The TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel 5 Precursor (S5-P) satellite provides methane (CH4) measurements with high accuracy and exceptional temporal and spatial ...resolution and sampling. TROPOMI CH4 measurements are highly valuable to constrain emissions inventories and for trend analysis, with strict requirements on the data quality. This study describes the improvements that we have implemented to retrieve CH4 from TROPOMI using the RemoTeC full-physics algorithm. The updated retrieval algorithm features a constant regularization scheme of the inversion that stabilizes the retrieval and yields less scatter in the data and includes a higher resolution surface altitude database. We have tested the impact of three state-of-the-art molecular spectroscopic databases (HITRAN 2008, HITRAN 2016 and Scientific Exploitation of Operational Missions – Improved Atmospheric Spectroscopy Databases SEOM-IAS) and found that SEOM-IAS provides the best fitting results. The most relevant update in the TROPOMI XCH4 data product is the implementation of an a posteriori correction fully independent of any reference data that is more accurate and corrects for the underestimation at low surface albedo scenes and the overestimation at high surface albedo scenes. After applying the correction, the albedo dependence is removed to a large extent in the TROPOMI versus satellite (Greenhouse gases Observing SATellite – GOSAT) and TROPOMI versus ground-based observations (Total Carbon Column Observing Network – TCCON) comparison, which is an independent verification of the correction scheme. We validate 2 years of TROPOMI CH4 data that show the good agreement of the updated TROPOMI CH4 with TCCON (−3.4 ± 5.6 ppb) and GOSAT (−10.3 ± 16.8 ppb) (mean bias and standard deviation). Low- and high-albedo scenes as well as snow-covered scenes are the most challenging for the CH4 retrieval algorithm, and although the a posteriori correction accounts for most of the bias, there is a need to further investigate the underlying cause.
Transport of carbonyl sulfide (OCS) from the troposphere to the stratosphere contributes sulfur to the stratospheric aerosol layer, which reflects incoming short‐wave solar radiation, cooling the ...climate system. Previous analyses of OCS observations have shown no significant trend, suggesting that OCS is unlikely to be a major contributor to the reported increases in stratospheric aerosol loading and indicating a balanced OCS budget. Here we present analyses of ground‐based Fourier transform spectrometer measurements of OCS at three Southern Hemisphere sites spanning 34.45°S to 77.80°S. At all three sites statistically significant positive trends are seen from 2001 to 2014 with an observed overall trend in total column OCS at Wollongong of 0.73 ± 0.03%/yr, at Lauder of 0.43 ± 0.02%/yr, and at Arrival Heights of 0.45 ± 0.05%/yr. These observed trends in OCS imply that the OCS budget is not balanced and could contribute to constraints on current estimates of sources and sinks.
Key Points
First observed positive trend in OCS in the Southern Hemisphere
Observed trends indicate imbalanced OCS budget
Temporal structure of trend is similar across middle‐ and high‐latitude sites
This paper provides an overview of the validation of National Oceanic and Atmospheric Administration (NOAA) operational retrievals of atmospheric carbon trace gas profiles, specifically carbon ...monoxide (CO), methane (CH4) and carbon dioxide (CO2), from the NOAA-Unique Combined Atmospheric Processing System (NUCAPS), a NOAA enterprise algorithm that retrieves atmospheric profile environmental data records (EDRs) under global non-precipitating (clear to partly cloudy) conditions. Vertical information about atmospheric trace gases is obtained from the Cross-track Infrared Sounder (CrIS), an infrared Fourier transform spectrometer that measures high resolution Earth radiance spectra from NOAA operational low earth orbit (LEO) satellites, including the Suomi National Polar-orbiting Partnership (SNPP) and follow-on Joint Polar Satellite System (JPSS) series beginning with NOAA-20. The NUCAPS CO, CH4, and CO2 profile EDRs are rigorously validated in this paper using well-established independent truth datasets, namely total column data from ground-based Total Carbon Column Observing Network (TCCON) sites, and in situ vertical profile data obtained from aircraft and balloon platforms via the NASA Atmospheric Tomography (ATom) mission and NOAA AirCore sampler, respectively. Statistical analyses using these datasets demonstrate that the NUCAPS carbon gas profile EDRs generally meet JPSS Level 1 global performance requirements, with the absolute accuracy and precision of CO 5% and 15%, respectively, in layers where CrIS has vertical sensitivity; CH4 and CO2 product accuracies are both found to be within ±1%, with precisions of ≈1.5% and ⪅0.5%, respectively, throughout the tropospheric column.
