In-service Aircraft For A Global Observing System Research Articles

Variability in the properties of the distribution of the relative humidity with respect to ice: implications for contrail formation

Abstract. Relative humidity with respect to ice (RHi) is a key variable in the formation of cirrus clouds and contrails. We document its probability density function (PDF) using long-term Measurements of Ozone, Water Vapour, Carbon Monoxide and Nitrogen Oxides by In-Service Airbus Aircraft (MOZAIC) and the In-service Aircraft for a Global Observing System (IAGOS) observations over the period 1995–2022 in the upper troposphere (UT) and the lower stratosphere (LS) between 325 and 175 hPa. The characteristics of the RHi PDF differ in the UT and in the LS of the high-latitude regions (HLs) and mid-latitude regions (MLs) of the Northern Hemisphere. In the LS, this PDF decreases exponentially with increasing RHi. In the UT, it first increases exponentially in subsaturated conditions and then decreases exponentially in supersaturated conditions. Because of these different behaviors, the PDF for the combined UT and LS is bimodal. In contrast to the HLs and the MLs, the RHi PDF in the tropical troposphere decreases exponentially with increasing RHi. The different forms of PDF, in the tropics and in the higher-latitude regions, lead to a global PDF of RHi in subsaturated tropospheric conditions that is almost uniform. These findings invite caution when using MOZAIC and IAGOS measurements to calibrate large-scale simulations of RHi. The variability in RHi properties associated with that of temperature also has implications for the formation of contrails. We examined the impact of switching fuel (from kerosene to bioethanol or liquid hydrogen) on the frequency of contrail formation using the Schmidt–Appleman criterion. We show that bioethanol and, to a larger extent, liquid hydrogen would produce more contrails. The impact of a potential change from kerosene to these alternative fuels decreases with decreasing pressure but increases when moving from the higher latitudes of the Northern Hemisphere to the tropics. Finally, we emphasize that investigations of the impact on contrail occurrence frequency as a result of switching from fossil kerosene to more sustainable fuels must be carried out in various meteorological conditions.

Opinion: New directions in atmospheric research offered by research infrastructures combined with open and data-intensive science

Abstract. The acquisition and dissemination of essential information for understanding global biogeochemical interactions between the atmosphere and ecosystems and how climate–ecosystem feedback loops may change atmospheric composition in the future comprise a fundamental prerequisite for societal resilience in the face of climate change. In particular, the detection of trends and seasonality in the abundance of greenhouse gases and short-lived climate-active atmospheric constituents is an important aspect of climate science. Therefore, easy and fast access to reliable, long-term, and high-quality observational environmental data is recognised as fundamental to research and the development of environmental forecasting and assessment services. In our opinion article, we discuss the potential role that environmental research infrastructures in Europe (ENVRI RIs) can play in the context of an integrated global observation system. In particular, we focus on the role of the atmosphere-centred research infrastructures ACTRIS (Aerosol, Clouds and Trace Gases Research Infrastructure), IAGOS (In-service Aircraft for a Global Observing System), and ICOS (Integrated Carbon Observation System), also referred to as ATMO-RIs, with their capabilities for standardised collection and provision of long-term and high-quality observational data, complemented by rich metadata. The ATMO-RIs provide data through open access and offer data interoperability across different research fields including all fields of environmental sciences and beyond. As a result of these capabilities in data collection and provision, we elaborate on the novel research opportunities in atmospheric sciences which arise from the combination of open-access and interoperable observational data, tools, and technologies offered by data-intensive science and the emerging collaboration platform ENVRI-Hub, hosted by the European Open Science Cloud (EOSC).

Distribution and morphology of non-persistent contrail and persistent contrail formation areas in ERA5

