Polar stratospheric clouds (PSCs) play a key role in the formation of the Antarctic ozone hole. Here, we report the first observations of the most abundant PSC composition class, NAT-containing mixtures (one of whose components is nitric acid trihydrate, NAT, particles), from measurements of a passive nadir-viewing sounder, the Infrared Atmospheric Sounding Interferometer (IASI). We show the unambiguous presence of the characteristic peak signature of small NAT particles near 820 in IASI spectra. By developing a detection method specific to the South Pole, we further demonstrate that NAT-containing PSCs can be detected systematically during the polar winter, despite a reduced sensitivity over the continent. This method allows us to obtain an innovative data set in terms of spatial and temporal sampling. With respect to the physicochemical processes at play in the Antarctic stratosphere, we show a high degree of consistency between the 2008-2024 time series of detected NAT-containing PSCs, stratospheric temperatures and total columns of nitric acid.

Abstract. Large positive anomalies of nitrous oxide (N2O) were observed in the northern hemisphere lower stratosphere in the late 2018/2019 boreal winter. Thanks to its long lifetime in the lower stratosphere, N2O is a robust tracer for stratospheric transport. This study investigates the magnitude, vertical structure, and dynamical origin of the late 2018/2019 boreal winter N2O anomaly using multiple chemical transport model simulations, chemical reanalyses, a specified-dynamics chemistry-climate model, and merged satellite observations. All datasets consistently show pronounced N2O positive anomalies in February 2019 in the northern mid-latitudes at 50 hPa. The N2O Transformed Eulerian Mean budget indicates that the N2O anomalies are primarily driven by enhanced meridional residual advection, which is in turn determined by enhanced planetary wave forcing. The extratropical effects of the quasi-biennial oscillation (QBO) determine these transport anomalies: the poleward QBO secondary circulation was unusually strong in the late 2018/2019 boreal winter, and a marked northward displacement of the zero wind line induced the enhanced planetary wave forcing. The combined strengthening of both the northward QBO secondary circulation and the planetary wave forcing led to unusually strong poleward advection in the northern lower stratosphere, which ultimately built up the N2O positive anomalies. These results indicate the value of long-lived stratospheric tracers such as N2O for diagnosing dynamically driven extreme events and for disentangling the contributions of different transport processes. We highlight the importance of the QBO teleconnections, particularly as a warming climate may change the frequency and intensity of extreme events thereby impacting these teleconnections.

Tropospheric ozone (O3) is an important short-lived climate forcer and a critical secondary air pollutant, detrimental to human health and ecosystems. It is the dominant source of the hydroxyl radical OH that is highly reactive with organic and inorganic compounds. Global tropospheric O3 concentrations have been rising considerably since the pre-industrial period as a result of the increase in the anthropogenic emissions of O3 precursors. Assessing the long-term tropospheric O3 trends is critical for understanding the impact of human activity and climate change on atmospheric chemistry. Since 2007, the IASI (Infrared Atmospheric Sounding Interferometer) instruments have been embarked on board the polar-orbiting meteorological satellites Metop-A, -B and -C. The European Organization for the Exploitation of Meteorological Satellites (EUTMETSAT) is currently reprocessing the IASI O3 dataset providing a homogeneous record of O3. In this study, we aim to assess tropospheric ozone distributions and trends on the global and regional scales for the period 2008-2023 using the homogeneous IASI O3 dataset. Comparisons of the IASI data with the Cross-track Infrared Sounder (CrIS) satellite observations are also performed.