In a 3.5-year long study, the long-term
performance of a mobile, solar absorption Bruker EM27/SUN spectrometer, used
for greenhouse gas observations, is checked with respect to a co-located
reference ...Bruker IFS 125HR spectrometer, which is part of the Total Carbon
Column Observing Network (TCCON). We find that the EM27/SUN is stable on
timescales of several years; the drift per year between the EM27/SUN and the
official TCCON product is 0.02 ppmv for XCO2 and 0.9 ppbv for
XCH4, which is within the 1σ precision of the comparison,
0.6 ppmv for XCO2 and 4.3 ppbv for XCH4. The bias between
the two data sets is 3.9 ppmv for XCO2 and 13.0 ppbv for
XCH4. In order to avoid sensitivity-dependent artifacts, the EM27/SUN
is also compared to a truncated IFS 125HR data set derived from
full-resolution TCCON interferograms. The drift is 0.02 ppmv for
XCO2 and 0.2 ppbv for XCH4 per year, with 1σ
precisions of 0.4 ppmv for XCO2 and 1.4 ppbv for XCH4,
respectively. The bias between the two data sets is 0.6 ppmv for
XCO2 and 0.5 ppbv for XCH4. With the presented long-term
stability, the EM27/SUN qualifies as an useful supplement to the existing
TCCON network in remote areas. To achieve consistent performance, such an
extension requires careful testing of any spectrometers involved by
application of common quality assurance measures. One major aim of the
COllaborative Carbon Column Observing Network (COCCON) infrastructure is to
provide these services to all EM27/SUN operators. In the framework of COCCON
development, the performance of an ensemble of 30 EM27/SUN spectrometers was
tested and found to be very uniform, enhanced by the centralized inspection
performed at the Karlsruhe Institute of Technology prior to deployment.
Taking into account measured instrumental line shape parameters for each
spectrometer, the resulting average bias across the ensemble with respect to
the reference EM27/SUN used in the long-term study in XCO2 is
0.20 ppmv, while it is 0.8 ppbv for XCH4. The average standard
deviation of the ensemble is 0.13 ppmv for XCO2 and 0.6 ppbv for
XCH4. In addition to the robust metric based on absolute differences,
we calculate the standard deviation among the empirical calibration factors.
The resulting 2σ uncertainty is 0.6 ppmv for XCO2 and
2.2 ppbv for XCH4. As indicated by the executed long-term study on
one device presented here, the remaining empirical calibration factor deduced
for each individual instrument can be assumed constant over time. Therefore
the application of these empirical factors is expected to further improve the
EM27/SUN network conformity beyond the scatter among the empirical
calibration factors reported above.
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.
The Australian continent contributes substantially to the year-to-year variability of the global terrestrial carbon dioxide (CO
) sink. However, the scarcity of in situ observations in remote areas ...prevents the deciphering of processes that force the CO
flux variability. In this study, by examining atmospheric CO
measurements from satellites in the period 2009-2018, we find recurrent end-of-dry-season CO
pulses over the Australian continent. These pulses largely control the year-to-year variability of Australia's CO
balance. They cause two to three times larger seasonal variations compared with previous top-down inversions and bottom-up estimates. The pulses occur shortly after the onset of rainfall and are driven by enhanced soil respiration preceding photosynthetic uptake in Australia's semiarid regions. The suggested continental-scale relevance of soil-rewetting processes has substantial implications for our understanding and modeling of global climate-carbon cycle feedbacks.
Understanding greenhouse gas–climate processes and feedbacks is a fundamental step in understanding climate variability and its links to greenhouse gas fluxes. Chemical transport models are the ...primary tool for linking greenhouse gas fluxes to their atmospheric abundances. Hence, accurate simulations of greenhouse gases are essential. Here, we present a new simulation in the GEOS-Chem chemical transport model that couples the two main greenhouse gases—carbon dioxide (CO2) and methane (CH4)—along with the indirect greenhouse gas carbon monoxide (CO) based on their chemistry. Our updates include the online calculation of the chemical production of CO from CH4 and the online production of CO2 from CO, both of which were handled offline in the previous versions of these simulations. In the newly developed coupled (online) simulation, we used consistent hydroxyl radical (OH) fields for all aspects of the simulation, resolving biases introduced by inconsistent OH fields in the currently available uncoupled (offline) CH4, CO and CO2 simulations. We compare our coupled simulation with the existing v12.1.1 GEOS-Chem uncoupled simulations run the way they are currently being used by the community. We discuss differences between the uncoupled and coupled calculation of the chemical terms and compare our results with surface measurements from the NOAA Global Greenhouse Gas Reference Network (NOAA GGGRN), total column measurements from the Total Carbon Column Observing Network (TCCON) and aircraft measurements from the Atmospheric Tomography Mission (ATom). Relative to the standard uncoupled simulations, our coupled results suggest a stronger CO chemical production from CH4, weaker production of CO2 from CO and biases in the OH fields. However, we found a significantly stronger chemical production of CO2 in tropical land regions, especially in the Amazon. The model–measurement differences point to underestimated biomass burning emissions and secondary production for CO. The new self-consistent coupled simulation opens new possibilities when identifying biases in CH4, CO and CO2 source and sink fields, as well as a better understanding of their interannual variability and co-variation.