Abstract. The contrail formation potential as well as its temporal and spatial distribution is estimated using meteorological conditions of temperature and relative humidity from the ERA5 re-analysis provided by the European Centre for Medium-Range Weather Forecasts. Contrail formation is estimated with the Schmidt–Appleman criterion (SAc), solely considering thermodynamic effects. The focus is on a region ranging from the Eastern United States (110–65° W) to central Europe (5° W–30° E). Around 18 000 flight trajectories from the In-service Aircraft for a Global Observing System (IAGOS) are used as a representative subset of transatlantic, commercial flights. The typical crossing distance through a contrail-prone area is determined based on IAGOS measurements of temperature T and relative humidity r and then based on co-located ERA5 simulations of the same quantities. Differences in spatial resolution between IAGOS and ERA5 are addressed from an aircraft-centered perspective, using 1 km segments, and a model-centered perspective, using 19 km flight sections. Using the aircraft-centered approach, 50 % of the crossings of persistent contrail (PC) regions based on IAGOS are shorter than 9 km, while in ERA5 the median is 155 km. Time-averaged IAGOS data lead to a median crossing length of 66 km. The difference between the two data sets is attributed to the higher variability of r in IAGOS compared to ERA5. The model-centered approach yields similar results, but typical crossing lengths are larger by only up to 10 %. Binary masks of PC formation are created by applying the SAc on the two-dimensional fields of T and r from ERA5. In a second step the morphology of PC regions is also assessed. Half of the PC regions in ERA5 are found to be smaller than ≈ 35 000 km2 (at 200 hPa), and the median of the maximum dimension is shorter than 760 km (at 200 hPa). Furthermore, PC regions tend to be of near-circular shape with a tendency to a slight oval shape and a preferred alignment along the dominant westerly flow. Seasonal, vertical distributions of PC formation potential 𝒫 are characterized by a maximum between 250 and 200 hPa. 𝒫 is subject to seasonal variations with a maximum in magnitude and extension during the winter months and a minimum during summer. The horizontal distribution of PC regions suggests that PC regions are likely to appear in the same location on adjacent pressure levels. Climatologies of T, r, wind speed U, and resulting PC formation potential are calculated to identify the constraining effects of T and r on 𝒫. PC formation is primarily limited by conditions that are too warm below and conditions that are too dry above the formation region. The distribution of PCs is slanted towards lower altitudes from 30 to 70° N, following lines of constant T and r. For an observed co-location of high U and 𝒫, it remains unclear whether PC formation and the jet stream are favored by the same meteorological conditions or if the jet stream itself favors PC occurrence. This analysis suggests that some PC regions will be difficult to avoid by rerouting aircraft because of their large vertical and horizontal extents.

Advantages of assimilating multispectral satellite retrievals of atmospheric composition: a demonstration using MOPITT carbon monoxide products

Abstract. The Measurements Of Pollution In The Troposphere (MOPITT) is an ideal instrument to understand the impact of (1) assimilating multispectral and joint retrievals versus single spectral products, (2) assimilating satellite profile products versus column products, and (3) assimilating multispectral and joint retrievals versus assimilating individual products separately. We use the Community Atmosphere Model with chemistry with the Data Assimilation Research Testbed (CAM-chem+DART) to assimilate different MOPITT carbon monoxide (CO) products to address these three questions. Both anthropogenic and fire CO emissions are optimized in the data assimilation experiments. The results are compared with independent CO observations from TROPOspheric Monitoring Instrument (TROPOMI), the Total Carbon Column Observing Network (TCCON), NOAA Carbon Cycle Greenhouse Gases (CCGG) sites, In-service Aircraft for a Global Observing System (IAGOS), and Western wildfire Experiment for Cloud chemistry, Aerosol absorption and Nitrogen (WE-CAN). We find that (1) assimilating the MOPITT joint (multispectral; near-IR and thermal IR) column product leads to better model–observation agreement at and near the surface than assimilating the MOPITT thermal-IR-only column retrieval. (2) Assimilating column products has a larger impact and improvement for background and large-scale CO compared to assimilating profile products due to vertical localization in profile assimilation. However, profile assimilation can outperform column assimilations in fire-impacted regions and near the surface. (3) Assimilating multispectral and joint products results in similar or slightly better agreement with observations compared to assimilating the single spectral products separately.

Evaluation of modelled climatologies of O3, CO, water vapour and NOy in the upper troposphere–lower stratosphere using regular in situ observations by passenger aircraft

Abstract. Evaluating global chemistry models in the upper troposphere–lower stratosphere (UTLS) is an important step toward an improved understanding of the chemical composition in this region. This composition is regularly sampled through in situ measurements based on passenger aircraft, in the framework of the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. This study focuses on the comparison of the IAGOS measurements in ozone, carbon monoxide (CO), nitrogen reactive species (NOy) and water vapour, with a 25-year simulation output from the LMDZ-OR-INCA chemistry–climate model. For this purpose, we present and apply an extension of the Interpol-IAGOS software that projects the IAGOS data onto any model grid, in order to derive a gridded IAGOS product and a masked (sub-sampled) model product that are directly comparable to one another. Climatologies are calculated in the upper troposphere (UT) and in the lower stratosphere (LS) separately but also in the UTLS as a whole, as a demonstration for the models that do not sort out the physical variables necessary to distinguish between the UT and the LS. In the northern extratropics, the comparison in the UTLS layer suggests that the geographical distribution in the tropopause height is well reproduced by the model. In the separated layers, the model simulates well the water vapour climatologies in the UT and the ozone climatologies in the LS. There are opposite biases in CO in both UT and LS, which suggests that the cross-tropopause transport is overestimated. The NOy observations highlight the difficulty of the model in parameterizing the lightning emissions. In the tropics, the upper-tropospheric climatologies are remarkably well simulated for water vapour. They also show realistic CO peaks due to biomass burning in the most convective systems, and the ozone latitudinal variations are well correlated between the observations and the model. Ozone is more sensitive to lightning emissions than to biomass burning emissions, whereas the CO sensitivity to biomass burning emissions strongly depends on location and season. The present study demonstrates that the Interpol-IAGOS software is a tool facilitating the assessment of global model simulations in the UTLS, which is potentially useful for any modelling experiment involving chemistry climate or chemistry transport models.