Assessing tropospheric ozone (O3) variability is essential for understanding its impact on air quality, health, and climate change. The Infrared (IR) Atmospheric Sounding Interferometer (IASI) mission onboard the Metop platforms has been providing global measurements of O3 concentrations since 2007. This study presents the first comprehensive analysis of the 16-year O3 Climate Data Record (CDR) from IASI/Metop (2008-2023), a homogeneous dataset offering valuable insights into the variability and long-term trends of tropospheric O3. The IASI-CDR ozone product is evaluated against TROPESS (TRopospheric Ozone and its Precursors from Earth System Sounding) O3 retrievals from the Cross-track Infrared Sounder (CrIS). The comparison shows excellent agreement for total ozone (biases <1.2%, correlations >0.97) and good agreement for tropospheric ozone (biases 10 %-12 %, correlations 0.77-0.91). Comparisons with ozonesonde data indicate that IASI underestimates tropospheric ozone by 2 % in the tropics and by up to 10 % in mid and high latitudes. Drift analysis indicates the long-term temporal stability of IASI tropospheric ozone, with values below 3 % per decade globally and regionally, satisfying the stability criterion requirement. IASI data reveal a global decline in tropospheric O3 (-0.08 +/- 0.05 DU yr(-1), p=0.01), strongest in the tropics and Europe. The comparison with ozonesonde data, shows high-certainty decreases consistently observed in the tropics across all datasets (IASI, smoothed sonde, and raw sonde), supporting the robustness of the findings in this region. Vertical analysis reveals that negative trends dominate in the lower troposphere, while positive trends in the upper troposphere align with ultraviolet (UV) satellite observations. This vertical contrast highlights the importance of separating lower and upper tropospheric layers when comparing IR and UV datasets. Although discrepancies remain when considering the full tropospheric column, both UV and IR satellite instruments show a significant drop in tropospheric ozone starting in 2020, partly due to pandemic-related emission reductions. This study emphasizes the importance of long-term, consistent datasets for tracking ozone trends and the need for improved data retrieval and integration to address regional and temporal discrepancies.

The first Tropospheric Ozone Assessment Report (TOAR, 2014–2019) encountered several observational challenges that limited the confidence in estimates of the burden, short-term variability, and long-term changes of ozone in the free troposphere. One of these challenges is the difficulty to interpret the consistency of satellite measurements obtained with different techniques from multiple sensors, leading to differences in spatiotemporal sampling, vertical smoothing, a-priori information, and uncertainty characterisation. This motivated the Committee on Earth Observation Satellites (CEOS) to initiate a coordinated activity VC-20-01 on improving the assessment and harmonisation of tropospheric ozone measured from space. Here, we report on work that contributes to this CEOS activity, as well as to the ongoing second TOAR assessment (TOAR-II, 2020–2025). Our objective is to harmonise the spatiotemporal perspective of (sixteen) satellite ozone data records, thereby accounting as much as possible for differences in vertical smoothing and sampling. Four harmonisation methods are presented to achieve this goal: two for ozone profiles obtained from nadir sounders (UV-visible, IR, and combined UV-IR), and two for tropospheric ozone column products derived by one of the residual methods (Convective Cloud Differential or Limb–Nadir Matching). We discuss to what extent harmonisation may affect assessments of the spatial distribution, seasonal cycle, and long-term changes in free tropospheric ozone, and we anchor the harmonised profile data to ozonesonde measurements recently homogenised as part of TOAR-II. We find that approaches that use global ozone fields as a transfer standard (here the Copernicus Atmosphere Monitoring Service ReAnalysis, CAMSRA) to constrain the harmonisation generally lead to the largest reduction of the inter-product dispersion (IPD) between satellite datasets. These harmonisation efforts, however, only partially account for the observed discrepancies between the satellite datasets, with a reduction of about 10 %–40 % of the IPD upon harmonisation, depending on the products involved and with strong spatiotemporal dependences. This work therefore provides evidence that it is not only the differences in spatiotemporal smoothing and sampling, but rather the differences in measurement uncertainty that pose the main challenge to the assessment of the spatial distribution and temporal evolution of free tropospheric ozone from satellite observations.

