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EM27/SUN devices are portable solar-viewing Fourier transform spectrometers (FTSs) that are being widely used to constrain measurements of greenhouse gas emissions and validate satellite trace gas measurements. On a 6-week-long campaign in the summer of 2018, four EM27/SUN devices were taken to five Total Carbon Column Observing Network (TCCON) stations in North America, to measure side by side, to better understand their durability, the accuracy and precision of retrievals from their trace gas measurements, and to constrain site-to-site bias among TCCON sites. We developed new EM27/SUN data products using both previous and current versions of the retrieval algorithm (GGG2014 and GGG2020) and used coincident AirCore measurements to tie the gas retrievals to the World Meteorological Organization (WMO) trace gas standard scales. We also derived air-mass-dependent correction factors for the EM27/SUN devices. Pairs of column-averaged dry-air mole fractions (denoted with an X) measured by the EM27/SUN devices remained consistent compared to each other during the entire campaign, with a 10 min averaged precision of 0.3 ppm (parts per million) for XCO 2 , 1.7 ppb (parts per billion) for XCH 4 , and 2.5 ppb for XCO. The maximum biases between TCCON stations were reduced in GGG2020 relative to GGG2014 from 1.3 to 0.5 ppm for XCO 2 and from 5.4 to 4.3 ppb for XCH 4 but increased for XCO from 2.2 to 6.1 ppb. The increased XCO biases in GGG2020 are driven by measurements at sites influenced by urban emissions (Caltech and the Armstrong Flight Research Center) where the priors overestimate surface CO. In addition, in 2020, one EM27/SUN instrument was sent to the Canadian Arctic TCCON station at Eureka, and side-by-side measurements were performed in March–July. In contrast to the other TCCON stations that showed an improvement in the biases with the newer version of GGG, the biases between Eureka's TCCON measurements and those from the EM27/SUN degraded with GGG2020, but this degradation was found to be caused by a temperature dependence in the EM27/SUN oxygen retrievals that is not apparent in the GGG2014 retrievals. [ABSTRACT FROM AUTHOR]

Measurements of Pollution In The Troposphere (MOPITT) is an instrument on NASA's Terra satellite that has measured tropospheric carbon monoxide (CO) from early 2000 to the present day. Validation of data from satellite instruments like MOPITT is often conducted using ground-based measurements to ensure the continued accuracy of the space-based instrument's measurements and its scientific results. Previous MOPITT validation studies generally found a larger bias in the MOPITT data poleward of 60 ∘ N. In this study, we use data from 2006 to 2019 from the Bruker IFS 125HR Fourier Transform Infrared spectrometer (FTIR) located at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut, Canada, to validate the MOPITT version 8 (V8) retrievals. These comparisons utilize mid- and near-infrared FTIR measurements made as part of the Network for the Detection for Atmospheric Composition Change (NDACC) and the Total Carbon Column Observing Network (TCCON), respectively. All MOPITT version 8 retrievals within a radius of 110 km (1 ∘) from the PEARL Ridge Laboratory and within a 24 h time interval are used in this validation study. MOPITT retrieval products include those from the near-infrared (NIR) channel, the thermal infrared (TIR) channel, and a joint product from the thermal and near-infrared (TIR–NIR) channels. Each channel's detector has 4 pixels. We calculated the MOPITT pixel-to-pixel biases for each pixel, which were found to vary based on the season and surface type (land or water). The systematic bias for pixel 1 over land is larger than that for other pixels, which can reach up to 20 ppb. We use a small-region approximation method to find filtering criteria. We then apply the filters to the MOPITT dataset to minimize the MOPITT pixel bias and the number of outliers in the dataset. The sensitivity of each MOPITT pixel and each product is examined over the Canadian high Arctic. We then follow the methodologies recommended by NDACC and TCCON for the comparison between the FTIR and satellite total column retrievals. MOPITT averaging kernels are used to weight the NDACC and TCCON retrievals and take into account the different vertical sensitivities between the satellite and PEARL FTIR measurements. We use a modified Taylor diagram to present the comparison results from each pixel for each product over land and water with NDACC and TCCON measurements. Our results show overall consistency between MOPITT and the NDACC and TCCON measurements. When compared to the FTIR, the NIR MOPITT retrievals have a positive bias of 3 %–10 % depending on the pixel. The bias values are negative for the TIR product, with values between -5 % and 0 %. The joint TIR–NIR products show differences of -4 % to 7 %. The drift in MOPITT biases (in units of % yr -1) relative to NDACC and TCCON varies by MOPITT data product. In the NIR, drifts vs. TCCON are smaller than those vs. NDACC; however, this scenario is reversed for the MOPITT TIR and joint TIR–NIR products. Overall, this study aims to provide detailed validation for MOPITT version 8 measurements in the Canadian high Arctic. [ABSTRACT FROM AUTHOR]

