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During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season. [ABSTRACT FROM AUTHOR]

Chemistry Climate Models (CCMs) are essential tools for characterizing and predicting the role of atmospheric composition and chemistry in Earth's climate system. This study demonstrates the use of airborne in situ observations to diagnose the representation of chemical composition and transport by CCMs. Process‐based diagnostics using dynamical and chemical coordinates are presented which minimize the spatial and temporal sampling differences between airborne in situ measurements and CCM grid points. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves as a rapid transport pathway for surface emissions to reach the upper troposphere and lower stratosphere (UTLS). We examine two CCM configurations for their representation of the ASM UTLS using a set of airborne observations from south Asia. The diagnostics reveal good model performance at representing tropospheric tracer distribution throughout the troposphere and lower stratosphere, and excellent representation of chemical aging in the lower stratosphere when chemical loss is dominated by photolysis. Identified model limitations include the use of zonally averaged mole fraction boundary conditions for species with sufficiently short tropospheric lifetimes, which may obscure enhanced regional emissions sources. Overall, the diagnostics underscore the skill of current‐generation models at representing pollution transport from the boundary layer to the stratosphere via the ASM mechanism, and demonstrate the strength of airborne in situ observations toward characterizing this representation. Plain Language Summary: The chemical composition of Earth's atmosphere is important to understand for future climate prediction. This study establishes an approach for evaluating the representation of chemical composition in global climate models, and demonstrates the capabilities of the approach using a set of observations collected by research aircraft. We specifically target an evaluation of the Asian summer monsoon, a process with a well‐documented transport pathway for chemical species near the surface to reach the upper atmosphere. In doing so, we identify specific areas where focused model improvement is needed. Key Points: Process‐based diagnostics for model evaluation using airborne in situ observations are presentedThe Asian summer monsoon is explored for its role in impacting global composition and climateThe diagnostics use dynamical and chemical coordinates to identify model strengths and limitations [ABSTRACT FROM AUTHOR]

The pristine atmosphere of the southwest Indian Ocean (SWIO) basin underwent significant perturbations during the 2020 austral summer. This study documents the complex variability of aerosols and carbon monoxide (CO) over this remote oceanic region and identifies the processes governing it in the upper troposphere – lower stratosphere (UT-LS). Aerosol profiles exhibit a multi-layer structure in the tropical UT-LS in January and February 2020. The numerical models (FLEXPART and MIMOSA) showed that the modulation of the aerosol content in the lower stratosphere is due to the intense and persistent stratospheric aerosol smoke layer generated during the 2019–20 extreme Australian bushfire events. One part of this stratospheric aerosol smoke layer was advected zonally by the prevailing easterly winds and its passage over Reunion was recorded by increased aerosol extinction profiles on 27th and 28th January. The analysis of the advected potential vorticity highlights an isentropic transport of air masses containing Australian biomass burning aerosol from extra-tropical latitudes to Reunion at the 400 K isentropic level, on 28th January. Interestingly, our results show that the biomass burning activity in eastern Africa, weak during this season, contributed to modulate (up to 90 %) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. The simultaneous presence of African and Australian aerosols smoke layers has been recorded by ground-based observations at Reunion. This study highlights for the first time the influence of the African emissions from biomass burning to the CO and aerosols distribution in the upper troposphere over the SWIO basin during the convective season. The results show that besides PyroCb -driven injection of biomass burning products to the stratosphere, an alternative pathway may exist during the regular deep-convection season in the tropics. [ABSTRACT FROM AUTHOR]

In recent years (2017–2019), several moderate volcanic eruptions and wildfires have perturbed the stratospheric composition and concentration with distinct implications on radiative forcing and climate. The Stratospheric Aerosol and Gas Experiment III instruments onboard the International Space Station (SAGE III/ISS) have been providing aerosol extinction coefficient (EC) profiles at multiple wavelengths since June 2017. In this study, a method to invert the spectral stratospheric aerosol optical depth (sAOD) or EC values from SAGE III/ISS (to retrieve the number/volume size distributions and other microphysical properties) is presented, and the sensitivity of these retrievals is evaluated. It was found that the retrievals are strongly dependent on the choices of wavelengths, which in turn determine the shapes of the calculated curves. Further, we examine the changes in stratospheric aerosol spectral behavior, size distribution properties, time evolution (growth/decay) characteristics associated with subsequent moderate volcanic eruptions, namely, Ambae (15 ∘ S, 167 ∘ E; April and July 2018), Raikoke (48 ∘ N, 153 ∘ E; June 2019), and Ulawun (5 ∘ S, 151 ∘ E; June and August 2019), in different spatial regions. The observational period was classified with reference to Ambae eruptions into four phases (pre-Ambae, Ambae1, Ambae2, and post-Ambae). The pre-Ambae and post-Ambe periods comprise the 2017 Canadian fires and 2019 Raikoke/Ulawun eruptions, respectively. The spectral dependence of sAOD was comparable and lowest during the pre-Ambae and Ambae1 periods in all regions. The number concentration at the principal mode radius (between 0.07 and 0.2 μ m) was observed to be higher during the Ambae2 period over the Northern Hemisphere (NH). The rate of change (growth/decay) in the sAOD on a global scale resembled the changes in the Southern Hemisphere (SH), unlike the time-lag-associated changes in the NH. These differences could be attributed to the prevailing horizontal and vertical dispersion mechanisms in the respective regions. Lastly, the radiative forcing estimates of Ambae and Raikoke/Ulawun eruptions, as reported in recent studies, was discussed by taking clues from other major and moderate eruptions to gain insight on their role in climate change. [ABSTRACT FROM AUTHOR]

As a consequence of extreme heat and drought, record-breaking wildfires developed and ravaged south-eastern Australia during the fire season 2019-2020. The fire strength reached its paroxysmal phase at the turn of the year 2019-2020. During this phase, pyro-Cb developed and injected biomass burning aerosols and gases into the upper-troposphere--lowerstratosphere (UTLS). The UTLS aerosol layer was massively perturbed by these fires, with aerosol extinction increased by a factor 3 in the visible spectral range in the Southern Hemisphere, with respect to a background atmosphere, and stratospheric aerosol optical depth reaching values as large as 0.015 in February 2020. Using the best available description of this event by observations, we estimate the radiative forcing (RF) of such perturbations of the Southern-Hemispheric aerosol layer. We use offline radiative transfer modelling driven by observed information of the aerosol extinction perturbation and its spectral variability obtained from limb satellite measurements. Based on hypotheses on the absorptivity and the angular scattering properties of the aerosol layer, the regional (at three latitude bands in the Southern Hemisphere) clear-sky TOA (top-ofatmosphere) RF is found varying from small positive values to relatively large negative values (up to -2.0 W/m2), and the regional clear-sky surface RF is found to be consistently negative and reaching large values (up to -4.5 W/m2). We argue that clear-sky positive values are unlikely for this event, if the aging/mixing of the biomass burning plume is mirrored by the evolution of its optical properties. Our best estimate for the area-weighted global-equivalent clear-sky RF is -0.35±0.21 TOA RF) and -0.94±0.26 W/m2 (surface RF), thus the strongest documented for a fire event and of comparable magnitude with the strongest volcanic eruptions of the post-Pinatubo era. The surplus of RF at the surface, with respect to TOA, is due absorption within the plume that has contributed to the generation of ascending smoke vortices in the stratosphere. Highly reflective underlying surfaces, like clouds, can nevertheless swap negative to positive TOA RF, with global average RF as high as +1.0 W/m2 assuming highly absorbing particles. [ABSTRACT FROM AUTHOR]