Tropical tropospheric ozone and carbon monoxide distributions: characteristics, origins, and control factors, as seen by IAGOS and IASI

Abstract. The characteristics and seasonal variability in the tropical tropospheric distributions of ozone (O3) and carbon monoxide (CO) were analysed based on in situ measurements provided by the In-service Aircraft for a Global Observing System (IAGOS) programme since 1994 and 2002, respectively, combined with observations from the Infrared Atmospheric Sounding (IASI) instrument on board the MetOp-A satellite since 2008. The SOFT-IO (SOft attribution using FlexparT and carbon monoxide emission inventories for In-situ Observation database) model, which couples back trajectories with CO emission inventories, was used to explore the origins and sources of the tropical CO observed by IAGOS. The highest O3 and CO mixing ratios occur over western Africa in the lower troposphere (LT: surface to 750 hPa) during the fire season (75 ppb of O3 at 2.5 km and 850 ppb of CO at 0.3 km over Lagos in January), mainly due to anthropogenic (AN) emissions and a major contribution from fires. The secondary maxima are observed in Asia in the mid-troposphere (MT: 750–300 hPa) and upper troposphere (UT: 300–200 hPa) in April for O3 and in the LT in January for CO, with larger contributions from AN emissions. The lowest O3 and CO mixing ratios occur over Caracas. In the tropical LT, the majority of the location clusters are affected by local and regional AN emissions. The highest AN impact is found over Asia, Arabia and eastern Africa, and South America (>75 % of CO). Biomass burning (BB) emissions also originate from local or regional sources but with stronger seasonal dependence. The highest BB impact is found over southern tropical Africa (57 %–90 %), except in April, mostly due to local fires, but also from Northern Hemisphere Africa in January (45 %–73 %) and Southern Hemisphere South America in October (29 % over Windhoek). In the MT and UT, AN emissions are more important and dominate in the eastern part of the tropics (from the Middle East to Asia). BB contributions are more important than in the LT, especially from the African fires in January and July and from South East and equatorial Asia in April and October. The overall highest amount of CO is exported from Africa, with the main transport pathway from the dry-season African regions towards the wet-season ones. In contrast, the impact of the Asian emissions in the LT and MT is limited on a local or regional scale. The transport of polluted Asian air masses is important in the UT during the Asian summer monsoon and post-monsoon seasons, when convection is active.

Comparison of Actual and Time-Optimized Flight Trajectories in the Context of the In-Service Aircraft for a Global Observing System (IAGOS) Programme

Airlines optimize flight trajectories in order to minimize their operational costs, of which fuel consumption is a large contributor. It is known that flight trajectories are not fuel-optimal because of airspace congestion and restrictions, safety regulations, bad weather and other operational constraints. However, the extent to which trajectories are not fuel-optimal (and therefore CO2-optimal) is not well known. In this study, we present two methods for optimizing the flight cruising time by taking best advantage of the wind pattern at a given flight level and for constant airspeed. We test these methods against actual flight trajectories recorded under the In-service Aircraft for a Global Observing System (IAGOS) programme. One method is more robust than the other (computationally faster) method, but when successful, the two methods agree very well with each other, with optima generally within the order of 0.1%. The IAGOS actual cruising trajectories are on average 1% longer than the computed optimal for the transatlantic route, which leaves little room for improvement given that by construction the actual trajectory cannot be better than our optimum. The average degree of non-optimality is larger for some other routes and can be up to 10%. On some routes, there are also outlier flights that are not well optimized; however, the reason for this is not known.