Ozone in the troposphere is a prominent pollutant whose production is sensitive to the emissions of nitrogen oxides (NOx) and volatile organic compounds (VOCs). Here, we assess the variation of tropospheric ozone levels, trends, ozone photochemical regimes and radiative effects using the ECHAM6–HAMMOZ chemistry–climate model for the period 1998–2019 and satellite measurements. The global mean simulated trend in tropospheric column ozone (TRCO) for the study period (1998–2019) is 0.89 ppb decade−1. During the overlapping period with Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) observations (2005–2019), the simulated global mean TRCO trends (1.58 ppb decade−1) show fair agreement with OMI/MLS estimates (1.4 ppb decade−1). The simulations for doubling emissions of NOx (DoubNOx), VOCs (DoubVOC), and halving emissions of NOx (HalfNOx) and VOCs (HalfVOC) show nonlinear responses to ozone trends and tropospheric ozone photochemical regimes. The DoubNOx simulations show VOC-limited regimes over the Indo-Gangetic Plain, eastern China, western Europe and the eastern US, while HalfNOx simulations show NOx-limited regimes over North America and Asia. Emissions changes in NOx (DoubNOx/HalfNOx) influence the shift in tropospheric ozone photochemical regimes compared to VOCs (DoubVOC/HalfVOC). The estimated global mean TO3RE during 1998–2019 from the control (CTL) simulations is 1.21 W m−2. The global mean TO3RE shows enhancement by 0.36 W m−2 in DoubNOx simulations compared to CTL. While TO3RE shows a reduction in other simulations compared to CTL (DoubVOC: −0.005 W m−2, HalfNOx: −0.12 W m−2 and HalfVOC: −0.03 W m−2). We show that emission changes in anthropogenic NOx cause more significant changes in TO3RE than anthropogenic VOCs.

Ozone is a potent air pollutant in the lower troposphere and an important short-lived climate forcer (SLCF) in the upper troposphere. Studies investigating long-term trends in the tropospheric column ozone (TCO3) have shown large-scale spatio-temporal inconsistencies. Here, we investigate the long-term trends in lower-tropospheric column ozone (LTCO3, surface–450 hPa sub-column) by exploiting a synergy of satellite and ozonesonde data sets and an Earth system model (UK's Earth System Model, UKESM) over North America, Europe, and East Asia for the decade 2008–2017. Overall, we typically find small LTCO3 linear trends with large uncertainty ranges using the Ozone Monitoring Instrument (OMI) and the Infrared Atmospheric Sounding Interferometer (IASI), while model simulations indicate a stable LTCO3 tendency. The satellite a priori data sets show negligible trends, indicating that any year-to-year changes in the spatio-temporal sampling of these satellite data sets over the period concerned have not artificially influenced their LTCO3 temporal evolution. The application of the satellite averaging kernels (AKs) to the UKESM simulated ozone profiles, accounting for the satellite vertical sensitivity and allowing for like-for-like comparisons, has a limited impact on the modelled LTCO3 tendency in most cases. While, in relative terms, this is more substantial (e.g. on the order of 100 %), the absolute magnitudes of the model trends show negligible change. However, as the model has a near-zero tendency, artificial trends were imposed on the model time series (i.e. LTCO3 values rearranged from smallest to largest) to test the influence of the AKs, but simulated LTCO3 trends remained small. Therefore, the LTCO3 tendencies between 2008 and 2017 in northern-hemispheric regions are likely to be small, with large uncertainties, and it is difficult to detect any small underlying linear trends due to interannual variability or other factors which require further investigation (e.g. the radiative transfer scheme (RTS) used and/or the inputs (e.g. meteorological fields) used in the RTS).

Using state-of-the-art satellite ozone profile products, and a chemical transport model, we provide an updated estimate of the tropospheric ozone radiative effect (TO3RE) and observational constraint on its variability over the decade 2008–2017. Previous studies have shown the short-term (i.e. a few years) globally weighted average TO3RE to be 1.17 ± 0.03 W m−2. However, from our analysis, using decadal (2008–2017) ozone profile datasets from the Infrared Atmospheric Sounding Interferometer, average TO3RE ranges between 1.21 and 1.26 W m−2. Over this decade, the modelled and observational TO3RE linear trends show a negligible change (e.g. ± 0.1 % yr−1). Two model sensitivity experiments fixing emissions and meteorology to 1 year (i.e. start year – 2008) show that temporal changes in ozone precursor emissions (increasing contribution) and meteorological factors (decreasing contribution) have counteracting tendencies, leading to a negligible globally weighted average TO3RE trend.

