Search

The atmospheric concentration of CFC-11 (CCl3F) has declined in response to the phase-out of its production by the Montreal Protocol. Nevertheless, this atmospheric concentration decline suffered a slow-down around 2012 due to emissions from non-reported production. Since CFC-11 is one of the most important ozone-depleting chlorofluorocarbons (CFCs), its continuous monitoring is essential. We present the CFC-11 total column time series (2000-2020) retrieved in a consistent way from ground-based high-resolution solar absorption Fourier transform infrared (FTIR) spectra. These observations were recorded at two remote stations of the Network for the Detection of Atmospheric Composition Change (NDACC): the Jungfraujoch station (Northern Hemisphere) and the Lauder station (Southern Hemisphere). These time series are new. They were produced using improved line parameters and merged considering the instrument changes and setup modifications. Afterwards, they were compared with Cape Grim station in situ surface observations conducted within the Advanced Global Atmospheric Gases Experiment (AGAGE) network and with total column datasets calculated by the TOMCAT/SLIMCAT 3-D chemical transport model. Trend analyses were performed, using an advanced statistical tool, in order to identify the timing and magnitude of the trend change in both hemispheres. The observations are consistent with the model results and confirm the slowdown in the CFC-11 atmospheric concentration decay, since ≈2011 in the Northern Hemisphere, and since ≈2014 in the Southern Hemisphere.

Ground-based observations are indispensable for the long-term monitoring of atmospheric constituents. In this work, we take advantage of multiple collocated instruments to analyze potential biases and drifts in ground-based ozone observations, within the context of the HEGIFTOM (Harmonization and Evaluation of Ground-based Instruments for Free Tropospheric Ozone Measurements) working group in the Tropospheric Ozone Assessment Report, Phase II (TOAR-II). This work is performed at Lauder (New Zealand), Boulder (Colorado), and Mauna Loa (Hawaii) where comparisons are made between Fourier Transform Infrared (FTIR) spectroscopy, Dobson Umkehr, and ozonesonde observations. The validation is performed with respect to FTIR as arbitrary reference, while considering the differences between the a priori profile information for the techniques that employ these as well as accounting for the different vertical resolution of each measurement technique. Such intercomparison is done for a handful discrete altitude partial columns, defined to have independent pieces of information also in the case of the low vertical resolution techniques (FTIR and Umkehr). This leads to 4 independent vertical layers to be compared, including one in the troposphere where ozone plays an important role as a greenhouse gas and as a risk to human health. In this tropospheric layer we compare the FTIR, Dobson Umkehr and ozonesonde techniques and derive a consistent bias from the FTIR data of about 5%, which we attribute in part to the assumed spectroscopy. Fitting the time series of the relative measurement differences using multiple linear regression, we obtain a linear trend, which quantifies the drift between pairs of techniques. Within the uncertainties, we find no significant drift between FTIR and Umkehr or ozone sonde data in the troposphere.

The presence of reactive bromine in polar regions is a widespread phenomenon that plays an important role in the photochemistry of the Arctic and Antarctic lower troposphere, including the destruction of ozone, the disturbance of radical cycles, and the oxidation of gaseous elemental mercury. The chemical mechanisms leading to the heterogeneous release of gaseous bromine compounds from saline surfaces are in principle well understood. There are, however, substantial uncertainties about the contribution of different potential sources to the release of reactive bromine, such as sea ice, brine, aerosols, and the snow surface, as well as about the seasonal and diurnal variation and the vertical distribution of reactive bromine. Here we use continuous long-term measurements of the vertical distribution of bromine monoxide (BrO) and aerosols at the two Antarctic sites Neumayer (NM) and Arrival Heights (AH), covering the periods of 2003–2021 and 2012–2021, respectively, to investigate how chemical and physical parameters affect the abundance of BrO. We find the strongest correlation between BrO and aerosol extinction (R=0.56 for NM and R=0.28 for AH during spring), suggesting that the heterogeneous release of Br2 from saline airborne particles (blowing snow and aerosols) is a dominant source for reactive bromine. Positive correlations between BrO and contact time of air masses, both with sea ice and the Antarctic ice sheet, suggest that reactive bromine is not only emitted by the sea ice surface but by the snowpack on the ice shelf and in the coastal regions of Antarctica. In addition, the open ocean appears to represent a source for reactive bromine during late summer and autumn when the sea ice extent is at its minimum. A source–receptor analysis based on back trajectories and sea ice maps shows that main source regions for BrO at NM are the Weddell Sea and the Filchner–Ronne Ice Shelf, as well as coastal polynyas where sea ice is newly formed. A strong morning peak in BrO frequently occurring during summer and that is particularly strong during autumn suggests a night-time build-up of Br2 by heterogeneous reaction of ozone on the saline snowpack in the vicinity of the measurement sites. We furthermore show that BrO can be sustained for at least 3 d while travelling across the Antarctic continent in the absence of any saline surfaces that could serve as a source for reactive bromine.

The Antarctic ozone hole remains the focus of scientific attention because of its importance to the health of the biosphere and its influence on the climate of the southern hemisphere. Here we examine the general characteristics of the 2020 Antarctic ozone hole using a variety of observational and reanalysis data and compare and contrast its behaviour with earlier years. The main feature of the 2020 ozone hole was its relatively large size, and persistence to the beginning of the 2020/2021 summer, with new maximum records being set for the ozone hole daily area and ozone mass deficit during November and December. This was in strong contrast to 2019 when the ozone hole was one of the smallest observed. We show that a key factor in 2020 was the relative stability and strength of the stratospheric polar vortex, which allowed low temperatures in the Antarctic lower stratosphere to enhance ozone depletion reactions in relative isolation from the rest of the global atmosphere. These conditions were associated with relatively weak Rossby wave activity at high southern latitudes that occurred during the strengthening westerly phase of the Quasi Biennial Oscillation as well as the emerging La Niña phase of the El Niño Southern Oscillation. A consequence of the conditions in early summer was the measurement of new maximum values of ultraviolet radiation at Australia’s three Antarctic research stations of Mawson, Davis and Casey. Indications of anomalous chlorine partitioning above Arrival Heights in Antarctica prior to the 2020 winter are provided, which may relate to effects from the 2019/2020 Australian wildfires. We also examine the effect of the downward coupling of the 2020 ozone hole to the climate of the wider southern hemisphere, which showed regional influences on surface temperature and precipitation in common with other strong vortex years.

