accompanied by the COVID-19 pandemic lockdowns over highly industrialized and urbanized regions in China. While the model initially overestimates surface PM2.5 concentrations by 47.58 % and 20.60 % in the North China Plain (NCP) region and South Korea (hereafter referred to as Korea), the sequential emissions adjustments that led to overall decreases in NOx and primary PM emissions by 7.84 % and 9.03 %, respectively, substantially reduce the extents of PM2.5 underestimation to 19.58 % and 6.81 %, respectively. These findings indicate that the series of emissions adjustments, supported by the TROPOMI and GEMS-involved data fusion products, performed in this study are generally effective at reducing model biases in simulations of aerosol loading over East Asia; in particular, the model performance tends to improve to a greater extent on the condition that spatiotemporally more continuous and frequent observational references are used to capture variations in bottom-up estimates of emissions. In addition to reconfirming the close association between aerosol precursor emissions and AOD as well as surface PM2.5 concentrations, the findings of this study could provide a useful basis for how to most effectively exploit multisource top-down information for capturing highly varying anthropogenic emissions.

We evaluated carbon dioxide (CO2) adsorption on the internal surface of the cylinder and the fractionation of CO2 and air during the preparation of standard mixtures with atmospheric CO2 level through multistep dilution. The CO2 molar fractions in the standard mixtures deviated from the gravimetric values by -0.207±0.060 µmolmol-1 on average, which is larger than the compatibility goal (0.1 µmolmol-1) recommended by the World Meteorological Organization. The deviation was consistent with those calculated using two fractionation factors: one was estimated by the mother–daughter transfer experiment in which CO2–air mixtures were transferred from a mother cylinder to an evacuated daughter cylinder, and another was computed by applying the Rayleigh model to the change in CO2 molar fractions in a source gas as its pressure was depleted from 11.5 to 1.1 MPa. The mother–daughter transfer experiments showed that the deviation was caused by the fractionation of CO2 and air during the transfer of the source gas (CO2–air mixture with a higher CO2 molar fraction than that in the prepared gas mixture). The CO2 fractionation was less significant when the transfer speed decreased to less than 3 L min-1, indicating that thermal diffusion mainly caused the fractionation. The CO2 adsorption on the internal cylinder surface was experimentally evaluated by emitting a CO2–air mixture from a cylinder. When the cylinder pressure was reduced from 11.0 to 0.1 MPa, the CO2 molar fractions in the mixture exiting the cylinder increased by 0.16±0.04 µmolmol-1. By applying the Langmuir adsorption–desorption model to the measured data, the amount of CO2 adsorbed on the internal surfaces of a 10 L aluminum cylinder when preparing a standard mixture with atmospheric CO2 level was estimated to be 0.027±0.004 µmolmol-1 at 11.0 MPa.