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The TROPOspheric Monitoring Instrument (TROPOMI) provides a daily, spatially resolved (initially 7×7 km 2 , upgraded to 7×5.6 km 2 in August 2019) global dataset of CO columns; however, due to the relative sparseness of reliable ground-based data sources, it can be challenging to characterize the validity and accuracy of satellite data products in remote regions such as the high Arctic. In these regions, satellite intercomparisons can supplement model- and ground-based validation efforts and serve to verify previously observed differences. In this paper, we compare the CO products from TROPOMI, the Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer (FTS), and a high-Arctic ground-based FTS located at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut (80.05 ∘ N, 86.42 ∘ W). A global comparison of TROPOMI reference profiles scaled by the retrieved total column with ACE-FTS CO partial columns for the period from 28 November 2017 to 31 May 2020 displays excellent agreement between the two datasets (R=0.93) and a small relative bias of -0.83±0.26% (bias ± standard error of the mean). Additional comparisons were performed within five latitude bands: the north polar region (60 to 90 ∘ N), northern mid-latitudes (20 to 60 ∘ N), the equatorial region (20 ∘ S to 20 ∘ N), southern mid-latitudes (60 to 20 ∘ S), and the south polar region (90 to 60 ∘ S). Latitudinal comparisons of the TROPOMI and ACE-FTS CO datasets show strong correlations ranging from R=0.93 (southern mid-latitudes) to R=0.86 (equatorial region) between the CO products but display a dependence of the mean differences on latitude. Positive mean biases of 7.93±0.61% and 7.21±0.52% were found in the northern and southern polar regions, respectively, while a negative bias of -9.41±0.55% was observed in the equatorial region. To investigate whether these differences are introduced by cloud contamination, which is reflected in the TROPOMI averaging kernel shape, the latitudinal comparisons were repeated for cloud-covered pixels and clear-sky pixels only, as well as for the unsmoothed and smoothed cases. Clear-sky pixels were found to be biased higher with poorer correlations on average than clear + cloudy scenes and cloud-covered scenes only. Furthermore, the latitudinal dependence on the biases was observed in both the smoothed and unsmoothed cases. To provide additional context to the global comparisons of TROPOMI with ACE-FTS in the Arctic, both satellite datasets were compared against measurements from the ground-based PEARL-FTS. Comparisons of TROPOMI with smoothed PEARL-FTS total columns in the period of 3 March 2018 to 27 March 2020 display a strong correlation (R=0.88); however, a positive mean bias of 14.7±0.16% was also found. A partial column comparison of ACE-FTS with the PEARL-FTS in the period from 25 February 2007 to 18 March 2020 shows good agreement (R=0.79) and a mean positive bias of 7.89±0.21% in the ACE-FTS product relative to the ground-based FTS. The magnitude and sign of the mean relative differences are consistent across all intercomparisons in this work, as well as with recent ground-based validation efforts, suggesting that the current TROPOMI CO product exhibits a positive bias in the high-Arctic region. However, the observed bias is within the TROPOMI mission accuracy requirement of ±15% , providing further confirmation that the data quality in these remote high-latitude regions meets this specification. [ABSTRACT FROM AUTHOR]

This paper reports on ground-based validation of the atmospheric OClO data record produced in the framework of EUMETSAT's Satellite Application Facility on Atmospheric Chemistry Monitoring (AC SAF) using the GOME2-A and -B instruments over the 2007-2016 and 2013-2016 periods, respectively. OClO slant column densities are compared to correlative measurements collected from 9 NDACC Zenith-Scattered-Light DOAS (ZSL-DOAS) instruments distributed in both the Arctic and Antarctic. Sensitivity tests are performed on the ground-based data to estimate the impact of the different OClO DOAS analysis settings. On this basis, we infer systematic uncertainties of about 25 % between the different ground-based data analysis, reaching total uncertainties ranging from about 26 % to 33 % for the different stations. Time-series at the different sites show good agreement between satellite and ground-based data, both for the inter-annual variability and the overall OClO seasonal behavior. GOME-2A results are found to be nosier than those of GOME-2B, especially after 2011, probably due to instrumental degradation effects. Daily linear regression analysis for OClO activated periods yield correlation coefficients of 0.8 for GOME-2A and 0.87 for GOME-2B, with slopes of 0.64 and 0.72, respectively. Biases are within 8 x 1013 molec/cm2 with some differences between GOME-2A and GOME- 2B, depending on the station. Overall, considering all the stations, a median bias of about -2.2 x 1013 molec/cm2 is found for both GOME-2 instruments. [ABSTRACT FROM AUTHOR]