&lt;p&gt;As part of the Ozone and Precursors in the Tropics (OPT) working group of the Tropospheric Ozone Assessment Report Phase 2 (TOAR-II), we present the first results on the distribution of tropospheric ozone (O3) and its precursors (carbon monoxide, CO; formaldehyde, HCHO; nitrogen dioxide, NO2) in the tropics over the past 20-25 years. The goal is to give an overview of the seasonal, geographical and vertical variabilities of tropical tropospheric O3 and its precursors. To do so, we use in situ measurements of O3 and its precursors from surface sites, sounding balloons (SHADOZ) and instrumented aircraft (IAGOS and ATOM), as well as ground-based (FTIR) and spatial (IASI, OMI, GOME-2) remote-sensed observations. The observations are averaged monthly over the longest available time-period as well as over the first five years of the time period. The results for these two time periods give the context to interpret distributions and variabilities of O3 and its precursors over the most recent five years as we call it &amp;#8220;Present-day&amp;#8221;. &amp;#160;Special emphasis is given to the differences of O3 and its precursors&amp;#8217; distributions between remote and polluted regions and to the relationships between the gaseous species. Model output will be included to fill gaps in space and time when necessary to help the interpretation of the analysis based on observations.&lt;/p&gt;&lt;p&gt;From IAGOS measurements, the highest O3 and CO maxima occur in the lower troposphere of Northern Hemisphere Africa, which remains the most influenced by biomass burning. CO maxima are attributed using SOFT-IO model to anthropogenic emissions by 60%. Second maxima are observed in the lower troposphere of Asia, mostly due to anthropogenic emissions. The highest amount of transported CO in the tropics originates from Africa.&lt;/p&gt;

In this paper, we exploit the first 10-year data record (2008–2017) of nitric acid (HNO3) total columns measured by the IASI-A/MetOp infrared sounder, characterized by an exceptional daily sampling and a good vertical sensitivity in the lower-to-mid stratosphere (around 50 hPa), to monitor the relationship between the temperature decrease and the observed HNO3 loss that occurs each year in the Antarctic stratosphere during the polar night. Since the HNO3 depletion results from the formation of polar stratospheric clouds (PSCs), which trigger the development of the ozone (O3) hole, its continuous monitoring is of high importance. We verify here, from the 10-year time evolution of HNO3 together with temperature (taken from reanalysis at 50 hPa), the recurrence of specific regimes in the annual cycle of IASI HNO3 and identify (for each year) the day and the 50 hPa temperature (“drop temperature”) corresponding to the onset of strong HNO3 depletion in the Antarctic winter. Although the measured HNO3 total column does not allow for the uptake of HNO3 by different types of PSC particles along the vertical profile to be differentiated, an average drop temperature of 194.2 ± 3.8 K, close to the nitric acid trihydrate (NAT) existence threshold (∼ 195 K at 50 hPa), is found in the region of potential vorticity lower than −10 × 10−5 Km2kg-1s-1 (similar to the 70–90∘ S equivalent latitude region during winter). The spatial distribution and interannual variability of the drop temperature are investigated and discussed. This paper highlights the capability of the IASI sounder to monitor the evolution of polar stratospheric HNO3, a key player in the processes involved in the depletion of stratospheric O3.