The Total Carbon Column Observing Network (TCCON) is a global network dedicated to the precise and accurate measurements of greenhouse gases (GHG) in the atmosphere. The TCCON station in Burgos, ...Ilocos Norte, Philippines was established with the primary purpose of validating the upcoming Greenhouse gases Observing SATellite-2 (GOSAT-2) mission and in general, to respond to the need for reliable ground-based validation data for satellite GHG observations in the region. Here, we present the first 4 months of data from the new TCCON site in Burgos, initial comparisons with satellite measurements of C O 2 and model simulations of C O . A nearest sounding from Japan’s GOSAT as well as target mode observations from NASA’s Orbiting Carbon Observatory 2 (OCO-2) showed very good consistency in the retrieved column-averaged dry air mole fractions of C O 2 , yielding TCCON - satellite differences of 0.86 ± 1.06 ppm for GOSAT and 0.83 ± 1.22 ppm for OCO-2. We also show measurements of enhanced C O , probably from East Asia. GEOS-Chem model simulations were used to study the observed C O variability. However, despite the model capturing the pattern of the C O variability, there is an obvious underestimation in the C O magnitude in the model. We conclude that more measurements and modeling are necessary to adequately sample the variability over different seasons and to determine the suitability of current inventories.
In Australia, bushfires are a natural part of the country’s landscape and essential for the regeneration of plant species; however, the 2019–20 bushfires were unprecedented in their extent and ...intensity. This paper is focused on the 2019–20 Australian bushfires and the resulting surface and column atmospheric carbon monoxide (CO) anomalies around Wollongong. Column CO data from the ground-based Total Carbon Column Observing Network (TCCON) and Network for the Detection of Atmospheric Composition Change (NDACC) site in Wollongong are used together with surface in situ measurements. A systematic comparison was performed between the surface in situ and column measurements of CO to better understand whether column measurements can be used as an estimate of the surface concentrations. If so, satellite column measurements of CO could be used to estimate the exposure of humans to CO and other fire-related pollutants. We find that the enhancements in the column measurements are not always significantly evident in the corresponding surface measurements. Topographical features play a key role in determining the surface exposures from column abundance especially in a coastal city like Wollongong. The topography at Wollongong, combined with meteorological effects, potentially exacerbates differences in the column and surface. Hence, satellite column amounts are unlikely to provide an accurate reflection of exposure at the ground during major events like the 2019–2020 bushfires.
In this study, we present the assimilation of data from the Orbiting Carbon Observatory-2 (OCO-2) (land nadir and glint data, version 9) to estimate the Australian carbon surface fluxes for the year ...2015. To perform this estimation, we used both a regional-scale atmospheric transport–dispersion model and a four-dimensional variational assimilation scheme. Our results suggest that Australia was a carbon sink of -0.41 ± 0.08 PgC yr-1 compared to the prior estimate 0.09 ± 0.20 PgC yr-1 (excluding fossil fuel emissions). Most of the carbon uptake occurred in northern Australia over the savanna ecotype and in the western region over areas with sparse vegetation. Analysis of the enhanced vegetation index (EVI) suggests that the majority of the carbon uptake over the savanna ecosystem was due to an increase of vegetation productivity (positive EVI anomalies) amplified by an anomalous increase of rainfall in summer. Further from this, a slight increase of carbon uptake in Western Australia over areas with sparse vegetation (the largest ecosystem in Australia) was noted due to increased land productivity in the area caused by positive rainfall anomalies. The stronger carbon uptake estimate in this ecosystem was partially due to the land surface model (CABLE-BIOS3) underestimating the gross primary productivity of the ecosystem. To evaluate the accuracy of our carbon flux estimates from OCO-2 retrievals, we compare our posterior concentration fields against the column-averaged carbon retrievals from the Total Carbon Column Observing Network (TCCON) and ground-based in situ monitoring sites located around our domain. The validation analysis against TCCON shows that our system is able to reduce bias mainly in the summer season. Comparison with surface in situ observations was less successful, particularly over oceanic monitoring sites that are strongly affected by oceanic fluxes and subject to less freedom by the inversion. For stations located far from the coast, the comparison with in situ data was more variable, suggesting difficulties matching the column-integrated and surface data by the inversion, most likely linked to model vertical transport. Comparison of our fluxes against the OCO-2 model intercomparison (MIP) was encouraging. The annual carbon uptake estimated by our inversion falls within the ensemble of the OCO-2 MIP global inversions and presents a similar seasonal pattern.
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