EM27/SUNs are portable solar-viewing Fourier Transform Spectrometers (FTSs) that are being widely used to constrain measurements of greenhouse gas emissions and validate satellite trace gas measurements. On a six-week-long campaign in the summer of 2018, four EM27/SUNs were taken to five Total Carbon Column Observing Network (TCCON) stations in North America to measure side-by-side to better understand their durability, as well as the accuracy and precision of retrievals from their trace gas measurements and to constrain site-to-site bias among TCCON sites. We developed new EM27/SUN data products using both previous and current versions of the retrieval algorithm (GGG2014 and GGG2020) and used coincident AirCore measurements to tie the gas retrievals to the World Meteorological Organization (WMO) trace gas standard scales. We also derived airmass-dependent correction factors for the EM27/SUNs. Pairs of column-averaged dry-air mole fractions (denoted with an X) measured by the EM27/SUNs remained consistent compared to each other during the entire campaign, with a 10-minute averaged precision of 0.3 ppm for XCO2, 1.7 ppb for XCH4 and 2.5 ppb for XCO. The maximum biases between TCCON stations were reduced in GGG2020 relative to GGG2014 from 1.3 ppm to 0.5 ppm for XCO2 and from 5.4 ppb to 4.3 for XCH4 but increased for XCO from 2.2 to 6.1 ppb. The increased XCO biases in GGG2020 are driven by measurements at sites influenced by urban emissions (Caltech and AFRC) where the priors overestimate surface CO. In addition in 2020, one EM27/SUN instrument was sent to the Canadian Arctic TCCON station at Eureka and side-by-side measurements were performed in March–July. In contrast to the other TCCON stations that showed an improvement in the biases with the newer version of GGG, the biases between Eureka's TCCON measurements and those from the EM27/SUN degraded with GGG2020, but this degradation was found to be caused by a temperature dependence in the EM27/SUN oxygen retrievals that is not apparent in the GGG2014 retrievals. [ABSTRACT FROM AUTHOR]

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]

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]

Improving measurements of water vapour in the upper troposphere and lower stratosphere (UTLS) is a priority for the atmospheric science community. In this work, UTLS water vapour profiles derived from Atmospheric Chemistry Experiment (ACE) satellite measurements are assessed with coincident ground-based measurements taken at a high Arctic observatory at Eureka, Nunavut, Canada. Additional comparisons to satellite measurements taken by the Atmospheric Infrared Sounder (AIRS), Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), Microwave Limb Sounder (MLS), Scanning Imaging Absorption Spectrometer for Atmospheric CHartography (SCIAMACHY), and Tropospheric Emission Spectrometer (TES) are included to put the ACE Fourier transform spectrometer (ACE-FTS) and ACE Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) results in context. Measurements of water vapour profiles at Eureka are made using a Bruker 125HR solar absorption Fourier transform infrared spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL) and radiosondes launched from the Eureka Weather Station. Radiosonde measurements used in this study were processed with software developed by the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) to account for known biases and calculate uncertainties in a well-documented and consistent manner. ACE-FTS measurements were within 11 ppmv (parts per million by volume; 13 %) of 125HR measurements between 6 and 14 km. Between 8 and 14 km ACE-FTS profiles showed a small wet bias of approximately 8 % relative to the 125HR. ACE-FTS water vapour profiles had mean differences of 13 ppmv (32 %) or better when compared to coincident radiosonde profiles at altitudes between 6 and 14 km; mean differences were within 6 ppmv (12 %) between 7 and 11 km. ACE-MAESTRO profiles showed a small dry bias relative to the 125HR of approximately 7 % between 6 and 9 km and 10 % between 10 and 14 km. ACE-MAESTRO profiles agreed within 30 ppmv (36 %) of the radiosondes between 7 and 14 km. ACE-FTS and ACE-MAESTRO comparison results show closer agreement with the radiosondes and PEARL 125HR overall than other satellite datasets – except for AIRS. Close agreement was observed between AIRS and the 125HR and radiosonde measurements, with mean differences within 5 % and correlation coefficients above 0.83 in the troposphere between 1 and 7 km. Comparisons to MLS at altitudes around 10 km showed a dry bias, e.g. mean differences between MLS and radiosondes were -25.6 %. SCIAMACHY comparisons were very limited due to minimal overlap between the vertical extent of the measurements. TES had no temporal overlap with the radiosonde dataset used in this study. Comparisons between TES and the 125HR showed a wet bias of approximately 25 % in the UTLS and mean differences within 14 % below 5 km. [ABSTRACT FROM AUTHOR]

High-resolution, laboratory, absorption spectra of the a1Δg←X3Σg- oxygen (O2) band measured using cavity ring-down spectroscopy were fitted using the Voigt and speed-dependent Voigt line shapes. We found that the speed-dependent Voigt line shape was better able to model the measured absorption coefficients than the Voigt line shape. We used these line shape models to calculate absorption coefficients to retrieve atmospheric total columns abundances of O2 from ground-based spectra from four Fourier transform spectrometers that are a part of the Total Carbon Column Observing Network (TCCON). Lower O2 total columns were retrieved with the speed-dependent Voigt line shape, and the difference between the total columns retrieved using the Voigt and speed-dependent Voigt line shapes increased as a function of solar zenith angle. Previous work has shown that carbon dioxide (CO2) total columns are better retrieved using a speed-dependent Voigt line shape with line mixing. The column-averaged dry-air mole fraction of CO2 (XCO2) was calculated using the ratio between the columns of CO2 and O2 retrieved (from the same spectra) with both line shapes from measurements taken over a 1-year period at the four sites. The inclusion of speed dependence in the O2 retrievals significantly reduces the air mass dependence of XCO2 , and the bias between the TCCON measurements and calibrated integrated aircraft profile measurements was reduced from 1 % to 0.4 %. These results suggest that speed dependence should be included in the forward model when fitting near-infrared CO2 and O2 spectra to improve the accuracy of XCO2 measurements. [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 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]

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]