The presence of reactive bromine in polar regions is a widespread phenomenon that plays an important role in the photochemistry of the Arctic and Antarctic lower troposphere, including the destruction of ozone, the disturbance of radical cycles, and the oxidation of gaseous elemental mercury. The chemical mechanisms leading to the heterogeneous release of gaseous bromine compounds from saline surfaces are in principle well understood. There are, however, substantial uncertainties about the contribution of different potential sources to the release of reactive bromine, such as sea ice, brine, aerosols, and the snow surface, as well as about the seasonal and diurnal variation and the vertical distribution of reactive bromine. Here we use continuous long-term measurements of the vertical distribution of bromine monoxide (BrO) and aerosols at the two Antarctic sites Neumayer (NM) and Arrival Heights (AH), covering the periods of 2003–2021 and 2012–2021, respectively, to investigate how chemical and physical parameters affect the abundance of BrO. We find the strongest correlation between BrO and aerosol extinction (R=0.56 for NM and R=0.28 for AH during spring), suggesting that the heterogeneous release of Br2 from saline airborne particles (blowing snow and aerosols) is a dominant source for reactive bromine. Positive correlations between BrO and contact time of air masses, both with sea ice and the Antarctic ice sheet, suggest that reactive bromine is not only emitted by the sea ice surface but by the snowpack on the ice shelf and in the coastal regions of Antarctica. In addition, the open ocean appears to represent a source for reactive bromine during late summer and autumn when the sea ice extent is at its minimum. A source–receptor analysis based on back trajectories and sea ice maps shows that main source regions for BrO at NM are the Weddell Sea and the Filchner–Ronne Ice Shelf, as well as coastal polynyas where sea ice is newly formed. A strong morning peak in BrO frequently occurring during summer and that is particularly strong during autumn suggests a night-time build-up of Br2 by heterogeneous reaction of ozone on the saline snowpack in the vicinity of the measurement sites. We furthermore show that BrO can be sustained for at least 3 d while travelling across the Antarctic continent in the absence of any saline surfaces that could serve as a source for reactive bromine.

The analysis of biological and ecological traits has a long history in evolutionary and ecological research. However, trait data are often scattered and standardised terminology that transcends taxonomic and biogeographical context are generally missing. As part of the development of a global trait database of marine species, we collated trait information for European seaweeds and structured the data within the standardised framework of the World Register of Marine Species (WoRMS). We collected 45,175 records for 21 biologically and ecologically relevant traits of seaweeds. This resulted in a trait database for 1,745 European seaweed species of which more than half (56 %) of the records were documented at the species level, while the remaining 44 % was documented at a higher taxonomic level and subsequently inherited at lower levels. The trait database for European seaweeds will serve as a foundation for future research on diversity and evolution of seaweeds, and their responses to global changes. The data will contribute to developing detailed trait-based ecosystem models, and will be an important tool to inform marine conservation policies. The data is publicly accessible through the AlgaeTraits portal, algaetraits.org, doi: https://doi.org/10.14284/574, (AlgaeTraits, 2022).

This study presents an updated evaluation of stratospheric ozone profile trends in the 60∘ S–60∘ N latitude range over the 2000–2020 period using an updated version of the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) regression model that was used to evaluate such trends up to 2016 for the last WMO Ozone Assessment (2018). In addition to the derivation of detailed trends as a function of latitude and vertical coordinates, the regressions are performed with the datasets averaged over broad latitude bands, i.e. 60–35∘ S, 20∘ S–20∘ N and 35–60∘ N. The same methodology as in the last assessment is applied to combine trends in these broad latitude bands in order to compare the results with the previous studies. Longitudinally resolved merged satellite records are also considered in order to provide a better comparison with trends retrieved from ground-based records, e.g. lidar, ozonesondes, Umkehr, microwave and Fourier transform infrared (FTIR) spectrometers at selected stations where long-term time series are available. The study includes a comparison with trends derived from the REF-C2 simulations of the Chemistry Climate Model Initiative (CCMI-1). This work confirms past results showing an ozone increase in the upper stratosphere, which is now significant in the three broad latitude bands. The increase is largest in the Northern and Southern Hemisphere midlatitudes, with ∼2.2 ± 0.7 % per decade at ∼2.1 hPa and ∼2.1 ± 0.6 % per decade at ∼3.2 hPa respectively compared to ∼1.6 ± 0.6 % per decade at ∼2.6 hPa in the tropics. New trend signals have emerged from the records, such as a significant decrease in ozone in the tropics around 35 hPa and a non-significant increase in ozone in the southern midlatitudes at about 20 hPa. Non-significant negative ozone trends are derived in the lowermost stratosphere, with the most pronounced trends in the tropics. While a very good agreement is obtained between trends from merged satellite records and the CCMI-1 REF-C2 simulation in the upper stratosphere, observed negative trends in the lower stratosphere are not reproduced by models at southern and, in particular, at northern midlatitudes, where models report an ozone increase. However, the lower-stratospheric trend uncertainties are quite large, for both measured and modelled trends. Finally, 2000–2020 stratospheric ozone trends derived from the ground-based and longitudinally resolved satellite records are in reasonable agreement over the European Alpine and tropical regions, while at the Lauder station in the Southern Hemisphere midlatitudes they show some differences.

The COllaborative Carbon Column Observing Network (COCCON) uses low-resolution, portable EM27/SUN Fourier transform spectrometers (FTSs) to make retrievals of column-averaged dry-air mole fractions (DMFs, represented as Xgas) of CO2, CH4, CO and H2O from near-infrared solar absorption spectra. The COCCON has developed rapidly over recent years and complements the Total Carbon Column Observing Network (TCCON). In this work, we provide details of the first seasonal time series of near-infrared XCO2, XCH4 and XCO retrievals from measurements made in Antarctica during the deployment of an EM27/SUN to the Arrival Heights laboratory on Ross Island over the austral summer of 2019–2020 under the auspices of the COCCON. The DMFs of all three species were lower in Antarctica than at mid-latitude, and for XCO2 and XCO, the retrieved values were less variable. For XCH4 however, the variability was significantly greater and it was found that this was strongly correlated to the proximity of the polar vortex. In order to ensure the stability of the instrument and the traceability of the retrievals, side-by-side comparisons to the TCCON station at Lauder, New Zealand and retrievals of the instrument line shape (ILS) were made before and after the measurements in Antarctica. These indicate that, over the course of the deployment, the instrument stability was such that the change in retrieved XCO2 was well below 0.1 %. The value of these data for satellite validation is demonstrated by making comparisons with the TROPOspheric Monitoring Instrument (TROPOMI) on the Sentinel-5 precursor (S5P) satellite. The dataset is available from the COCCON central facility hosted by the ESA Atmospheric Validation Data Centre (EVDC) https://doi.org/10.48477/coccon.pf10.arrivalheights.R02 (Pollard, 2021).