Abstract. Near-surface ozone is an harmful air pollutant, which is determined to a considerable extent by weather-controlled processes, and may be significantly impacted by water vapour forming complexes with peroxy radicals. The role of water in the reaction of HO2 radical with nitrogen oxides is known from the literature, and in current models the water complex is considered by assuming a linear dependence on water concentrations. In fact, recent experimental evidence has been published, showing the significant role of water on the kinetics of one of the most important reaction for ozone chemistry, namely NO2 + OH. Here, the available kinetic data for the HOx + NOx reactions have been included in the atmospheric chemistry model ECHAM5/MESSy (EMAC) to test its global significance. Among the modified kinetics, the newly added HNO3 channel from HO2 + NO, dominates, significantly reducing NO2. A major removal process of near-surface ozone is dry deposition accounting for 20 % of the total tropospheric ozone loss mostly occurring over vegetation. However, parameterizations for modelling dry deposition represent a major source of uncertainty for tropospheric ozone simulations. This potentially belongs to the reasons why global models, such as EMAC used here, overestimate ozone with respect to observations. In fact, the employed parameterization is hardly sensitive to local meteorological conditions (e.g., humidity) and lacks non-stomatal deposition. In this study, a dry deposition scheme including these features have been used in EMAC, affecting not only the deposition of ozone but of its precursors, resulting in lower chemical production of ozone. Additionally, we improved the emissions of isoprene and nitrous acid (HONO). Namely, for isoprene emissions we have accounted for the impact of drought stress which confers a higher model sensitivity to meteorology leading to reduced annual emissions down to 32 %. For HONO, we have implemented soil emissions, which depend on soil moisture and thus on precipitation. We estimate for the first time a global source strength of 7 Tg(N) a−1. Furthermore, the usage of a parameterization for the production of lightning NOx that depends on cloud top height contributes to a more realistic representation of NO2 columns over remote oceans with respect to the satellite measurements of the Ozone Monitoring Instrument (OMI). The combination of all the model modifications reduces the simulated global ozone burden by ≈ 20 % to 337 Tg, which is in better agreement with recent estimates. By comparing simulation results with measurements from the Infrared Atmospheric Sounding Interferometer (IASI) and the Tropospheric Ozone Assessment Report (TOAR) databases (of 2009) we demonstrate an overall reduction of the ozone bias by a factor of 2.

Large parts of the troposphere are affected by clouds, whose aqueous-phase chemistry differs significantly from gas-phase chemistry. Box-model studies have demonstrated that clouds influence the tropospheric oxidation capacity. However, most global atmospheric models do not represent this chemistry reasonably well and are largely limited to sulfur oxidation. Therefore, we have developed the Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC), making a detailed in-cloud oxidation model of oxygenated volatile organic compounds (OVOCs) readily available for box as well as for regional and global simulations that are affordable with modern supercomputers. JAMOC includes the phase transfer of species containing up to ten carbon atoms, and the aqueous-phase reactions of a selection of species containing up to four carbon atoms, e.g., ethanol, acetaldehyde, glyoxal. The impact of in-cloud chemistry on tropospheric composition is assessed on a regional and global scale by performing a combination of box-model studies using the Chemistry As A Boxmodel Application (CAABA) and the global atmospheric model ECHAM/MESSy (EMAC). These models are capable to represent the described processes explicitly and integrate the corresponding ODE system with a Rosenbrock solver. Overall, the explicit in-cloud oxidation leads to a reduction of predicted OVOCs levels. By comparing EMAC's prediction of methanol abundance to spaceborne retrievals from the Infrared Atmospheric Sounding Interferometer (IASI), a reduction in EMAC's overestimation is observed in the tropics. Further, the in-cloud OVOC oxidation shifts the hydroperoxyl radicals (HO2) production from the gas- to the aqueous-phase. As a result, the in-cloud destruction (scavenging) of ozone (O3) by the superoxide anion (O2-) is enhanced and accompanied by a reduction in both sources and sinks of tropospheric O3 in the gas phase. By considering only the in-cloud sulfur oxidation by O3, about 13 Tg a-1 of O3 are scavenged, which increases to 336 Tg a-1 when JAMOC is used. With the full oxidation scheme, the highest O3 reduction of 12 % is predicted in the upper troposphere/lower stratosphere (UTLS). Based on the IASI O3 retrievals, it is demonstrated that these changes in the free troposphere significantly reduce the modelled tropospheric O3 columns, which are known to be generally overestimated by global atmospheric models. Finally, the relevance of aqueous-phase oxidation of organics for ozone in hazy polluted regions will be presented.