Characterisation of a self-sustained, water-based condensation particle counter for aircraft cruising pressure level operation

Abstract. Aerosol particle number concentration measurements are a crucial part of aerosol research. Vertical profile measurements and high-altitude/low-pressure performance of the respective instruments become more important for remote sensing validation and a vital tool for the observation of climate variables. This study tests the new, commercially available water condensation particle counter (MAGIC 210-LP) for the deployment at aircraft cruising pressure levels that the European research infrastructure IAGOS (In-service Aircraft for a Global Observing System; http://www.iagos.org, last access: 2 May 2023) is aiming for by operating measurement instrumentation onboard passenger aircraft. We conducted laboratory experiments for conditions to simulate passenger aircraft flight altitude at operation pressure. We demonstrate that this type of water condensation particle counter shows excellent agreement with a butanol-based instrument used in parallel. A Faraday cup aerosol electrometer serves as the reference instrument. Experiments are performed with test aerosol ammonium sulfate and fresh combustion soot at pressure levels ranging from 700 to 200 hPa. For soluble particles like ammonium sulfate, the 50 % detection efficiency cut-off diameter (D50) is around 5 nm and does not differ significantly for all performed experiments. For non-soluble fresh soot particles, the D50 cut-off diameter of approximately 10 nm does not vary substantially as a function of pressure, whereas the 90 % detection efficiency cut-off diameter D90 increases from 19 nm at 700 hPa to 37 nm at 200 hPa. The overall counting efficiency for particles larger than 40 nm reaches 100 % for working pressures of 200 hPa and higher.

The Long-Term Trends and Interannual Variability in Surface Ozone Levels in Beijing from 1995 to 2020

Tropospheric ozone is an important atmospheric pollutant as well as an efficient greenhouse gas. Beijing is one of the cities with the most serious ozone pollution. However, long-term date of observed ozone in Beijing are limited. In this paper, we combine the measurements of the In-service Aircraft for a Global Observing System (IAGOS), ozonesonde observations as well as the recently available ozone monitoring network observations to produce a unique data record of surface ozone (at 14:00 Beijing time) in Beijing from 1995 to 2020. Using this merged dataset, we investigate the variability in surface ozone in Beijing on multiple timescales. The long-term change is primarily characterized by a sudden drop in 2011–2012 with an insignificant linear trend during the full period. Based on CAM-chem model simulations, meteorological factors played important roles in the 2011–2012 ozone drop. Before and after this sudden drop, ozone levels in Beijing increased significantly by 0.42 ± 0.27 ppbv year−1 before 2011 and 0.43 ± 0.41 ppbv year−1 after 2013. We also found a substantial increase in the amplitude of the ozone annual cycle in Beijing, which has not been documented in previous studies. This is consistent with ozone increases in summer and ozone decreases in winter. In addition, the results by the Ensemble Empirical Mode Decomposition (EEMD) analysis indicate significant interannual variations in ozone levels in Beijing with different time oscillation periods, which may be associated with natural variabilities and subsequent changes in meteorological conditions.

A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018

Abstract. Tropopause folds are the key process underlying stratosphere-to-troposphere transport (STT) of ozone, and thus they affect tropospheric ozone levels and variability. In the present study we perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 during folding events over Europe and for the time period from 2003 to 2018. A 3-D labeling algorithm is applied to detect tropopause folds in CAMSRA, while ozonesonde data from WOUDC (World Ozone and Ultraviolet Radiation Data Centre) and aircraft measurements from IAGOS (In-service Aircraft for a Global Observing System) are used for CAMSRA O3 evaluation. The profiles of observed and CAMSRA O3 concentrations indicate that CAMSRA reproduces the observed O3 increases in the troposphere during the examined folding events. Nevertheless, at most of the examined sites, CAMSRA overestimates the observed O3 concentrations, mostly at the upper portion of the observed increases, with a median fractional gross error (FGE) among the examined sites >0.2 above 400 hPa. The use of a control run without data assimilation reveals that the aforementioned overestimation of CAMSRA O3 arises from the data assimilation implementation. Overall, although data assimilation assists CAMSRA O3 to follow the observed O3 enhancements in the troposphere during the STT events, it introduces biases in the upper troposphere resulting in no clear quantitative improvement compared to the control run without data assimilation. Less biased assimilated O3 products, with finer vertical resolution in the troposphere, in addition to higher IFS (Integrated Forecasting System) vertical resolution, are expected to provide a better representation of O3 variability during tropopause folds.

High concentrations of ice crystals in upper-tropospheric tropical clouds: is there a link to biomass and fossil fuel combustion?