We describe the change in operational instrument for the routine measurement of column-averaged dry-air mole fraction of several greenhouse gases (denoted Xgas) at the Lauder Total Carbon Column Observing Network (TCCON) site and the steps taken to demonstrate comparability between the two observation systems following a systematic methodology. Further, we intercompare retrieved Xgas values during an intensive intercomparison period during October and November 2018, when both instruments were performing optimally, and on subsequent, less frequent occasions. The average difference between the two observing systems was found to be well below the expected level of uncertainty for TCCON retrievals for all compared species. In the case of XCO2 the average difference was 0.0264±0.0465 % (0.11±0.19 µmol mol−1).

While the Montreal Protocol is reducing stratospheric ozone loss, recent increases in some ozone depleting substance (ODS) emissions have been identified that may impact southern hemisphere climate systems. In this study, we discuss characteristics of the 2018 and 2019 Antarctic ozone holes using surface in situ, satellite and reanalysis data to gain a better understanding of recent ozone variability. These ozone holes had strongly contrasting characteristics. In 2018, the Antarctic stratospheric vortex was relatively stable and cold in comparison to most years of the prior decade. This resulted in a large and persistent ozone hole that ranked in the upper-tercile of metrics quantifying Antarctic ozone depletion. In contrast, strong stratospheric warming in the spring of 2019 curtailed the development of the ozone hole, causing it to be anomalously small and of similar size to ozone holes in the 1980s. As known from previous studies, the ability of planetary waves to propagate into the stratosphere at high latitudes is an important factor that influences temperatures of the polar vortex and the overall amount of ozone loss in any particular year. Disturbance and warming of the vortex by strong planetary wave activity were the dominant factors in the small 2019 ozone hole. In contrast, planetary wave disturbances to the vortex in the winter–spring of 2018 were much weaker than in 2019. These results increase our understanding of the impact of Montreal Protocol controls on ODS and the effects of Antarctic ozone on the southern hemisphere climate system.

The paper — Seaweed ecosystems may not mitigate CO2 emissions (Gallagher et al., 2022) — claims that seaweed ecosystems are carbon sources rather than carbon sinks because ‘respiration subsidies’ (from inputs of allochthonous organic carbon) create negative net ecosystem production. That is, that seaweed ecosystems produce more CO2 than they draw down, and thus may not mitigate CO2 emissions. They make this claim using a compiled dataset which shows that, on average, seaweed ecosystems are net heterotrophic. However, their assessment is flawed and conceptually misleading as key terms are misinterpreted, the data presented are biased, and the conclusions are not supported statistically. Here we discuss four flaws in the argument presented by Gallagher et al., which we believe risk confusing further research on seaweed blue carbon and unjustifiably seeding doubt around motivations and initiatives to protect and restore seaweed forests.

A breakdown in host-bacteria relationships have been associated with the progression of a number of marine diseases and subsequent mortality events. For the Pacific oyster, Crassostrea gigas, Summer Mortality Syndrome (SMS) is one of the biggest constraints to growth of the sector and is set to expand into temperate systems as ocean temperatures rise. Currently, a lack of understanding of natural spatiotemporal dynamics of the host-bacteria relationship limits our ability to develop microbial-based monitoring approaches. Here, we characterised the associated bacterial community of C. gigas, at two Irish oyster farms, unaffected by SMS, over the course of a year. We found C. gigas harboured spatiotemporally variable bacterial community that were distinct from bacterioplankton in surrounding seawater. Whilst the majority of bacteria-oyster associations were transient and highly variable, we observed clear patterns of stability in the form of a small core consisting of six persistent Amplicon Sequence Variants (ASVs). This core made up a disproportionately large contribution to sample abundance (34 ± 0.14 %), despite representing only 0.034% of diversity across the study, and have been associated with healthy oysters in other systems. Overall, our study demonstrates the consistent features of oyster bacterial communities across spatial and temporal scales and provides an ecologically meaningful baseline to track environmental change.

The Brewer-Dobson Circulation (BDC) determines the distribution of long-lived tracers in the stratosphere; therefore, their changes can be used to diagnose changes in the BDC. We investigate decadal (2005-2018) trends of nitrous oxide (N2O) stratospheric columns (12-40 km) as measured by four Fourier transform infrared (FTIR) ground-based instruments and by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and compare them with simulations by two models: a chemistry-transport model (CTM) driven by four different reanalyses, and the Whole Atmosphere Chemistry-Climate Model (WACCM). The limited sensitivity of the FTIR instruments can hide negative N2O trends in the mid-stratosphere because of the large increase in the lowermost stratosphere. When applying the ACE-FTS sampling on model datasets, the reanalyses by the European Centre for Medium Range Weather Forecast (ECMWF) compare best with ACE-FTS, but the N2O trends are consistently exaggerated. Model sensitivity tests show that while decadal N2O trends reflect changes in transport, these trends are less significant in the northern extratropics due to the larger variability of transport over timescales shorter than two years in that region. We further investigate the N2O Transformed Eulerian Mean (TEM) budget in three model datasets. The TEM analysis shows that enhanced advection affects the stratospheric N2O trends more than changes in mixing. While no ideal observational dataset currently exists, this model study of N2O trends still provides new insights about the BDC and its changes thanks to relevant sensitivity tests and the TEM analysis.

Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and a large sulfur reservoir maintained by both direct oceanic, geologic, biogenic, and anthropogenic emissions and the oxidation of other sulfur-containing source species. It is the largest source of sulfur transported to the stratosphere during volcanically quiescent periods. Data from 22 ground-based globally dispersed stations are used to derive trends in total and partial column OCS. Middle infrared spectral data are recorded by solar-viewing Fourier transform interferometers that are operated as part of the Network for the Detection of Atmospheric Composition Change between 1986 and 2020. Vertical information in the retrieved profiles provides analysis of discreet altitudinal regions. Trends are found to have well-defined inflection points. NASA | Science Mission Directorate (SMD). Grant Numbers: NNX17AE38 G S003, 80NSSC21K0891. Natural Sciences and Engineering Research Council of Canada (NSERC); the Canadian Space Agency (CSA); Environment and Climate Change Canada (ECCC); Sorbonne Université; French Research Center CNRS; French Space Agency CNES. F.R.S.-FNRS. Grant Numbers: J.0147.18, J.0126.21. CONACYT. Grant Number: 290589. PAPIIT. Grant Number: IN111521. NIWA; New Zealand’s Ministry of Business, Innovation and Employment Strategic Science Investment Fund German research foundation. Grant Number: 268020496 German Bundesministerium für Wirtschaft und Energie (BMWi). Grant Numbers: 50EE1711A, 50EE1711D. Helmholtz Society Australian Research Council. Université de La Réunion. Grant Numbers: LACy-UMR8105, UMS3365.

The magnitude and distribution of net primary production (NPP) in the coastal ocean remains poorly constrained, particularly for shallow marine vegetation. Here, using a compilation of in situ annual NPP measurements across >400 sites in 72 geographic ecoregions, we provide global predictions of the productivity of seaweed habitats, which form the largest vegetated coastal biome on the planet. We find that seaweed NPP is strongly coupled to climatic variables, peaks at temperate latitudes, and is dominated by forests of large brown seaweeds. Seaweed forests exhibit exceptionally high per-area production rates (a global average of 656 and 1711 gC m −2 year −1 in the subtidal and intertidal, respectively), being up to 10 times higher than coastal phytoplankton in temperate and polar seas. Our results show that seaweed NPP is a strong driver of production in the coastal ocean and call for its integration in the oceanic carbon cycle, where it has traditionally been overlooked.

The Brewer-Dobson Circulation (BDC) determines the distribution of long-lived tracers in the stratosphere; therefore, their changes can be used to diagnose changes in the BDC. We evaluate decadal (2005-2018) trends of nitrous oxide (N

Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and the primary sulfur reservoir maintained by direct oceanic, geologic, biogenic and anthropogenic emissions and t...

Using multidecadal time series of ground-based and satellite Fourier transform infrared measurements of inorganic fluorine (i.e., total fluorine resident in stratospheric fluorine reservoirs), we investigate stratospheric circulation changes over the past 20 years. The representation of these changes in five modern reanalyses is further analyzed through chemical-transport model (CTM) simulations. From the observations but also from all reanalyses, we show that the inorganic fluorine is accumulating less rapidly in the Southern Hemisphere than in the Northern Hemisphere during the 21st century. Comparisons with a study evaluating the age-of-air of these reanalyses using the same CTM allow us to link this hemispheric asymmetry to changes in the Brewer-Dobson circulation (BDC), with the age-of-air of the Southern Hemisphere getting younger relative to that of the Northern Hemisphere. Large differences in simulated total columns and absolute trend values are, nevertheless, depicted between our simulations driven by the five reanalyses. Superimposed on this multidecadal change, we, furthermore, confirm a 5–7-year variability of the BDC that was first described in a recent study analyzing long-term time series of hydrogen chloride (HCl) and nitric acid (HNO3). It is important to stress that our results, based on observations and meteorological reanalyses, are in contrast with the projections of chemistry-climate models in response to the coupled increase of greenhouse gases and decrease of ozone-depleting substances, calling for further investigations and the continuation of long-term observations.

The historically large and severe wildfires in Australia from September 2019 to March 2020 are known to have injected a smoke plume into the stratosphere around New Year, due to pyro-cumulonimbus (pyro-Cb) activity, that was subsequently distributed throughout the Southern Hemisphere (SH). We show with satellite, ground based remote sensing, and in situ observations that the fires before New Year, had already a substantial impact on the SH atmosphere, starting as early as September 2019, with subsequent long-range transport of trace gas plumes in the upper-troposphere. Airborne in situ measurements above Southern Argentina in November 2019 show elevated CO mixing ratios at an altitude of 11 km and can be traced back using FLEXPART trajectories to the Australian fires in mid-November 2019. Ground based solar-FTS (Fourier Transform Spectroscopy) observations of biomass burning tracers CO, HCN and C2H6 at Lauder, South Island, New Zealand show enhanced tropospheric columns already starting in September 2019. In MLS observations averaged over 30°–60°S, enhanced CO mixing ratios compared to previous years become visible in late October 2019 only at and below the 147 hPa pressure level. Peak differences are found with satellite and ground-based observations for all altitude levels in the Southern Hemisphere in January. With still increased aerosol values following the Ulawun eruption in 2019, averaged satellite observations show no clear stratospheric and upper-tropospheric aerosol enhancements from the Australian fires, before the pyro-Cb events at the end of December 2019. However, with the clear enhancement of fire tracers, we suggest the period September to December 2019 (prior to the major pyro-Cb events) should be taken into account in terms of fire pollutant emissions when studying the impact of the Australian fires on the SH atmosphere.

Column-averaged dry-air mole fraction of CO (XCO) measurements are obtained from two ground-based Fourier transform infrared (FTIR) spectrometer networks: the Total Carbon Column Observing Network (TCCON) and the Network for the Detection of Atmospheric Composition Change (NDACC). In this study, the differences between the TCCON and NDACC XCO measurements are investigated and discussed based on six NDACC–TCCON sites using data over the period 2007–2017. A direct comparison shows that the NDACC XCO measurements are about 5.5 % larger than the TCCON data at Ny-Ålesund, Bremen, and Izaña (Northern Hemisphere), and the absolute bias between the NDACC and TCCON data is within 2 % at Saint-Denis, Wollongong and Lauder (Southern Hemisphere). The hemispheric dependence of the bias is mainly attributed to their smoothing errors. The systematic smoothing error of the TCCON XCO data varies in the range between 0.2 % (Bremen) and 7.9 % (Lauder), and the random smoothing error varies in the range between 2.0 % and 3.6 %. The systematic smoothing error of NDACC data is between 0.1 % and 0.8 %, and the random smoothing error of NDACC data is about 0.3 %. For TCCON data, the smoothing error is significant because it is higher than the reported uncertainty, particularly at Southern Hemisphere sites. To reduce the influence from the a priori profiles and different vertical sensitivities, the scaled NDACC a priori profiles are used as the common a priori profiles for comparing TCCON and NDACC retrievals. As a result, the biases between TCCON and NDACC XCO measurements become more consistent (5.6 %–8.5 %) with a mean value of 6.8 % at these sites. To determine the sources of the remaining bias, regular AirCore measurements at Orléans and Sodankylä are compared to co-located TCCON measurements. It is found that TCCON XCO measurements are 6.1 ± 1.6 % and 8.0 ± 3.2 % smaller than the AirCore measurements at Orléans and Sodankylä, respectively, indicating that the scaling factor of TCCON XCO data should be around 1.0000 instead of 1.0672. Further investigations should be carried out in the TCCON community to determine the correct scaling factor to be applied to the TCCON XCO data. This paper also demonstrates that the smoothing error must be taken into account when comparing FTIR XCO data, and especially TCCON XCO data, with model or satellite data.

Atmospheric observations of CO2 and other greenhouse gases have been widely used to constrain estimates of terrestrial and oceanic CO2 fluxes through atmospheric inverse modelling. Yet, applying these methods at national scale to verify and improve the National Inventory Report (NIR) and support the Paris agreement remains at the frontier of CO2 science.We use inverse modelling to estimate New Zealand’s carbon uptake and emissions using atmospheric measurements and model. This effort is part of a five year CarbonWatch-NZ research programme, which aims to develop a complete top-down picture of New Zealand's carbon balance using national inverse modelling and targeted studies of New Zealand’s forest, grassland and urban environments. In addition to quantifying New Zealand’s carbon emissions on a national scale, we also focus on identifying the prevailing processes driving CO2 changes in New Zealand to support climate mitigation.In an initial study based on the inversion system used in CarbonWatch-NZ, a significantly stronger (30-60 %) sink was found relative to the NIR (Steinkamp et al., 2017), suggesting a strong CO2 uptake in Fiordland, a region covered by indigenous temperate rainforest in New Zealand's South Island. Here, we present new results of CarbonWatch-NZ by expanding the studied time period from 2011-2013 to 2020, expanding our atmospheric observing network from two (Baring Head, 41.41°S, 174.87°E and Lauder, 38.33°S, 176.38°E) to a total of eleven in situ greenhouse gas measurement sites and improving our atmospheric model resolution by roughly a factor of ten (NAME model, 1.5 km).Our new results suggest that the strong sink observed in 2011-2013 did not diminish, but for recent years we have found an even stronger sink than for before. Additional measurements collected in the Fiordland region (i.e., mixing ratios, CO2 isotopes, carbonyl sulphide) also suggest a stronger CO2 uptake, supporting our inversion results. Both the measurements and inversion results show that the CO2 uptake does not seem to shut down completely during winter time, suggesting that there might be something about this ecosystem that we do not yet understand. This winter uptake signal is also present in independent data collected in and around New Zealand as part of the ATom campaigns (Atmospheric Tomography Mission). Implementing observations from an additional site in the North Island (Maunga Kakaramea, 45.034°S, 169.68°E) has increased the strength of the sink, pointing to additional strong sink region at the top of the North Island. ReferencesKay Steinkamp, Sara E. Mikaloff Fletcher, Gordon Brailsford, Dan Smale, Stuart Moore, Elizabeth D. Keller, W. Troy Baisden, Hitoshi Mukai and Britton B. Stephens, Atmospheric CO2 observations and models suggest strong carbon uptake by forests in New Zealand, Atmospheric Chemistry and Physics, 2017.

The Sentinel-5 Precursor (S5P) mission with the TROPOspheric Monitoring Instrument (TROPOMI) onboard has been measuring solar radiation backscattered by the Earth's atmosphere and its surface since its launch on 13 October 2017. Methane (CH4) and carbon monoxide (CO) data with a spatial resolution (initially 7 x 7 km2, upgraded to 5.5 x 7 km2 on 6th of August 2019) have been retrieved from shortwave infrared (SWIR) and near-infrared (NIR) measurements since the end of November 2017 and made available to the experts for early validation and quality checks before the official product release. In this paper, we present for the first time the S5P CH4 and CO validation results (covering a period from November 2017 to September 2020) 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 required bias (systematic error) of 1.5 % and random error of 1 % for the S5P standard and bias-corrected methane data are met for measurements over land surfaces with pixels having quality assurance (QA) value > 0.5. The systematic difference between the S5P standard XCH4 and TCCON data is on average −0.69 ± 0.73 %. The systematic difference changes to a value of −0.25 ± 0.57 % for the S5P bias-corrected XCH4 data. We found a correlation of above 0.6 for most stations, which is mostly dominated by the seasonal cycle. The contributions of smoothing uncertainty at the individual stations are estimated and found to be dependent on the location. The highest contribution of the smoothing uncertainty is observed for mid-latitude TCCON stations and high latitude stations for NDACC. A seasonal dependency of the relative bias is seen. We observe a high bias during the springtime measurements at high SZA and a decreasing bias with increasing SZA for the rest of the year.We found that the required bias (systematic error) of 15 % and random error of < 10 % for the S5P carbon monoxide data are met in general for measurements over all surfaces with pixels having quality assurance value of > 0.5. There are a few stations where this is not the case, mostly due to co-location mismatches and the limited availability of co-located data. We compared the S5P XCO data with respect to standard TCCON XCO and unscaled TCCON XCO (without application of the empirical scaling factor) data sets. The systematic difference between the S5P XCO and the TCCON data is on average 9.14 ± 3.33 % (standard TCCON XCO data) and 2.36 ± 3.22 % (unscaled TCCON XCO data). We found that the systematic difference between the S5P CO column and NDACC CO column data (excluding two stations that were obvious outliers) is on average 6.44 ± 3.79 %. We found a correlation of above 0.9 for most TCCON and NDACC stations indicating that the temporal variations in CO column captured by the ground-based instruments are reproduced very similarly by the S5P CO column. The contribution of smoothing uncertainty at the individual stations is estimated and found to be significant. They are found to be dependent on the location with large changes seen for stations located in the Southern Hemisphere as compared to the Northern Hemisphere and at highly polluted stations. A cone co-location criterion, which gives a better match between the ground-based instrument's line-of-sight and satellite pixels, seems to give better results for high latitude stations and stations located close to emission sources. The validation results for the clear-sky and cloud cases of S5P pixels are comparable to the validation results including all pixels with quality assurance value of > 0.5. We observe that the relative bias increases with increasing SZA. We estimated this increase is about 10 % over the complete range of measurement SZAs.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.