Because of its important role in the Martian carbon cycle, carbon monoxide (CO) has been the subject of many measurements from ground and from space. Daytime measurements have been mostly exploited to measure the CO abundance because of their good signal-to-noise ratio, but night-time observations have not been documented yet. We demonstrate here the possibility of using PFS (Planetary Fourier Spectrometer) night-time observations to measure the Martian CO abundance. More particularly in this paper, we show that measuring CO during night with PFS can be achieved by averaging a large number of spectra to reach sufficient signal-to-noise. Furthermore, we show that the number of averaged spectra is not the only driving parameter for the detection of CO. High surface temperatures and high thermal contrast (negative in our case) are the two other conditions required for the measurement of the night-time CO abundance. Because of this, the retrievals are especially successful in the Southern Hemisphere during spring and summer when and where these two conditions are met. For night-time spectra with a positive detection, CO vertical profiles are successfully retrieved using the Optimal Estimation method and are characterized in terms of vertical sensitivity. Successful retrievals imply the use of accurate temperature profiles, and in particular an appropriate representation of the thermal inversion in the lower atmosphere. The temperature was obtained by using the relevant information from the CO2 nu(3) band (Bauduin et al., 2020, this issue). A complete error budget of the retrieved CO profiles is also performed and includes different sources of uncertainty. Although the retrieved profiles are not resolved vertically, we show in particular that night-time PFS observations carry information mostly on the CO abundance for the 0-10 km altitude region, and thus provide a stronger constraint on the near-surface CO abundance compared to daytime observations.

In liquid cloud droplets, superoxide anion (O2(aq)-) is known to quickly consume ozone (O3(aq)), which is relatively insoluble. The significance of this reaction as a tropospheric O3 sink is sensitive to the abundance of O2(aq)- and therefore to the production of its main precursor, the hydroperoxyl radical (HO2(aq)). The aqueous-phase oxidation of oxygenated volatile organic compounds (OVOCs) is the major source of HO2(aq) in cloud droplets. Hence, the lack of explicit aqueous-phase chemical kinetics in global atmospheric models leads to a general underestimation of clouds as O3 sinks. In this study, the importance of in-cloud OVOC oxidation for tropospheric composition is assessed by using the Chemistry As A Boxmodel Application (CAABA) and the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model, which are both capable of explicitly representing the relevant chemical transformations. For this analysis, three different in-cloud oxidation mechanisms are employed: (1) one including the basic oxidation of SO2(aq) by O3(aq) and H2O2(aq), which thus represents the capabilities of most global models; (2) the more advanced standard EMAC mechanism, which includes inorganic chemistry and simplified degradation of methane oxidation products; and (3) the detailed in-cloud OVOC oxidation scheme Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC). By using EMAC, the global impact of each mechanism is assessed focusing mainly on tropospheric volatile organic compounds (VOCs), HOx (HOx=OH+HO2), and O3. This is achieved by performing a detailed HOx and O3 budget analysis in the gas and aqueous phase. The resulting changes are evaluated against O3 and methanol (CH3OH) satellite observations from the Infrared Atmospheric Sounding Interferometer (IASI) for 2015. In general, the explicit in-cloud oxidation leads to an overall reduction in predicted OVOC levels and reduces EMAC's overestimation of some OVOCs in the tropics. The in-cloud OVOC oxidation shifts the HO2 production from the gas to the aqueous phase. As a result, the O3 budget is perturbed with scavenging being enhanced and the gas-phase chemical losses being reduced. With the simplified in-cloud chemistry, about 13 Tg yr−1 of O3 is scavenged, which increases to 336 Tg yr−1 when JAMOC is used. The highest O3 reduction of 12 % is predicted in the upper troposphere–lower stratosphere (UTLS). These changes in the free troposphere significantly reduce the modelled tropospheric ozone columns, which are known to be generally overestimated by EMAC and other global atmospheric models.