The GEOS-Chem simulation of atmospheric CH4 was evaluated against observations from the Thermal and Near Infrared Sensor for Carbon Observations Fourier Transform Spectrometer (TANSO-FTS) on the Greenhouse Gases Observing Satellite (GOSAT), the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and the Total Carbon Column Observing Network (TCCON). We focused on the model simulations at the 4∘×5∘ and 2∘×2.5∘ horizontal resolutions for the period of February–May 2010. Compared to the GOSAT, TCCON, and ACE-FTS data, we found that the 2∘×2.5∘ model produced a better simulation of CH4 , with smaller biases and a higher correlation to the independent data. We found large resolution-dependent differences such as a latitude-dependent XCH4 bias, with higher column abundances of CH4 at high latitudes and lower abundances at low latitudes at the 4∘×5∘ resolution than at 2∘×2.5∘. We also found large differences in CH4 column abundances between the two resolutions over major source regions such as China. These differences resulted in up to 30 % differences in inferred regional CH4 emission estimates from the two model resolutions. We performed several experiments using 222Rn , 7Be , and CH4 to determine the origins of the resolution-dependent errors. The results suggested that the major source of the latitude-dependent errors is excessive mixing in the upper troposphere and lower stratosphere, including mixing at the edge of the polar vortex, which is pronounced at the 4∘×5∘ resolution. At the coarser resolution, there is weakened vertical transport in the troposphere at midlatitudes to high latitudes due to the loss of sub-grid tracer eddy mass flux in the storm track regions. The vertical air mass fluxes are calculated in the model from the degraded coarse-resolution wind fields and the model does not conserve the air mass flux between model resolutions; as a result, the low resolution does not fully capture the vertical transport. This produces significant localized discrepancies, such as much greater CH4 abundances in the lower troposphere over China at 4∘×5∘ than at 2∘×2.5∘. Although we found that the CH4 simulation is significantly better at 2∘×2.5∘ than at 4∘×5∘ , biases may still be present at 2∘×2.5∘ resolution. Their importance, particularly in regards to inverse modeling of CH4 emissions, should be evaluated in future studies using online transport in the native general circulation model as a benchmark simulation. [ABSTRACT FROM AUTHOR]

The primary instrument on the Greenhouse gases Observing SATellite (GOSAT) is the Thermal And Near infrared Sensor for carbon Observations (TANSO) Fourier transform spectrometer (FTS). TANSO-FTS uses three shortwave infrared (SWIR) bands to retrieve total columns of CO2 and CH4 along its optical line of sight and one thermal infrared (TIR) channel to retrieve vertical profiles of CO2 and C< volume mixing ratios (VMRs) in the troposphere. We examine version 1 of the TANSO-FTS TIR CH4 product by comparing co-located CH4 VMR vertical profiles from two other remote-sensing FTS systems: the Canadian Space Agency's Atmospheric Chemistry Experiment FTS (ACEFTS) on SCISAT (version 3.5) and the European Space Agency's Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat (ESA ML2PP version 6 and IMK-IAA reduced-resolution version V5R_CH4_224/225), as well as 16 ground stations with the Network for the Detection of Atmospheric Composition Change (NDACC). This work follows an initial inter-comparison study over the Arctic, which incorporated a ground-based FTS at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Canada, and focuses on tropospheric and lowerstratospheric measurements made at middle and tropical latitudes between 2009 and 2013 (mid-2012 for MIPAS). For comparison, vertical profiles from all instruments are interpolated onto a common pressure grid, and smoothing is applied to ACE-FTS, MIPAS, and NDACC vertical profiles. Smoothing is needed to account for differences between the vertical resolution of each instrument and differences in the dependence on a priori profiles. The smoothing operators use the TANSO-FTS a priori and averaging kernels in all cases. We present zonally averaged mean CH4 differences between each instrument and TANSO-FTS with and without smoothing, and we examine their information content, their sensitive altitude range, their correlation, their a priori dependence, and the variability within each data set. Partial columns are calculated from the VMR vertical profiles, and their correlations are examined. We find that the TANSO-FTS vertical profiles agree with the ACE-FTS and both MIPAS retrievals' vertical profiles within 4% (± ~ 40 ppbv) below 15 km when smoothing is applied to the profiles from instruments with finer vertical resolution but that the relative differences can increase to on the order of 25% when no smoothing is applied. Computed partial columns are tightly correlated for each pair of data sets. We investigate whether the difference between TANSO-FTS and other CH4 VMR data products varies with latitude. Our study reveals a small dependence of around 0.1% per 10 degrees latitude, with smaller differences over the tropics and greater differences towards the poles. [ABSTRACT FROM AUTHOR]