Abstract. Eight years of upper-tropospheric (UT) ice crystal measurements with the backscatter cloud probe (BCP), installed on commercial aircraft operated as part of the In-Service Aircraft for a Global Observing System (IAGOS), have been analyzed to assess the frequency and characteristics of extreme ice crystal events (EIEs), defined in this study as encounters with clouds that have number concentrations exceeding 5000 L−1. A total of 3196 events, in clouds of horizontal extent ≥ 2.5 km, were identified during the period from December 2011 to March 2020 in the latitude band between 30∘ S and 30∘ N. Regions of anthropogenic sources of carbon monoxide, with particles that can alter cloud microphysics, were attributed to these EIEs in UT clouds using the SOFT-IO model. The evaluation of low- and upper-level kinematic variables from the European Centre for Medium-Range Weather Forecasts (ERA5) reanalysis, combined with spatial distributions of aerosol optical depth and regions of biomass burning, highlights the physical mechanisms by which the particles are lofted to flight levels in regions of deep convection. The maps of lightning frequency, derived from the World Wide Lightning Location Network (WWLLN), provide additional evidence of the role of deep convection in transporting aerosol particles, cloud hydrometeors and carbon monoxide to aircraft cruising altitudes. The evaluation of aerosol particle mass concentrations and composition from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) contributes additional evidence for a link between regions of EIEs and surface emissions of dust, black carbon (BC), organic carbon (OC) and sulfate particles. Given the composition of the source aerosols and the role of deep convection in their transport to the UT, the sampled ice clouds likely originate from the homogeneous or heterogeneous freezing of droplets formed on these particles, as has been reported in previous studies. The results from this study, which have been obtained from a large sample of measurements, have ramifications related to satellite measurement validation, weather forecasting and climate change. In addition, over 2000 of the randomly sampled clouds had derived ice water contents larger than 1 g m−3, a concentration that is considered potentially hazardous to commercial aircraft operations.

The effects of the COVID-19 lockdowns on the composition of the troposphere as seen by In-service Aircraft for a Global Observing System (IAGOS) at Frankfurt

Abstract. The European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) equips commercial aircraft with a system for measuring atmospheric composition. A range of essential climate variables and air quality parameters are measured throughout the flight, from take-off to landing, giving high-resolution information in the vertical in the vicinity of international airports and in the upper troposphere–lower stratosphere during the cruise phase of the flight. Six airlines are currently involved in the programme, achieving a quasi-global coverage under normal circumstances. During the COVID-19 crisis, many airlines were forced to ground their fleets due to a fall in passenger numbers and imposed travel restrictions. Deutsche Lufthansa, a partner in IAGOS since 1994 was able to operate an IAGOS-equipped aircraft during the COVID-19 lockdown, providing regular measurements of ozone and carbon monoxide at Frankfurt Airport. The data form a snapshot of an unprecedented time in the 27-year time series. In May 2020, we see a 32 % increase in ozone near the surface with respect to a recent reference period, a magnitude similar to that of the 2003 heatwave. The anomaly in May is driven by an increase in ozone at nighttime which might be linked to the reduction in NO during the COVID-19 lockdowns. The anomaly diminishes with altitude becoming a slightly negative anomaly in the free troposphere. The ozone precursor carbon monoxide shows an 11 % reduction in MAM (March–April–May) near the surface. There is only a small reduction in CO in the free troposphere due to the impact of long-range transport on the CO from emissions in regions outside Europe. This is confirmed by data from the Infrared Atmospheric Sounding Interferometer (IASI) using retrievals performed by SOftware for a Fast Retrieval of IASI Data (SOFRID), which display a clear drop of CO at 800 hPa over Europe in March but otherwise show little change to the abundance of CO in the free troposphere.

Recent ozone trends in the Chinese free troposphere: role of the local emission reductions and meteorology

Abstract. Free tropospheric ozone (O3) trends in the Central East China (CEC) and export regions are investigated for 2008–2017 using the IASI (Infrared Atmospheric Sounding Interferometer) O3 observations and the LMDZ-OR-INCA model simulations, including the most recent Chinese emission inventory. The observed and modelled trends in the CEC region are −0.07 ± 0.02 and −0.08 ± 0.02 DU yr−1, respectively, for the lower free troposphere (3–6 km column) and −0.05 ± 0.02 and −0.06 ± 0.02 DU yr−1, respectively, for the upper free troposphere (6–9 km column). The statistical p value is smaller to 0.01 for all the derived trends. A good agreement between the observations and the model is also observed in the region, including the Korean Peninsula and Japan and corresponding to the region of pollution export from China. Based on sensitivity studies conducted with the model, we evaluate, at 60 % and 52 %, the contribution of the Chinese anthropogenic emissions to the trend in the lower and upper free troposphere, respectively. The second main contribution to the trend is the meteorological variability (34 % and 50 %, respectively). These results suggest that the reduction in NOx anthropogenic emissions that has occurred since 2013 in China led to a decrease in ozone in the Chinese free troposphere, contrary to the increase in ozone at the surface. We designed some tests to compare the trends derived by the IASI observations and the model to independent measurements, such as the In-service Aircraft for a Global Observing System (IAGOS) or other satellite measurements (Ozone Monitoring Instrument (OMI)/Microwave Limb Sounder (MLS)). These comparisons do not confirm the O3 decrease and stress the difficulty in analysing short-term trends using multiple data sets with various sampling and the risk of overinterpreting the results.

Origins and characterization of CO and O<sub>3</sub> in the African upper troposphere

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the Infrared Atmospheric Sounding Interferometer (IASI) instrument aboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10∘ from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5∘ N in DJFM and 128 to 149 ppb at 3–7∘ S in JJASO) and decreasing values southward and northward. The O3 meridional transects are characterized by mixing ratio minima of ∼42–54 ppb at the ITCZ (10–16∘ S in DJFM and 5–8∘ N in JJASO) framed by local maxima (∼53–71 ppb) coincident with the wind shear zones north and south of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO-enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution and drive the location of the observed UT CO maxima. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high-altitude air masses uplifted from either local or long-distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO) and must be created during transport by photochemistry.

Fifty years of balloon-borne ozone profile measurements at Uccle, Belgium: a short history, the scientific relevance, and the achievements in understanding the vertical ozone distribution

Abstract. Starting in 1969 and comprising three launches a week, the Uccle (Brussels, Belgium) ozonesonde dataset is one of longest and densest in the world. Moreover, as the only major change was the switch from Brewer-Mast (BM) to electrochemical concentration cell (ECC) ozonesonde types in 1997 (when the emissions of ozone-depleting substances peaked), the Uccle time series is very homogenous. In this paper, we briefly describe the efforts that were undertaken during the first 3 decades of the 50 years of ozonesonde observations to guarantee the homogeneity between ascent and descent profiles, under changing environmental conditions (e.g. SO2), and between the different ozonesonde types. This paper focuses on the 50-year-long Uccle ozonesonde dataset and aims to demonstrate its past, present, and future relevance to ozone research in two application areas: (i) the assessment of the temporal evolution of ozone from the surface to the (middle) stratosphere, and (ii) as the backbone for validation and stability analysis of both stratospheric and tropospheric satellite ozone retrievals. Using the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) multiple linear regression model (SPARC/IO3C/GAW, 2019), we found that the stratospheric ozone concentrations at Uccle have declined at a significant rate of around 2 % per decade since 1969, which is also rather consistent over the different stratospheric levels. This overall decrease can mainly be assigned to the 1969–1996 period with a rather consistent rate of decrease of around −4 % per decade. Since 2000, a recovery of between +1 % per decade and +3 % per decade of the stratospheric ozone levels above Uccle has been observed, although it is not significant and is not seen for the upper stratospheric levels measured by ozonesondes. Throughout the entire free troposphere, a very consistent increase in the ozone concentrations of 2 % per decade to 3 % per decade has been measured since both 1969 and 1995, with the trend since 1995 being in almost perfect agreement with the trends derived from the In-service Aircraft for a Global Observing System (IAGOS) ascent/descent profiles at Frankfurt. As the number of tropopause folding events in the Uccle time series has increased significantly over time, increased stratosphere-to-troposphere transport of recovering stratospheric ozone might partly explain these increasing tropospheric ozone concentrations, despite the levelling-off of (tropospheric) ozone precursor emissions and notwithstanding the continued increase in mean surface ozone concentrations. Furthermore, we illustrate the crucial role of ozonesonde measurements for the validation of satellite ozone profile retrievals. With the operational validation of the Global Ozone Monitoring Experiment-2 (GOME-2), we show how the Uccle dataset can be used to evaluate the performance of a degradation correction for the MetOp-A/GOME-2 UV (ultraviolet) sensors. In another example, we illustrate that the Microwave Limb Sounder (MLS) overpass ozone profiles in the stratosphere agree within ±5 % with the Uccle ozone profiles between 10 and 70 hPa. Another instrument on the same Aura satellite platform, the Tropospheric Emission Spectrometer (TES), is generally positively biased with respect to the Uccle ozonesondes in the troposphere by up to ∼ 10 ppbv, corresponding to relative differences of up to ∼ 15 %. Using the Uccle ozonesonde time series as a reference, we also demonstrate that the temporal stability of those last two satellite retrievals is excellent.

