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Abstract 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 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 whereas 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 transport of a small number of rBC particles that are negligible for concentration.
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Evaluating the Model Representation of Asian Summer Monsoon Upper Troposphere and Lower Stratosphere Transport and Composition Using Airborne In Situ Observations
Abstract 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.
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- PAR ID:
- 10492057
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 129
- Issue:
- 4
- ISSN:
- 2169-897X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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