Carbonyl sulfide (OCS) is an important atmospheric sulfur species that plays a dominant role in the formation of (non-volcanic) stratospheric sulfate aerosol in the middle stratosphere. Major uncertainties in surface sources and sinks and inconsistent model representation of vertical transport limit understanding of OCS distribution, particularly in the sparsely sampled upper atmosphere. During the 2022 Asian Summer Monsoon Chemical & CLimate Impact Project (ACCLIP) campaign in-situ measurements of OCS in the Upper Troposphere and Lower Stratosphere (UTLS) at the eastern edge of the Asian Summer Monsoon anticyclone (ASM), showed significant OCS enhancements (>750 ppt) near the tropopause from convectively influenced air parcels. Here we compare these novel Asian UTLS measurements with long term satellite observations and regional measurements to broaden understanding of OCS trends and its transport by the ASM. Trajectory analysis identifies the main source regions for deep convective lofting and demonstrates ASM entrainment of OCS enriched parcels in the UTLS, allowing evaluation of global model predictions for OCS’s stratospheric influence. The ACCLIP dataset provides vital in-situ validation of limited vertically resolved OCS data in a region of significant anthropogenic emissions, which serves to enhance our understanding of the global sulfur budget.

Refractory black carbon (rBC) is a primary aerosol species, produced through incomplete combustion, that absorbs sunlight and contributes to positive radiative forcing. The overall climate effect of rBC depends on its spatial distribution and atmospheric lifetime, both of which are impacted by the efficiency with which rBC is transported or removed by convective systems. These processes are poorly constrained by observations. It is especially interesting to investigate rBC transport efficiency through the Asian Summer Monsoon (ASM) since this meteorological pattern delivers vast quantities of boundary layer air from Asia, where rBC emissions are high, to the upper troposphere/lower stratosphere (UT/LS) where the lifetime of rBC is expected to be long. Here we present in-situ observations of rBC made during the Asian Summer Monsoon Chemistry and Climate Impact Project (ACCLIP) of summer, 2022. We use observed relationships between rBC and CO in ASM outflow to show that rBC is removed nearly completely (>98%) from uplifted air, and that rBC concentrations in ASM outflow are statistically indistinguishable from the UT/LS background. We compare observed rBC and CO concentrations to those expected based on two chemical transport models and find that the models reproduce CO to within a factor of 2 at all altitudes while rBC is overpredicted by a factor of 20-100 at altitudes associated with ASM outflow. We find that the rBC particles in recently convected air have thinner coatings than those found in the UTLS background, suggesting non-zero transport of rBC number that is not relevant to concentration.

The Asian Summer Monsoon (ASM) has garnered attention in recent years for its impacts on the composition of the upper troposphere and lower stratosphere (UTLS) via deep convection. A recent observational effort into this mechanism, the Asian summer monsoon Chemical and CLimate Impact Project (ACCLIP), sampled the composition of the ASM UTLS over the northwestern Pacific during boreal summer 2022 using two airborne platforms. In this work, we integrate Lagrangian trajectory modeling with convective cloud top observations to diagnose ASM convective transport which contributed to ACCLIP airborne observations. This diagnostic is applied to explore the properties of convective transport associated with prominent ASM sub-systems, revealing that convective transport along the East Asia Subtropical Front generally contained more pollutants than from South Asia, for species ranging in lifetime from days to months. The convective transport diagnostic is used to isolate three convective transport events over eastern Asia which had distinct chemical tracer relationship slopes, indicating the different economical behaviors of the contributing source regions. One of these transport events is explored in greater detail, where a polluted air mass was sampled from convection over the Northeast China Plain. This event was largely confined to 12-15 km altitude, which may be high enough to impact the composition of the stratosphere. Overall, the presented diagnosis of convective transport contribution to ACCLIP airborne sampling indicates a key scientific success of the campaign and enables process studies of the climate interactions from the two ASM sub-system.

Chemistry transport models (CTMs) 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 atmospheric composition by global CTMs. Process-based diagnostics are developed which minimize the spatial and temporal sampling differences between airborne in situ measurements and CTM grid points. The developed diagnostics make use of dynamical and chemical vertical coordinates as a means of highlighting areas where focused model improvement is needed. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves a unique pathway for rapid transport of surface emissions and pollutants to the stratosphere. Two global CTM configurations are examined for their representation of the ASM upper troposphere and lower stratosphere (UTLS), using airborne observations collected over south Asia. Application of the developed diagnostics to the CTMs reveals the limitations of zonally-averaged surface boundary conditions for species with sufficiently short tropospheric lifetimes, and that species whose stratospheric loss rates are dominated by photolysis have excellent agreement compared to that observed. Overall, the diagnostics demonstrate the strength of airborne observations toward improving model predictions, and highlight the utility of highly-resolved CTMs to improve the understanding of reactive transport of anthropogenic pollutants to the stratosphere.