Near-surface ozone is a harmful air pollutant, which is not only controlled by chemical production and loss processes. The major removal process of near-surface ozone is dry deposition accounting for 20 % of the total tropospheric ozone loss. Due to its significance, parameterizations used in atmospheric chemistry models represent a major source of uncertainty for tropospheric ozone simulations. This uncertainty might be one of the reasons why global models tend to overestimate ozone, when compared to observations. The model used in this study, the global atmospheric model ECHAM5/MESSy (EMAC), is no exception. Like most global models, EMAC employs a “resistances in series” scheme, which is hardly sensitive to local meteorological conditions (e.g. humidity) and lacks non-stomatal deposition. In this study, these missing features have been implemented in EMAC affecting not only the deposition of ozone but also the removal of ozone precursors, resulting in lower chemical production of ozone. Furthermore, near-surface ozone may be significantly impacted by water vapour forming complexes with peroxy radicals. The role of water in the reaction of HO2 radical with itself and nitrogen oxides is known from the literature. However, in current models only the former is considered by assuming a linear dependence on water concentrations. Recent experimental evidence for the significant role of water on the kinetics of one of the most important reaction for ozone chemistry, namely NO2 + OH, has been published. Here, the available kinetic data for the HOx + NOx reactions have been critically re-assessed and included in EMAC to test its global significance. Additionally, we considered the representation of isoprene and nitrous acid (HONO) as important oxidants for lower tropospheric chemistry. Namely, for isoprene emissions we added a drought stress factor which enables a higher sensitivity to meteorology leading to reduced emissions. Also, we firstly implemented soil emissions of HONO which is known as a missing source in models. The implications of these modifications on the global tropospheric composition are analysed, focusing on near-surface ozone and related precursors. The improved representation of ozone in EMAC is demonstrated using measurements from the Infrared Atmospheric Sounding Interferometers (IASI), the Tropospheric Ozone Assessment Report (TOAR) database and from the Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST). The overall changes might help to reduce the uncertainty and overestimation of models predicting near-surface ozone.

Nadir remote sensing of the night side of Mars is challenging, mainly due to the low signal-to-noise ratio of such observations. We show in a companion paper that the abundance of carbon monoxide (CO) during night can be retrieved from the observations of the Planetary Fourier Spectrometer (PFS). This requires, however, an accurate knowledge of the temperature profile, and especially of the night-time thermal inversions, to properly model the atmospheric emission. While the temperature profile is usually retrieved from the nu(2) band of CO2 (centered a 667 cm(-1)), this work shows that, for averaged night-time PFS observations built from a large ensemble of spectra, the temperature profile can be retrieved from the more saturated nu(3) band of CO2 (centered a 2349 cm(-1)). We show especially that, due to IFOV (instantaneous field-of-view) size differences and boresight offset between the longwave and shortwave channels of PFS, the temperature profile retrieved from the nu(3) band is more consistent with the emission observed in the 1-0 band of CO (centered a 2143 cm(-1)), which is used in the second part paper. We provide a complete characterization of the retrieved temperature profiles in terms of error and vertical sensitivity. Using this, we show that using the nu(3) CO2 band allows to properly constrain and characterize the thermal inversions encountered near the surface for most night-time observations. The resulting set of temperature profiles is essential for the retrieval of the night-time CO abundance that is presented in the companion paper. Beyond their usefulness for the night-time CO retrieval, we suggest with a last example that temperature profiles retrieved from the nu(3) band of CO2 could be use more generally to study surface thermal inversions encountered a night.

