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Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted.

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.

The Asian summer monsoon (ASM) as a chemical transport system is investigated using a suite of models in preparation for an airborne field campaign over the Western Pacific. Results show that the dynamical process of anticyclone eddy shedding in the upper troposphere rapidly transports convectively uplifted Asian boundary layer air masses to the upper troposphere and lower stratosphere over the Western Pacific. The models show that the transported air masses contain significantly enhanced aerosol loading and a complex chemical mixture of trace gases that are relevant to ozone chemistry. The chemical forecast models consistently predict the occurrence of the shedding events, but the predicted concentrations of transported trace gases and aerosols often differ between models. The airborne measurements to be obtained in the field campaign are expected to help reduce the model uncertainties. Furthermore, the large‐scale seasonal chemical structure of the monsoon system is obtained from modeled carbon monoxide, a tracer of the convective transport of pollutants, which provides a new perspective of the ASM circulation, complementing the dynamical characterization of the monsoon.

This study investigates the use of airborne in situ measurements to derive transit time distributions (TTD) from the boundary layer (BL) to the upper troposphere (UT) over the highly convective tropical western Pacific (TWP). The feasibility of this method is demonstrated using 42 volatile organic compounds (VOCs) measured during the Convective Transport of Active Species in the Tropics (CONTRAST) experiment. Two important approximations necessary for the application are the constant chemical lifetimes for each compound and the representation of the BL source by the local CONTRAST data. To characterize uncertainties associated with the first approximation, we quantify the changes in derived TTDs when chemical lifetimes are estimated using conditions of the BL, UT, and tropospheric average. With the support of a trajectory model study in a companion paper, we characterize the BL source region contributing to the transport to the sampled UT. In addition to the TTDs derived using a regional average, we analyze the potential information content in locally averaged measurements to represent the dynamical variability of the region. Around 150 TTDs, derived using measurements on a ∼100 km spatial scale, show a distribution of mean and mode transit times consistent with the wide range of convective conditions encountered during the campaign. Two extreme cases, with the shortest and the near‐longest TTD, are examined using the dynamical background of the measurements and back trajectory analyses. The result provides physical consistency supporting the hypothesis that sufficient information can be obtained from measurements to resolve dynamical variability of the region.

Although the tropopause is a well‐established concept, its definition and physical properties remain an active research topic. In the tropics, both the World Meteorological Organization established lapse rate tropopause definition and the minimum in the temperature profile (the cold point) are used to determine the tropopause height. We examine the differences produced by these two definitions using high‐resolution airborne in situ measurements of temperature, water vapor, and ozone in the tropical tropopause layer from a recent experiment over the western Pacific using the National Aeronautics and Space Administration (NASA) Global Hawk unmanned aircraft system. When the two definitions do not produce the same tropopause height, which is in about half of the cases, the combined temperature and trace gas analysis shows that the lapse rate definition better identifies the transition from the troposphere to the stratosphere.

Convective transport from the marine boundary layer to the upper troposphere (UT) is investigated using airborne in situ measurements of chemical species over the tropical western Pacific. Using 42 volatile organic compounds with photochemical lifetimes ranging from shorter than a day to multiple decades, we derive a transit time spectrumG(t)and the associated modal and mean transit times for the UT air mass over the convectively dominant tropical western Pacific region.G(t)describes relative contributions of air masses transported from the marine boundary layer to the UT via all transport paths with different transit times. We further demonstrate that the volatile organic compound‐derived transit time scale is broadly comparable to that estimated from convective mass flux. The observation‐based transit time spectrum not only provides insights into convective transport pathways, but also has the potential to serve as an effective diagnostic for evaluating the representation of convective transport in global models.

Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM‐chem and GEOS‐Chem. CAM‐chem uses an online air‐sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data‐oriented machine‐learning approach. The machine‐learning algorithm is trained using a global suite of seawater acetone measurements. GEOS‐Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global‐scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM‐chem and GEOS‐Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high‐latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere‐lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere.