Impact of molecular spectroscopy on carbon monoxide abundances from tropomi

The impact of SEOM–IAS (Scientific Exploitation of Operational Missions–Improved Atmospheric Spectroscopy) spectroscopic information on CO columns from TROPOMI (Tropospheric Monitoring Instrument) shortwave infrared (SWIR) observations was examined. HITRAN 2016 (High Resolution Transmission) and GEISA 2015 (Gestion et Etude des Informations Spectroscopiques Atmosphériques 2015) were used as a reference upon which the spectral fitting residuals, retrieval errors and inferred quantities were assessed. It was found that SEOM–IAS significantly improves the quality of the CO retrieval by reducing the residuals to TROPOMI observations. The magnitude of the impact is dependent on the climatological region and spectroscopic reference used. The difference in the CO columns was found to be rather small, although discrepancies reveal, for selected scenes, in particular, for observations with elevated molecular concentrations. A brief comparison to Total Column Carbon Observing Network (TCCON) and Network for the Detection of Atmospheric Composition Change (NDACC) also demonstrated that both spectroscopies cause similar columns; however, the smaller retrieval errors in the SEOM with Speed-Dependent Rautian and line-Mixing (SDRM) inferred CO turned out to be beneficial in the comparison of post-processed mole fractions with ground-based references

Technical note: First spectral measurement of the Earth's upwelling emission using an uncooled wideband Fourier transform spectrometer

The first spectral measurement of Earth's emitted radiation to space in the wideband range from 100 to 1400 cm^−1 with 0.5 cm^−1 spectral resolution is presented. The measurement was performed from a stratospheric balloon in tropical region using a Fourier transform spectrometer, during a field campaign held in Brazil in June 2005. The instrument, which has uncooled components including the detector module, is a prototype developed as part of the study for the REFIR (Radiation Explorer in the Far InfraRed) space mission. This paper shows the results of the field campaign with particular attention to the measurement capabilities of the prototype. The results are compared with measurements taken by IASI-balloon (Infrared Atmospheric Sounding Interferometer – Balloon version), aboard the same platform, and with forward model estimations. The infrared signature of clouds is observed in the measurements

Technical note: First spectral measurement of the Earth's upwelling emission using an uncooled wideband Fourier transform spectrometer

International audienceThe first spectral measurement of Earth's emitted radiation to space in the wideband range from 100 to 1400 cm-1 with 0.5 cm-1 spectral resolution is presented. The measurement was performed from a stratospheric balloon in tropical region using a Fourier transform spectrometer, during a field campaign held in Brazil in June 2005. The instrument, which has uncooled components including the detector module, is a prototype developed as part of the study for the REFIR (Radiation Explorer in the Far InfraRed) space mission. This paper shows the results of the field campaign with particular attention to the measurement capabilities of the prototype. The results are compared with measurements taken by IASI-balloon (Infrared Atmospheric Sounding Interferometer – Balloon version), aboard the same platform, and with forward model estimations. The infrared signature of clouds is observed in the measurements

First spectral measurement of the Earth's upwelling emission using an uncooled wideband Fourier transform spectrometer

International audienceThe first spectral measurement of Earth's emitted radiation to space in the wideband range from 100 to 1400 cm-1 with 0.5 cm-1 spectral resolution is presented. The measurement was performed from a stratospheric balloon in tropical region using a Fourier transform spectrometer, during a field campaign held in Brazil in June 2005. The instrument, which has uncooled components including the detector module, is a prototype developed as part of the study for the REFIR (Radiation Explorer in the Far InfraRed) space mission. This paper shows the results of the field campaign with particular attention to the measurement capabilities of the prototype. The results are compared with measurements taken by IASI-balloon (Infrared Atmospheric Sounding Interferometer – Balloon version), aboard the same platform, and with forward model estimations. The infrared signature of clouds is observed in the measurements

Calibration of sealed HCl cells used for TCCON instrumental line shape monitoring

The TCCON (Total Carbon Column Observing Network) FTIR (Fourier transform infrared) network provides highly accurate observations of greenhouse gas column-averaged dry-air mole fractions. As an important component of TCCON quality assurance, sealed cells filled with approximately 5 mbar of HCl are used for instrumental line shape (ILS) monitoring at all TCCON sites. Here, we introduce a calibration procedure for the HCl cells which employs a refillable, pressure-monitored reference cell filled with C_2H_2. Using this method, we identify variations of HCl purity between the TCCON cells as a non-negligible disturbance. The new calibration procedure introduced here assigns effective pressure values to each individual cell to account for additional broadening of the HCl lines. This approach will improve the consistency of the network by significantly reducing possible station-to-station biases due to inconsistent ILS results from different HCl cells. We demonstrate that the proposed method is accurate enough to turn the ILS uncertainty into an error source of secondary importance from the viewpoint of network consistency

Validation of OMPS Suomi NPP and OMPS NOAA‐20 Formaldehyde Total Columns With NDACC FTIR Observations

We validate formaldehyde (HCHO) vertical column densities (VCDs) from Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) instruments onboard the Suomi National Polar-orbiting Partnership (Suomi NPP) satellite for 2012–2020 and National Oceanic and Atmospheric Administration-20 (NOAA-20) satellite for 2018–2020, hereafter referred to as OMPS-NPP and OMPS-N20, with ground-based Fourier-Transform Infrared (FTIR) observations of the Network for the Detection of Atmospheric Composition Change (NDACC). OMPS-NPP/N20 HCHO products reproduce seasonal variability at 24 FTIR sites. Monthly variability of OMPS-NPP/N20 has a very good agreement with FTIR, showing correlation coefficients of 0.83 and 0.88, respectively. OMPS-NPP (N20) biases averaged over all sites are −0.9 (4) ± 3 (6)%. However, at clean sites (with VCDs 4.0 × 10$^{15}$ molecules cm$^{−2}$, negative biases of −15% ± 4% appear for OMPS-NPP, but OMPS-N20 shows smaller bias of 0.5% ± 6% due to its smaller ground pixel footprints. Therefore, smaller satellite footprint sizes are important in distinguishing small-scale plumes. In addition, we discuss a bias correction and provide lower limit for the monthly uncertainty of OMPS-NPP/N20 HCHO products. The total uncertainty for OMPS-NPP (N20) at clean sites is 0.7 (0.8) × 10$^{15}$ molecules cm$^{−2}$, corresponding to a relative uncertainty of 32 (30)%. In the case of HCHO VCDs > 4.0 × 10$^{15}$ molecules cm$^{−2}$, however, the relative uncertainty in HCHO VCDs for OMPS-NPP (N20) decreases to 31 (18)%

Validation of methane and carbon monoxide from Sentinel-5 Precursor using TCCON and NDACC-IRWG stations

The Sentinel-5 Precursor (S5P) mission with the TROPOspheric Monitoring Instrument (TROPOMI) on board has been measuring solar radiation backscattered by the Earth\u27s atmosphere and surface since its launch on 13 October 2017. In this paper, we present for the first time the S5P operational methane (CH4) and carbon monoxide (CO) products\u27 validation results covering a period of about 3 years using global Total Carbon Column Observing Network (TCCON) and Infrared Working Group of the Network for the Detection of Atmospheric Composition Change (NDACC-IRWG) network data, accounting for a priori alignment and smoothing uncertainties in the validation, and testing the sensitivity of validation results towards the application of advanced co-location criteria. We found that the S5P standard and bias-corrected CH4 data over land surface for the recommended quality filtering fulfil the mission requirements. The systematic difference of the bias-corrected total column-averaged dry air mole fraction of methane (XCH4) data with respect to TCCON data is -0.26 +/- 0.56 % in comparison to -0.68 +/- 0.74 % for the standard XCH4 data, with a correlation of 0.6 for most stations. The bias shows a seasonal dependence. We found that the S5P CO data over all surfaces for the recommended quality filtering generally fulfil the missions requirements, with a few exceptions, which are mostly due to co-location mismatches and limited availability of data. The systematic difference between the S5P total column-averaged dry air mole fraction of carbon monoxide (XCO) and the TCCON data is on average 9.22 +/- 3.45 % (standard TCCON XCO) and 2.45 +/- 3.38 % (unscaled TCCON XCO). We found that the systematic difference between the S5P CO column and NDACC CO column (excluding two outlier stations) is on average 6.5 +/- 3.54 %. We found a correlation of above 0.9 for most TCCON and NDACC stations. The study shows the high quality of S5P CH4 and CO data by validating the products against reference global TCCON and NDACC stations covering a wide range of latitudinal bands, atmospheric conditions and surface conditions