The primary instrument on the Greenhouse gases Observing SATellite (GOSAT) is the Thermal And Near infrared Sensor for carbon Observations (TANSO) Fourier Transform Spectrometer (FTS). TANSO-FTS uses three short-wave infrared (SWIR) bands to retrieve total columns of CO2 and CH4 along its optical line-of-sight, and one thermal infrared (TIR) channel to retrieve vertical profiles of CO2 and CH4 volume mixing ratios (VMRs) in the troposphere. We examine version 1 of the TANSO-FTS TIR CH4 product by comparing co-located CH4 VMR vertical profiles from two other remote sensing FTS systems: the Canadian Space Agency's Atmospheric Chemistry Experiment-FTS (ACE-FTS) on SCISAT (version 3.5), and the European Space Agency's Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat (ESA ML2PP version 6 and IMK-IAA reduced-resolution version V5R_CH4_224/225), as well as 16 ground stations with the Network for the Detection of Atmospheric Composition Change (NDACC). This work follows an initial inter-comparison study over the Arctic, which incorporated a ground-based FTS at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Canada, and focuses on tropospheric and lower-stratospheric measurements made at middle and tropical latitudes between 2009 to 2013 (mid 2012 for MIPAS). For comparison, vertical profiles from all instruments are interpolated onto a common pressure grid, and the ACE-FTS, MIPAS, and NDACC vertical profiles are smoothed using the TANSO-FTS averaging kernels. We present zonally-averaged mean CH4 differences between each instrument and TANSO-FTS with and without smoothing, examine their information content, sensitive altitude range, correlation, a priori dependence, and the variability within each data set. Partial columns are calculated from the VMR vertical profiles, and their correlations are examined. We find that the TANSO-FTS vertical profiles agree with the ACE-FTS and both MIPAS retrievals' vertical profiles within 4% below 15km when smoothing is applied to the profiles from instruments with finer vertical resolution, but that the relative differences can increase to on the order of 25% when no smoothing is applied. Computed partial columns are tightly correlated for each pair of data sets. We investigated whether the difference between TANSO-FTS and other CH4 VMR data products varies with latitude. Our study reveals a small dependence of around 0.1% per ten degrees latitude, with smaller differences over the equator, and greater differences towards the poles. [ABSTRACT FROM AUTHOR]

This paper presents eight years (2006-2013) of measurements obtained from Fourier Transform Spectrometers (FTSs) in the high Arctic at the Polar Environment Atmospheric Research Laboratory (PEARL, 80.05°N, 86.42°W). These measurements were taken as part of the Canadian Arctic ACE (Atmospheric Chemistry Experiment) Validation Campaigns that have been carried out since 2004 during the polar sunrise period (from mid-February to mid-April). Each spring, two ground-based FTSs were used to measure total and partial columns of HF, O3, and trace gases that impact O3 depletion, namely, HCl, and HNO3. Additionally, some tropospheric greenhouse gases and pollutant species were measured, namely CH4, N2O, CO, and C2H6. During the same time period, the satellite-based ACE-FTS made measurements near Eureka and provided profiles of the same trace gases. Comparisons have been carried out between the measurements from PARIS-IR and the co-located high-resolution Bruker 125HR FTS, as well as with the latest version of the ACE-FTS retrievals (v3.5). The total column comparison between the two co-located ground-based FTSs, PARIS-IR and Bruker 125HR, found very good agreement for most of these species (except HF), with differences well below the estimated uncertainties (~6%) and with high correlations (R≥0.8). Partial columns have been used for the ground-based to space-borne comparison, with coincident measurements selected based on time, distance and scaled potential vorticity (sPV). The comparisons of the ground-based measurements with ACE-FTS show good agreement in the partial columns for most species within 6% (except for C2H6 and PARIS-IR HF), which are consistent with the total retrieval uncertainty of the ground-based instruments. The correlation coefficients (R) of the partial column comparisons for all eight species range from approximately 0.75 to 0.95. The comparisons show no significant increase in the mean differences over these eight years, indicating the consistency of these datasets and suggesting that the space-borne ACE-FTS measurements have been stable over this period. In addition, changes in the amounts of these trace gases during springtime between 2006 and 2013 are presented and discussed. Increased O3 (0.9%yr-1), HCl (1.7%yr-1), HF (3.8%yr-1), CH4 (0.5%yr-1) and C2H6 (2.3%yr-1, 2009-2013) have been found near PEARL from the Portable Atmospheric Research Interferometric Spectrometer for the InfraRed (PARIS-IR) dataset. [ABSTRACT FROM AUTHOR]

Motivated by the initial selection of a high-resolution solar occultation Fourier transform spectrometer (FTS) to fly to Mars on the ExoMars Trace Gas Orbiter, we have been developing algorithms for retrieving volume mixing ratio vertical profiles of trace gases, the primary component of which is a new algorithm and software for retrieving vertical profiles of temperature and pressure from the spectra. In contrast to Earth-observing instruments, which can rely on accurate meteorological models, a priori information, and spacecraft position, Mars retrievals require a method with minimal reliance on such data. The temperature and pressure retrieval algorithms developed for this work were evaluated using Earth-observing spectra from the Atmospheric Chemistry Experiment (ACE) FTS, a solar occultation instrument in orbit since 2003, and the basis for the instrument selected for a Mars mission. ACE-FTS makes multiple measurements during an occultation, separated in altitude by 1.5-5 km, and we analyse 10 CO2 vibration-rotation bands at each altitude, each with a different usable altitude range. We describe the algorithms and present results of their application and their comparison to the ACE-FTS data products. The Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC) provides vertical profiles of temperature up to 40 km with high vertical resolution. Using six satellites and GPS radio occultation, COSMIC's data product has excellent temporal and spatial coverage, allowing us to find coincident measurements with ACE with very tight criteria: less than 1.5 h and 150 km. We present an intercomparison of temperature profiles retrieved from ACE-FTS using our algorithm, that of the ACE Science Team (v3.5), and from COSMIC. When our retrievals are compared to ACE-FTS v3.5, we find mean differences between -5 and +2K and that our retrieved profiles have no seasonal or zonal biases but do have a warm bias in the stratosphere and a cold bias in the mesosphere. When compared to COSMIC, we do not observe a warm/cool bias and mean differences are between -4 and +1K. COSMIC comparisons are restricted to below 40 km, where our retrievals have the best agreement with ACE-FTS v3.5. When comparing ACE-FTS v3.5 to COSMIC we observe a cold bias in COSMIC of 0.5 K, and mean differences are between -0.9 and +0.6 K. [ABSTRACT FROM AUTHOR]

This paper reports on ground-based validation of the atmospheric OClO data record produced within the framework of EUMETSAT's Satellite Application Facility on Atmospheric Chemistry Monitoring (AC SAF) using the Global Ozone Monitoring Experiment (GOME)-2A and GOME-2B instrument measurements, covering the 2007–2016 and 2013–2016 periods, respectively. OClO slant column densities are compared to correlative measurements collected from nine Zenith-Scattered-Light Differential Optical Absorption Spectroscopy (ZSL-DOAS) instruments from the Network for the Detection of Atmospheric Composition Change (NDACC) distributed in both the Arctic and Antarctic. Sensitivity tests are performed on the ground-based data to estimate the impact of the different OClO DOAS analysis settings. On this basis, we infer systematic uncertainties of about 25 % (i.e., about 3.75×1013 molec. cm -2) between the different ground-based data analyses, reaching total uncertainties ranging from about 26 % to 33 % for the different stations (i.e., around 4 to 5×1013 molec. cm -2). Time series at the different sites show good agreement between satellite and ground-based data for both the inter-annual variability and the overall OClO seasonal behavior. GOME-2A results are found to be noisier than those of GOME-2B, especially after 2011, probably due to instrumental degradation effects. Daily linear regression analysis for OClO-activated periods yield correlation coefficients of 0.8 for GOME-2A and 0.87 for GOME-2B, with slopes with respect to the ground-based data ensemble of 0.64 and 0.72, respectively. Satellite minus ground-based offsets are within 8×1013 molec. cm -2 , with some differences between GOME-2A and GOME-2B depending on the station. Overall, considering all the stations, a median offset of about -2.2×1013 molec. cm -2 is found for both GOME-2 instruments. [ABSTRACT FROM AUTHOR]