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We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m−2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.

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.

We analysed ozone and carbon monoxide profiles measured by commercial aircrafts from the MOZAIC/IAGOS fleet, during ascending and descending flights over Caracas, in Venezuela, from August 1994 to December 2009, over Rio de Janeiro, from 1994 to 2004 and from July 2012 to June 2013, and over São Paulo, in Brazil, from August 1994 to 2005. For ozone, results showed a clean atmosphere over Caracas presenting the highest seasonal mean in March, April and May. Backward trajectory analyses with FLEXPART, of case studies for which the measured concentrations were high, showed that contributions from local, Central and North America, the Caribbean and Africa either from anthropogenic emissions, biomass burning or lightning were possible. Satellite products as fire counts from MODIS, lightning flash rates from LIS, and CO and O 3 from Infrared Atmospheric Sounding Interferometer and wind maps at different levels helped corroborate previous findings. Sensitivity studies performed with the chemical transport model GEOS-Chem captured the effect of anthropogenic emissions but underestimated the influence of biomass burning, which could be due to an underestimation of GFEDv2 emission inventory. The model detected the contribution of lightning from Africa in JJA and SON and from South America in DJF, possibly from the northeast of Brazil. Over São Paulo and Rio de Janeiro, GEOS-Chem captured the seasonal variability of lightning produced in South America and attributed this source as the most important in this region, except in JJA, when anthropogenic emissions were addressed as the more impacting source of ozone precursors. However, comparison with the measurements indicated that the model overestimated ozone formation, which could be due to the convective parameterisation or the stratospheric influence. The highest ozone concentration was observed during September to November, but the model attributed only a small influence of biomass burning from South America, with no contribution of long-range transport from Africa.

This paper reports atmospheric profiles of N2O retrieved from Metop/IASI with the Software for the Retrieval of IASI Data (SOFRID) for the 2008–2018 period and their validation with FTIR data from 12 stations of the Network for the Detection of Atmospheric Composition Changes (NDACC). SOFRID retrievals performed in the 2160–2218 cm−1 spectral window provide 3 independent pieces of information about the vertical profile of N2O. The FTIR versus SOFRID comparisons display a better agreement in the mid-troposphere (MT, 700–350 hPa) than in the lower (LT, Surface–700 hPa) and upper (UT, 350–110 hPa) troposphere with correlation coefficients (R) in the 0.49–0.83 range and comparable variabilities (3–5 ppbv). The agreement for oceanic and coastal stations (R > 0.77) is better than for continental ones (R < 0.72). The SOFRID MT N2O mixing ratios are significantly biased high (up to 16.8 ppbv) relative to FTIR at continental stations while the biases remain below 4.2 ppbv and mostly unsignificant when oceanic data are considered. The average MT decadal trends derived from SOFRID at the 8 NDACC stations with continuous observations during the 2008–2018 period (1.05 ± 0.1 ppbv·yr−1) is in good agreement with the corresponding FTIR trends (1.08 ± 0.1 ppbv·yr−1) and the NOAA-ESRL trends from surface in-situ measurements (0.95 ± 0.02 ppbv·yr−1). In the Northern Hemisphere where they are clearly detected, the N2O MT seasonal variations from SOFRID and FTIR are phased (summer minima) and have similar amplitudes. SOFRID also detects the UT summer maxima indicating independent MT and UT information. The global MT N2O oceanic distributions from SOFRID display low geographical variability and are mainly characterized by enhanced tropical mixing ratios relative to mid and high latitudes.