In this paper, we exploit the first 10-year data-record (2008-2017) of nitric acid (HNO 3) total columns measured by the IASI-A/Metop infrared sounder, characterized by an exceptional daily sampling and a good vertical sensitivity in the mid-stratosphere (around 50 hPa), to monitor the causal relationship between the temperature decrease and the observed HNO 3 loss that occurs each year in the Antarctic stratosphere during the polar night. Since the HNO 3 depletion results from the formation of polar stratospheric clouds (PSCs) which trigger the development of the ozone (O 3) hole, its continuous monitoring is of high 5 importance. We verify here, from the 10-year time evolution of the pair HNO 3-temperature (taken from reanalysis at 50 hPa), the recurrence of specific regimes in the cycle of IASI HNO 3 and identify, for each year, the day and the 50 hPa-temperature ("drop temperature") corresponding to the onset of denitrification in Antarctic winter. Although the measured HNO 3 total column does not allow differentiating the uptake of HNO 3 by different types of PSC particles along the vertical profile, an average drop temperature of ∼191 ± 3 K, consistent with the nitric acid trihydrate (NAT) formation temperature (close to 10 195 K at 50 hPa), is found. The spatial distribution and inter-annual variability of the drop temperature are briefly investigated and discussed in the context of previous PSCs studies. This paper highlights the capability of the IASI sounder to monitor the long-term evolution of the polar stratospheric composition and processes involved in the depletion of stratospheric O 3 .

We analyze the 2019 sudden stratospheric warming event that occurred in the Southern Hemisphere through its impact on the Antarctic ozone. Using temperature, ozone, and nitric acid data from the Infrared Atmospheric Sounding Interferometer (IASI), our results show that the average increase in stratospheric temperature reached a maximum of 34.4° on 20 September in the [60–90]°S latitude range when compared to the past 3 years. Dynamical parameters suggest a locally reversed and weakened zonal winds and a shift in the location of the polar jet vortex. This led to air masses mixing, to a reduced polar stratospheric clouds formation detected at a ground station, and as such to lower ozone and nitric acid depletion. 2019 total ozone columns for the months of September, October, and November were on average higher by 29%, 28%, and 26%, respectively, when compared to the 11‐year average of the same months.

In this paper, we present the global fingerprint of recent changes in middle–upper stratosphere (MUSt; <25 hPa) ozone (O3) in comparison with lower stratosphere (LSt; 150–25 hPa) O3 derived from the first 10 years of the IASI/Metop-A satellite measurements (January 2008–December 2017). The IASI instrument provides vertically resolved O3 profiles with very high spatial and temporal (twice daily) samplings, allowing O3 changes to be monitored in these two regions of the stratosphere. By applying multivariate regression models with adapted geophysical proxies on daily mean O3 time series, we discriminate anthropogenic trends from various modes of natural variability, such as the El Niño–Southern Oscillation (ENSO). The representativeness of the O3 response to its natural drivers is first examined. One important finding relies on a pronounced contrast between a positive LSt O3 response to ENSO in the extratropics and a negative one in the tropics, with a delay of 3 months, which supports a stratospheric pathway for the ENSO influence on lower stratospheric and tropospheric O3. In terms of trends, we find an unequivocal O3 recovery from the available period of measurements in winter–spring at middle to high latitudes for the two stratospheric layers sounded by IASI (>∼35∘ N–S in the MUSt and >∼45∘ S in the LSt) as well as in the total columns at southern latitudes (>∼45∘ S) where the increase reaches its maximum. These results confirm the effectiveness of the Montreal Protocol and its amendments and represent the first detection of a significant recovery of O3 concurrently in the lower, in the middle–upper stratosphere and in the total column from one single satellite dataset. A significant decline in O3 at northern mid-latitudes in the LSt is also detected, especially in winter–spring of the Northern Hemisphere. Given counteracting trends in the LSt and MUSt at these latitudes, the decline is not categorical in total O3. When freezing the regression coefficients determined for each natural driver over the whole IASI period but adjusting a trend, we calculate a significant speeding up in the O3 response to the decline of O3-depleting substances (ODSs) in the total column, in the LSt and, to a lesser extent, in the MUSt, at high southern latitudes over the year. Results also show a small significant acceleration of the O3 decline at northern mid-latitudes in the LSt and in the total column over the last few years. That, specifically, needs urgent investigation to identify its exact origin and apprehend its impact on climate change. Additional years of IASI measurements would, however, be required to confirm the O3 change rates observed in the stratospheric layers over the last few years.