Internal consistency of the IAGOS ozone and carbon monoxide measurements for the last 25 years

Abstract. The In-service Aircraft for a Global Observing System (IAGOS) is a European research infrastructure that equips the Airbus A340/330 with a system for monitoring atmospheric composition. The IAGOS instruments have three different configurations: IAGOS-Core, IAGOS – Measurement of Ozone and Water Vapor by Airbus In Service Aircraft (IAGOS-MOZAIC) and IAGOS – Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (IAGOS-CARIBIC). Since 1994, there have been a total of 17 aircraft equipped. In this study, we perform an intercomparison of about 8000 landing and takeoff profiles to compare the O3 and CO measurements performed from these different configurations. The collocated profiles used in the study met various selection criteria. The first was a maximal 1 h time difference between an ascent or descent by two different aircraft at the same airport and the second was a selection based on the similarity of air masses based on the meteorological data acquired by the aircraft. We provide here an evaluation of the internal consistency of the O3 and CO measurements since 1994. For both O3 and CO, we find no drift in the bias amongst the different instrument units (six O3 and six CO IAGOS-MOZAIC instruments, nine IAGOS-Core Package1 and the two instruments used in the IAGOS-CARIBIC aircraft). This result gives us confidence that the entire IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.

Interpol-IAGOS: a new method for assessing long-term chemistry–climate simulations in the UTLS based on IAGOS data, and its application to the MOCAGE CCMI REF-C1SD simulation

Abstract. A wide variety of observation data sets are used to assess long-term simulations provided by chemistry–climate models (CCMs) and chemistry-transport models (CTMs). However, the upper troposphere–lower stratosphere (UTLS) has hardly been assessed in these modelling exercises yet. Observations performed in the framework of IAGOS (In-service Aircraft for a Global Observing System) combine the advantages of in situ airborne measurements in the UTLS with an almost-global-scale sampling, a ∼20-year monitoring period and a high frequency. Even though a few model assessments have been made using the IAGOS database, none of them took advantage of the dense and high-resolution cruise data in their whole ensemble yet. The present study proposes a method to compare this large IAGOS data set to long-term simulations used for chemistry–climate studies. As a first application, the REF-C1SD reference simulation generated by the MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) CTM in the framework of Chemistry-Climate Model Initiative (CCMI) phase I has been evaluated during the 1994–2013 period for ozone (O3) and the 2002–2013 period for carbon monoxide (CO). The concept of the new comparison software proposed here (so-called Interpol-IAGOS) is to project all IAGOS data onto the 3-D grid of the model with a monthly resolution, since generally the 3-D outputs provided by chemistry–climate models for multi-model comparisons on multi-decadal timescales are archived as monthly means. This provides a new IAGOS data set (IAGOS-DM) mapped onto the model's grid and time resolution. To get a model data set consistent with IAGOS-DM for the comparison, a subset of the model's outputs is created (MOCAGE-M) by applying a mask that retains only the model data at the available IAGOS-DM grid points. Climatologies are derived from the IAGOS-DM product, and good correlations are reported between with the MOCAGE-M spatial distributions. As an attempt to analyse MOCAGE-M behaviour in the upper troposphere (UT) and the lower stratosphere (LS) separately, UT and LS data in IAGOS-DM were sorted according to potential vorticity. From this, we derived O3 and CO seasonal cycles in eight regions well sampled by IAGOS flights in the northern midlatitudes. They are remarkably well reproduced by the model for lower-stratospheric O3 and also good for upper-tropospheric CO. Along this model evaluation, we also assess the differences caused by the use of a weighting function in the method when projecting the IAGOS data onto the model grid compared to the scores derived in a simplified way. We conclude that the data projection onto the model's grid allows us to filter out biases arising from either spatial or temporal resolution, and the use of a weighting function yields different results, here by enhancing the assessment scores. Beyond the MOCAGE REF-C1SD evaluation presented in this paper, the method could be used by CCMI models for individual assessments in the UTLS and for model intercomparisons with respect to the IAGOS data set.

Insight into ozone profile climatology over northeast China from aircraft measurement and numerical simulation

Tropospheric ozone is a major pollutant that can harm human health, animals and plants. With a rapid development in Northeast China, ozone pollution has become an increasingly serious environmental challenge. To study the ozone distribution and the potential sources of ozone precursors in Northeast China, we analyzed vertical ozone profiles from the In-service Aircraft for a Global Observing System (IAGOS) in 2012–2014 and provided the climatological vertical structure of tropospheric ozone over Shenyang. The tropospheric ozone generally presents high in hot months, mainly due to the combined effects of the strong solar radiation and high volatile organic compounds emission in summer. While in cold months, the ozone is low because of weak solar radiation and high nitrogen oxides emission. Besides, a low-ozone center exists within lower troposphere in August, which is mainly caused by the East Asian summer monsoon prevailing in summer. To analyze the sources of ozone, typical ozone pollution episodes were studied and the results revealed the different pathways for the enhancement of ozone pollution in Shenyang: regional transport of anthropogenic emissions from North China Plain (NCP), long-range transport from Siberian biomass burning and local photochemical production. Modeling results show that the largest contribution to the surface ozone in Northeast China is local anthropogenic emissions (exceed 90%); the regional transport of NCP anthropogenic emissions contribute more to the pollutants around 2 km, and account for more than 50% pollutants during highly ozone polluted days; through long-range transport, Siberian biomass burning in the spring also have a nonnegligible effect on the near-ground ozone in Northeast China. Overall, this study provides tropospheric ozone climatology and its source attribution in Northeast China, and highlight the great importance of regional transport of anthropogenic and biomass burning emissions in ozone pollution.