We have used ozone data from the Infrared Atmospheric Sounding Interferometer to follow an event of ozone-enriched air-masses in the upper troposphere from eastern Africa to northern India. The ozone transport (hereafter called 'ozone river' or O3R) occurred during the Asian post-monsoon season in 2008 and was associated with Rossby wave propagation. The persistence of the O3R in a narrow channel was confirmed by MOZAIC airborne data over the northwestern Indian coast. The regions of origin of the O3R were identified by a transport analysis based on the Lagrangian model FLEXPART. The Lagrangian simulations combined with potential vorticity fields indicate that stratospheric intrusions are not likely to be the most important contributor to the observed O 3 enhancements. A high-resolution Eulerian model, Meso-NH, with tagged tracers was used to discriminate between African biomass burning, lightnings and Indian anthropogenic pollution as potential sources of precursors for the O3R. Lightning NOx emissions, associated with convective clouds over Africa, were found to be the principal contributor to the ozone enhancement over the Indian Ocean taking advantage of a northeastward jet. This case study illustrates African lightning emissions as an important source for enhanced O 3 in the upper troposphere over the Indian Ocean region during the post-monsoon season.

During the Asian summer monsoon, the circulation in the upper troposphere/lower stratosphere (UTLS) is dominated by the Asian monsoon anticyclone (AMA). Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the Eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3) and its precursors, such as carbon monoxide (CO) and nitrogen oxides (NOx). Many studies based on global modeling and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN) into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the MetOp-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9 % and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26 % but the correlation between both is high (0.94). GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼  25 ppbv) than East Asian emissions (∼  10 ppbv). The correlation between enhanced emissions over the Indo-Gangetic Plain and monsoon deep convection is responsible for this larger impact. Consistently, South Asian anthropogenic NOx emissions also play a larger role in producing O3 within the AMA (∼  8 ppbv) than East Asian emissions (∼  5 ppbv), but Asian lightning-produced NOx is responsible for the largest O3 production (10–14 ppbv). Stratosphere-to-troposphere exchanges are also important in transporting O3 in the upper part of the AMA.

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.

Vertical in situ measurements of aerosols and trace gases were conducted in Fairbanks, Alaska, during winter 2022 as part of the Alaskan Layered Pollution and Chemical Analysis campaign (ALPACA). Using a tethered balloon, the study explores the dispersion of pollutants in the continental high-latitude stable boundary layer (SBL). Analysis of 24 flights revealed a stratified SBL structure with different pollution layers in the lowest tens of meters of the atmosphere, offering unprecedented detail. Surface emissions generally accumulated in a surface mixing layer (ML) extending to an average of 51 m, with a well-mixed sublayer (MsL) reaching 22 m. The height and concentrations within the ML were strongly influenced by a local wind driven by nearby topography under anticyclonic conditions. During strong radiative cooling, a drainage flow increased turbulence near the surface, altering the temperature profile and deepening the ML. Above the ML, pollution concentrations decreased but showed clear signs of freshly released anthropogenic emissions. Higher in the atmosphere, above elevated inversions, pollution levels were similar to previously reported Arctic haze concentrations, even though Fairbanks' outflow concentrations below elevated inversions were up to 6 times higher, likely due to power plant emissions. In situ measurements indicated that gas and particle tracer ratios in elevated power plant plumes differed significantly from those near the surface. Overall, pollution layers were strongly correlated with the temperature stratification and emission heights, emphasizing the need for improved representation of temperature inversions and emission sources in air quality models to enhance pollution forecasts.

During the Asian summer monsoon, the circulation in the upper troposphere/lower stratosphere (UTLS) is dominated by the Asian monsoon anticyclone (AMA). Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the Eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3) and its precursors, such as carbon monoxide (CO) and nitrogen oxides (NOx). Many studies based on global modeling and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN) into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the MetOp-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9 % and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26 % but the correlation between both is high (0.94). GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼ 25 ppbv) than East Asian emissions (∼ 10 ppbv). The correlation between enhanced emissions over the Indo-Gangetic Plain and monsoon deep convection is responsible for this larger impact. Consistently, South Asian anthropogenic NOx emissions also play a larger role in producing O3 within the AMA (∼ 8 ppbv) than East Asian emissions (∼ 5 ppbv), but Asian lightning-produced NOx is responsible for the largest O3 production (10-14 ppbv). Stratosphere-to-troposphere exchanges are also important in transporting O3 in the upper part of the AMA.

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.