Solar trackers are often used by spectrometers to measure atmospheric trace gas concentrations using direct sun spectroscopy. The ideal solar tracker should be sufficiently accurate, highly reliable, and with a longevity that exceeds the lifetime of the spectrometer that it serves. It should also be affordable, easy to use, and not too complex should maintenance be required. In this paper we present a design that fulfils these requirements using some simple innovations. Our altitude–azimuth design features a custom coaxial power transformer, enabling continuous 360∘ azimuth rotation. This increases reliability and avoids the need to reverse the tracker each day. In polar regions, measurements can continue uninterrupted through the summer polar day. Tracking accuracy is enhanced using a simple optical feedback technique that adjusts error offset variables while monitoring the edges of a focused solar image with four photodiodes. Control electronics are modular, and our software is written in Python, running as a web server on a recycled laptop with a Linux operating system. Over a period of 11 years we have assembled four such trackers. These are in use at Lauder (45∘ S), New Zealand, and Arrival Heights (78∘ S), Antarctica, achieving a history of good reliability even in polar conditions. Tracker accuracy is analysed regularly and can routinely produce a pointing accuracy of 0.02∘.

We describe the change of operational instrument for the routine measurement of column-averaged dry-air mole fraction of several greenhouse gases (denoted Xgas) at the Lauder Total Carbon Column Observing Network (TCCON) site and the steps taken to demonstrate comparability between the two observation systems following a systematic methodology. Further, we intercompare retrieved Xgas values during an intensive intercomparison period during October and November 2018, when both instruments were performing optimally, and on subsequent, less frequent occasions. The average difference between the two observing systems was found to be well below the expected level of uncertainty for TCCON retrievals for all compared species. In the case of XCO2 the average difference was 0.0264 ± 0.0465 % (0.11 ± 0.19 μmol mol−1).

Although optical components in Fourier transform infrared (FTIR) spectrometers are preferably wedged, in practice, infrared spectra typically suffer from the effects of optical resonances (“channeling”) affecting the retrieval of weakly absorbing gases. This study investigates the level of channeling of each FTIR spectrometer within the Network for the Detection of Atmospheric Composition Change (NDACC). Dedicated spectra were recorded by more than twenty NDACC FTIR spectrometers using a laboratory mid-infrared source and two detectors. In the InSb detector domain (1900–5000 cm−1), we find that the amplitude of the most pronounced channeling frequency amounts to 0.1 to 2.0 ‰ of the spectral background level, with a mean of (0.68 ± 0.48) ‰ and a median of 0.60 ‰. In the HgCdTe detector domain (700–1300 cm−1), we find even stronger effects, with the largest amplitude ranging from 0.3 to 21 ‰ with a mean of (2.45 ± 4.50) ‰ and a median of 1.2 ‰. For both detectors, the leading channeling frequencies are 0.9 and 0.11 or 0.23 cm−1 in most spectrometers. These observed spectral frequencies correspond to the optical thickness of the air gap in between the beam splitter and compensator plate (0.9 cm−1) and the beam splitter substrate itself (0.11 and 0.23 cm−1). Since the air gap is a significant source of channeling and the corresponding amplitude differs strongly between spectrometers, we propose new beam splitters with the wedge of the air gap increased to at least 0.8°. We tested the insertion of spacers in a beam splitter’s air gap to demonstrate that increasing the wedge of the air gap decreases the 0.9 cm−1 channeling amplitude significantly. This study shows the potential for reducing channeling in the FTIR spectrometers operated by the NDACC, thereby increasing the quality of recorded spectra across the network.

We review the 2017 Antarctic ozone hole, making use of various meteorological reanalyses, and in-situ, satellite and ground-based measurements of ozone and related trace gases, and ground-based measurements of ultraviolet radiation. The 2017 ozone hole was associated with relatively high-ozone concentrations over the Antarctic region compared to other years, and our analysis ranked it in the smallest 25% of observed ozone holes in terms of size. The severity of stratospheric ozone loss was comparable with that which occurred in 2002 (when the stratospheric vortex exhibited an unprecedented major warming) and most years prior to 1989 (which were early in the development of the ozone hole). Disturbances to the polar vortex in August and September that were associated with intervals of anomalous planetary wave activity resulted in significant erosion of the polar vortex and the mitigation of the overall level of ozone depletion. The enhanced wave activity was favoured by below-average westerly winds at high southern latitudes during winter, and the prevailing easterly phase of the quasi-biennial oscillation (QBO). Using proxy information on the chemical make-up of the polar vortex based on the analysis of nitrous oxide and the likely influence of the QBO, we suggest that the concentration of inorganic chlorine, which plays a key role in ozone loss, was likely similar to that in 2014 and 2016, when the ozone hole was larger than that in 2017. Finally, we found that the overall severity of Antarctic ozone loss in 2017 was largely dictated by the timing of the disturbances to the polar vortex rather than interannual variability in the level of inorganic chlorine.

Man-made halogenated compounds emitted from the Earth’s surface ultimately reach the stratosphere where they undergo photolysis, leading to three main fluorine reservoirs: hydrogen fluoride (HF), carbonyl fluoride (COF2) and carbonyl chloride fluoride (COClF). This process is directly influenced by the strength of the mean meridional circulation of the stratosphere, the Brewer-Dobson Circulation (BDC). The BDC is projected to speed-up with the greenhouse gases induced global warming. However, studies have highlighted a multiyear variability in the strength of the BDC resulting in hemispheric asymmetries in observed and modelled trends of age of air and long-lived tracers.Total inorganic fluorine (Fy, the fluorine weighted sum of HF, COF2 and COClF) is used here as a tracer of the stratospheric circulation changes. We perform an analysis and interpretation of Fourier transform infrared (FTIR) multidecadal time-series of HF and COF2 from the Jungfraujoch (Switzerland, 46.55°N) and Lauder (New-Zealand, 45.03°S) stations and from the space-borne Atmospheric Chemistry Experiment - Fourier Transform Spectrometer (ACE-FTS). Indeed, the summation of HF and COF2 is a very good proxy of Fy as we determine, from ACE-FTS and the chemical-transport model (CTM) TOMCAT, that COClF is only accounting for less than 5% of the total Fy budget.The kinematic CTM BASCOE (Belgian assimilation system for chemical observations) is used here to assess the representation of the investigated circulation changes in four state-of-the-art meteorological reanalyses, i.e., ERA-Interim, JRA-55, MERRA and MERRA-2. We also investigate if WACCM4 (Whole Atmosphere Community Climate Model version 4) is able to reproduce these changes through a free-running simulation.The ground-based and satellite FTIR time-series of COF2 show contrasting results over their common time period (2004-2019), with a positive total column trend above the Jungfraujoch, and a non-significant (ground-based) or decreasing trend (ACE-FTS) above Lauder. We find large discrepancies between the BASCOE-CTM simulations, with MERRA-2 inducing overly large simulated Fy total columns which could confirm the weaker tropical upwelling highlighted in previous age of air studies.