Neutron-diffraction studies of amorphous CNx materials

The results of neutron-diffraction experiments performed on two samples of amorphous CNx, with nitrogen concentrations of 5 and 30 at. %, prepared by a combination of filtered cathodic are and Kaufman-type ion source, are presented. Increasing the N content of the samples is seen to cause a decrease of the average bond length and the first coordination number. An increase in the average bond angle from 113 degrees to 121 degrees is also observed. The pair-distribution functions indicate that N incorporation results in some transformation of sp(3) C sites to sp(2) sites, but there is no evidence for N inducing the formation of crystalline graphitic clusters, and the overall structure remains amorphous. A direct subtraction of the two data sets emphasizes the loss of sp(3) bonds and the increasing sp(2) character of the higher-N-content sample, and shows the occurrence of a variety of bonding environments for N. More limited information on second neighbor correlations involving N is also revealed

Carbon dioxide retrieval from OCO-2 satellite observations using the RemoTeC algorithm and validation with TCCON measurements

In this study we present the retrieval of the column-averaged dry air mole fraction of carbon dioxide (X-CO2) from the Orbiting Carbon Observatory-2 (OCO-2) satellite observations using the RemoTeC algorithm, previously successfully applied to retrieval of greenhouse gas concentration from the Greenhouse Gases Observing Satellite (GOSAT). The X-CO2, product has been validated with collocated ground-based measurements from the Total Carbon Column Observing Network (TCCON) for almost 2 years of OCO-2 data from September 2014 to July 2016. We found that fitting an additive radiometric offset in all three spec tral bands of OCO-2 significantly improved the retrieval. Based on a small correlation of the X-CO2, error over land with goodness of fit, we applied an a posteriori bias correction to our OCO-2 retrievals. In overpass averaged results, X-CO2, retrievals have an SD of similar to 1.30 ppm and a station-tostation variability of similar to 0.40 ppm among collocated TCCON sites. The seasonal relative accuracy (SRA) has a value of 0.52 ppm. The validation shows relatively larger difference with TCCON over high-latitude areas and some specific regions like Japan

Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates

Spaceborne formaldehyde (HCHO) measurements constitute an excellent proxy for the sources of non-methane volatile organic compounds (NMVOCs). Past studies suggested substantial overestimations of NMVOC emissions in state-of-the-art inventories over major source regions. Here, the QA4ECV (Quality Assurance for Essential Climate Variables) retrieval of HCHO columns from OMI (Ozone Monitoring Instrument) is evaluated against (1) FTIR (Fourier-transform infrared) column observations at 26 stations worldwide and (2) aircraft in situ HCHO concentration measurements from campaigns conducted over the USA during 2012–2013. Both validation exercises show that OMI underestimates high columns and overestimates low columns. The linear regression of OMI and aircraft-based columns gives ΩOMI=0.651Ωairc+2.95×1015 molec.cm-2, with ΩOMI and Ωairc the OMI and aircraft-derived vertical columns, whereas the regression of OMI and FTIR data gives ΩOMI=0.659ΩFTIR+2.02×1015 molec.cm-2. Inverse modelling of NMVOC emissions with a global model based on OMI columns corrected for biases based on those relationships leads to much-improved agreement against FTIR data and HCHO concentrations from 11 aircraft campaigns. The optimized global isoprene emissions (∼445Tgyr-1) are 25 % higher than those obtained without bias correction. The optimized isoprene emissions bear both striking similarities and differences with recently published emissions based on spaceborne isoprene columns from the CrIS (Cross-track Infrared Sounder) sensor. Although the interannual variability of OMI HCHO columns is well understood over regions where biogenic emissions are dominant, and the HCHO trends over China and India clearly reflect anthropogenic emission changes, the observed HCHO decline over the southeastern USA remains imperfectly elucidated.</p