Convective uplift of pollution from the Sichuan Basin into the Asian monsoon anticyclone during the StratoClim aircraft campaign

Abstract. The StratoClim airborne campaign took place in Nepal from 27 July to 10 August 2017 to document the physical and chemical properties of the South Asian upper troposphere–lower stratosphere (UTLS) during the Asian summer monsoon (ASM). In the present paper, simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of Asian monsoon anticyclone (AMA) and on the formation of the Asian tropopause aerosol layer (ATAL) during the StratoClim campaign. StratoClim took place during a break phase of the monsoon with intense convective activity over South China and Sichuan. Comparisons between brightness temperatures (BTs) at 10.8 µm observed by satellite sensors and simulated by Meso-NH highlight the ability of the model to correctly reproduce the life cycle of deep convective clouds. A comparison between CO and O3 concentrations from Meso-NH and airborne observations (StratoClim and IAGOS (In-service Aircraft for a Global Observing System)) demonstrates that the model captures most of the observed variabilities. Nevertheless, for both gases, the model tends to overestimate the concentrations and misses some thin CO plumes related to local convective events probably because the resolution is too coarse, but the convective uplift of pollution is very well captured by the model. We have therefore focused on the impact of Sichuan convection on the AMA composition. A dedicated sensitivity simulation showed that the 7 August convective event brought large amounts of CO deep into the AMA and even across the 380 K isentropic level located at 17.8 km. This Sichuan contribution enhanced the CO concentration by ∼15 % to reach more than 180 ppbv over a large area around 15 km height. It is noteworthy that Meso-NH captures the impact of the diluted Sichuan plume on the CO concentration during a StratoClim flight south of Kathmandu, highlighting its ability to reproduce the transport pathway of Sichuan pollution. According to the model, primary organic aerosol and black carbon particles originating from Sichuan are transported following the same pathway as CO. The large particles are heavily scavenged within the precipitating part of the convective clouds but remain the most important contributor to the particle mass in the AMA. Over the whole AMA region, the 7 August convective event resulted in a 0.5 % increase in CO concentration over the 10–20 km range that lasted about 2 d. The impact of pollution uplift from three regions (India, China, and Sichuan) averaged over the first 10 d of August has also been evaluated with sensitivity simulations. Even during this monsoon break phase, the results confirm the predominant role of India relative to China with respective contributions of 11 % and 7 % to CO concentration in the 10–15 km layer. Moreover, during this period a large part (35 %) of the Chinese contribution comes from the Sichuan Basin alone.

Multidecadal Measurements of UTLS Gravity Waves Derived From Commercial Flight Data

AbstractGravity waves (GWs) are key drivers of atmospheric dynamics, with major impacts on climate and weather processes. However, they are challenging to measure in observational data, and as a result no large‐area multidecadal GW time series yet exist. This has prevented us from quantifying the interactions between GWs and long–timescale climate processes. Here, we exploit temperatures measured by commercial aircraft since 1994 as part of the In‐Service Aircraft for a Global Observing System (IAGOS) atmospheric chemistry research program to produce a novel 26‐year time series of upper troposphere/lower stratosphere (UTLS) GW measurements across most of the Northern Hemisphere. We analyze 90,342 flight hours (76.2 million flight kilometers) of data, typically at a temporal resolution of seconds and with high temperature precision. We show that GW activity in the Northern Hemisphere UTLS is consistently strongest north of and above the upper tropospheric jet. We also show that GW sources not typically observed in stratospheric data but assumed in model schemes, such as the Rocky Mountains, are visible at these altitudes, suggesting that wave momentum from these sources is deposited specifically between ∼200 and 50 hPa. Our data show no significant impact of the Quasi‐Biennial Oscillation, the Northern Annular Mode, or climate change. However, we do see strong evidence of links with the El Niño–Southern Oscillation, which modulates the measured GW signal by ∼25%, and weak evidence of links with the 11‐year solar cycle. These results have important implications for atmospheric process modeling and for understanding large‐scale climate teleconnections.