During 2016 and again during 2019 through 2020 an EM27/SUN portable near infrared solar absorption Fourier Transform Spectrometer of the Karlsruhe Institute of Technology was transported first to Lauder, New Zealand (45.034S, 169.68E, alt. 370 m) and then to the Arrival Heights laboratory, Ross Island Antarctica (77.82S, 166.65E, 200 m). On the first occasion the EM27/SUN made the first ever near infrared solar absorption retrievals of carbon dioxide and methane in Antarctica over a period of two weeks. The second deployment had the aim of making retrievals in Antarctica throughout the 2019-2020 Austral summer.We report on the comparison of retrievals of carbon dioxide and methane from the EM27 spectra with those made by the Total Carbon Column Observing Network (TCCON) stations at both Karlsruhe and Lauder and compare with similar comparisons made throughout the Collaborative Carbon Column Observing Network (COCCON), as well as the latitudinal extension of these measurements to Antarctica.Further comparisons with observations from TROPOMI instrument on the Sentinel 5 precursor satellite will be discussed.

TROPOMI (the TROPOspheric Monitoring Instrument), on-board the Sentinel-5 Precursor satellite, has been monitoring the Earth's atmosphere since October 2017, with an unprecedented horizontal resolution (initially 7×3.5 km2, upgraded to 5.5×3.5 km2 since August 2019). Monitoring air quality is one of the main objectives of TROPOMI, with the measurements of important pollutants such as nitrogen dioxide, carbon monoxide, and formaldehyde (HCHO). In this paper we assess the quality of the latest HCHO TROPOMI products (version 1.1.[5-7]), using ground-based solar-absorption FTIR (Fourier Transform Infrared) measurements of HCHO from twenty-five stations around the world, including high, mid, and low latitude sites. Most of these stations are part of the Network for the Detection of Atmospheric Composition Change (NDACC), and they provide a wide range of observation conditions from very clean remote sites to those with high HCHO levels from anthropogenic or biogenic emissions. The ground-based HCHO retrieval settings have been optimized and harmonized at all the stations, ensuring a consistent validation among the sites. In this validation work, we first assess the accuracy of TROPOMI HCHO tropospheric columns, using the median of the relative differences between TROPOMI and FTIR ground-based data (BIAS). We observe that, at all sites, the TROPOMI accuracy is below the upper limit of the pre-launch requirements of 80 %, and below the lower limit of 40 % for 20 of the 25 stations. The provided TROPOMI systematic uncertainties are well in agreement with the observed biases at most of the stations, except for the highest HCHO levels site where it is found to be underestimated. We find that, while the BIAS has no latitudinal dependence, it is dependent on the HCHO concentration levels: an overestimation (+26 &pm; 5 %) of TROPOMI is observed for very small HCHO levels ( 8.0 × 1015 molec/cm2). This demonstrates the great value of such a harmonized network covering a wide range of concentration levels, the sites with high HCHO concentrations being crucial for the determination of the satellite bias at the regions of emissions, and the clean sites allowing a small TROPOMI offset to be determined. The wide range of sampled HCHO levels within the network allows the robust determination of the significant constant and proportional TROPOMI HCHO biases (TROPOMI=+ 1.10 (&pm; 0.05) × 1015+ 0.64 (&pm; 0.03) × FTIR, in molec/cm2). Second, the precision of TROPOMI HCHO data is estimated by the median absolute deviation (MAD) of the relative differences between TROPOMI and FTIR ground-based data. The clean sites are especially useful to minimize a possible additional collocation error. The precision requirement of 1.2 × 1016 molec/cm2 for a single pixel is reached at most of the clean sites, where it is found that the TROPOMI precision can even be twice better (0.5–0.8 × 1015 molec/cm2 for a single pixel). However, we find that the provided TROPOMI random uncertainties may be underestimated by a factor of 1.6 (for clean sites) to 2.3 (for high HCHO levels). The correlation is very good between TROPOMI and FTIR data (R = 0.88 for 3 hours-mean coincidences; R = 0.91 for monthly means coincidences). Using about 17 months of data (from May 2018 to September 2019), we show that the TROPOMI seasonal variability is in very good agreement at all of the FTIR sites. The FTIR network demonstrates the very good quality of the TROPOMI HCHO products which is well within the pre-launch requirements for both accuracy and precision. This paper advises for a refinement of the TROPOMI random uncertainty budget and of the TROPOMI quality assurance values for a better filtering of the remaining outliers.

TROPOMI (the TROPOspheric Monitoring Instrument), on board the Sentinel-5 Precursor (S5P) satellite, has been monitoring the Earth's atmosphere since October 2017 with an unprecedented horizontal resolution (initially 7 km2×3.5 km2, upgraded to 5.5 km2×3.5 km2 in August 2019). Monitoring air quality is one of the main objectives of TROPOMI; it obtains measurements of important pollutants such as nitrogen dioxide, carbon monoxide, and formaldehyde (HCHO). In this paper we assess the quality of the latest HCHO TROPOMI products versions 1.1.(5-7), using ground-based solar-absorption FTIR (Fourier-transform infrared) measurements of HCHO from 25 stations around the world, including high-, mid-, and low-latitude sites. Most of these stations are part of the Network for the Detection of Atmospheric Composition Change (NDACC), and they provide a wide range of observation conditions, from very clean remote sites to those with high HCHO levels from anthropogenic or biogenic emissions. The ground-based HCHO retrieval settings have been optimized and harmonized at all the stations, ensuring a consistent validation among the sites. In this validation work, we first assess the accuracy of TROPOMI HCHO tropospheric columns using the median of the relative differences between TROPOMI and FTIR ground-based data (BIAS). The pre-launch accuracy requirements of TROPOMI HCHO are 40 %–80 %. We observe that these requirements are well reached, with the BIAS found below 80 % at all the sites and below 40 % at 20 of the 25 sites. The provided TROPOMI systematic uncertainties are well in agreement with the observed biases at most of the stations except for the highest-HCHO-level site, where it is found to be underestimated. We find that while the BIAS has no latitudinal dependence, it is dependent on the HCHO concentration levels: an overestimation (+26±5 %) of TROPOMI is observed for very low HCHO levels (<2.5×1015 molec. cm−2), while an underestimation (-30.8%±1.4 %) is found for high HCHO levels (>8.0×1015 molec. cm−2). This demonstrates the great value of such a harmonized network covering a wide range of concentration levels, the sites with high HCHO concentrations being crucial for the determination of the satellite bias in the regions of emissions and the clean sites allowing a small TROPOMI offset to be determined. The wide range of sampled HCHO levels within the network allows the robust determination of the significant constant and proportional TROPOMI HCHO biases (TROPOMI =+1.10±0.05 ×1015+0.64±0.03 × FTIR; in molecules per square centimetre). Second, the precision of TROPOMI HCHO data is estimated by the median absolute deviation (MAD) of the relative differences between TROPOMI and FTIR ground-based data. The clean sites are especially useful for minimizing a possible additional collocation error. The precision requirement of 1.2×1016 molec. cm−2 for a single pixel is reached at most of the clean sites, where it is found that the TROPOMI precision can even be 2 times better (0.5–0.8×1015 molec. cm−2 for a single pixel). However, we find that the provided TROPOMI random uncertainties may be underestimated by a factor of 1.6 (for clean sites) to 2.3 (for high HCHO levels). The correlation is very good between TROPOMI and FTIR data (R=0.88 for 3 h mean coincidences; R=0.91 for monthly means coincidences). Using about 17 months of data (from May 2018 to September 2019), we show that the TROPOMI seasonal variability is in very good agreement at all of the FTIR sites. The FTIR network demonstrates the very good quality of the TROPOMI HCHO products, which is well within the pre-launch requirements for both accuracy and precision. This paper makes suggestions for the refinement of the TROPOMI random uncertainty budget and TROPOMI quality assurance values for a better filtering of the remaining outliers.

The El Niño–Southern Oscillation (ENSO) has been suggested as a strong forcing in the methane cycle and as a driver of recent trends in global atmospheric methane mole fractions [CH4]. Such a sensitivity of the global CH4 budget to climate events would have important repercussions for climate change mitigation strategies and the accuracy of projections for future greenhouse forcing. Here, we test the impact of ENSO on atmospheric CH4 in a correlation analysis. We use local and global records of [CH4], as well as stable carbon isotopic records of atmospheric CH4 (δ13CH4), which are particularly sensitive to the combined ENSO effects on CH4 production from wetlands and biomass burning. We use a variety of nominal, smoothed, and detrended time series including growth rate records. We find that at most 36 % of the variability in [CH4] and δ13CH4 is attributable to ENSO, but only for detrended records in the southern tropics. Trend-bearing records from the southern tropics, as well as all studied hemispheric and global records, show a minor impact of ENSO, i.e. CH4 production that responds less to ENSO than previously suggested. Dynamics of the removal by hydroxyl likely counteract the variation in emissions, but the expected isotope signal is not evident. It is possible that other processes obscure the ENSO signal, which itself indicates a minor influence of the latter on global CH4 emissions. Trends like the recent rise in atmospheric [CH4] can therefore not be attributed to ENSO. This leaves anthropogenic methane sources as the likely driver, which must be mitigated to reduce anthropogenic climate change.

Among the more than 20 ground-based FTIR (Fourier transform infrared) stations currently operating around the globe, only a few have provided formaldehyde (HCHO) total column time series until now. Although several independent studies have shown that the FTIR measurements can provide formaldehyde total columns with good precision, the spatial coverage has not been optimal for providing good diagnostics for satellite or model validation. Furthermore, these past studies used different retrieval settings, and biases as large as 50 % can be observed in the HCHO total columns depending on these retrieval choices, which is also a weakness for validation studies combining data from different ground-based stations.For the present work, the HCHO retrieval settings have been optimized based on experience gained from past studies and have been applied consistently at the 21 participating stations. Most of them are either part of the Network for the Detection of Atmospheric Composition Change (NDACC) or under consideration for membership. We provide the harmonized settings and a characterization of the HCHO FTIR products. Depending on the station, the total systematic and random uncertainties of an individual HCHO total column measurement lie between 12 % and 27 % and between 1 and 11×1014 molec cm−2, respectively. The median values among all stations are 13 % and 2.9×1014 molec cm−2 for the total systematic and random uncertainties.This unprecedented harmonized formaldehyde data set from 21 ground-based FTIR stations is presented and its comparison with a global chemistry transport model shows consistency in absolute values as well as in seasonal cycles. The network covers very different concentration levels of formaldehyde, from very clean levels at the limit of detection (few 1013 molec cm−2) to highly polluted levels (7×1016 molec cm−2). Because the measurements can be made at any time during daylight, the diurnal cycle can be observed and is found to be significant at many stations. These HCHO time series, some of them starting in the 1990s, are crucial for past and present satellite validation and will be extended in the coming years for the next generation of satellite missions.

Presented here is the validation of the CrIS (Cross-track Infrared Sounder) fast physical NH3 retrieval (CFPR) column and profile measurements using ground-based Fourier transform infrared (FTIR) observations. We use the total columns and profiles from seven FTIR sites in the Network for the Detection of Atmospheric Composition Change (NDACC) to validate the satellite data products. The overall FTIR and CrIS total columns have a positive correlation of r = 0.77 (N = 218) with very little bias (a slope of 1.02). Binning the comparisons by total column amounts, for concentrations larger than 1.0 × 1016 molecules cm−2, i.e. ranging from moderate to polluted conditions, the relative difference is on average ∼ 0–5 % with a standard deviation of 25–50 %, which is comparable to the estimated retrieval uncertainties in both CrIS and the FTIR. For the smallest total column range (