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    Local and Remote Controls on Arctic Mixed-Layer Evolution
    (Malden MA: Wiley-Blackwell, 2020) Neggers, R.A.J.; Chylik, J.; Egerer, U.; Griesche, H.; Schemann, V.; Seifert, P.; Siebert, H.; Macke, A.
    In this study Lagrangian large-eddy simulation of cloudy mixed layers in evolving warm air masses in the Arctic is constrained by in situ observations from the recent PASCAL field campaign. A key novelty is that time dependence is maintained in the large-scale forcings. An iterative procedure featuring large-eddy simulation on microgrids is explored to calibrate the case setup, inspired by and making use of the typically long memory of Arctic air masses for upstream conditions. The simulated mixed-phase clouds are part of a turbulent mixed layer that is weakly coupled to the surface and is occasionally capped by a shallow humidity layer. All eight simulated mixed layers exhibit a strong time evolution across a range of time scales, including diurnal but also synoptic fingerprints. A few cases experience rapid cloud collapse, coinciding with a rapid decrease in mixed-layer depth. To gain insight, composite budget analyses are performed. In the mixed-layer interior the heat and moisture budgets are dominated by turbulent transport, radiative cooling, and precipitation. However, near the thermal inversion the large-scale vertical advection also contributes significantly, showing a distinct difference between subsidence and upsidence conditions. A bulk mass budget analysis reveals that entrainment deepening behaves almost time-constantly, as long as clouds are present. In contrast, large-scale subsidence fluctuates much more strongly and can both counteract and boost boundary-layer deepening resulting from entrainment. Strong and sudden subsidence events following prolonged deepening periods are found to cause the cloud collapses, associated with a substantial reduction in the surface downward longwave radiative flux. ©2019. The Authors.
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    New SOA Treatments Within the Energy Exascale Earth System Model (E3SM): Strong Production and Sinks Govern Atmospheric SOA Distributions and Radiative Forcing
    (Malden MA: Wiley-Blackwell, 2020) Lou, Sijia; Shrivastava, Manish; Easter, Richard C.; Yang, Yang; Ma, Po‐Lun; Wang, Hailong; Cubison, Michael J.; Campuzano‐Jost, Pedro; Jimenez, Jose L.; Zhang, Qi; Rasch, Philip J.; Shilling, John E.; Zelenyuk, Alla; Dubey, Manvendra; Cameron‐Smith, Philip; Martin, Scot T.; Schneider, Johannes; Schulz, Christiane
    Secondary organic aerosols (SOA) are large contributors to fine particle mass loading and number concentration and interact with clouds and radiation. Several processes affect the formation, chemical transformation, and removal of SOA in the atmosphere. For computational efficiency, global models use simplified SOA treatments, which often do not capture the dynamics of SOA formation. Here we test more complex SOA treatments within the global Energy Exascale Earth System Model (E3SM) to investigate how simulated SOA spatial distributions respond to some of the important but uncertain processes affecting SOA formation, removal, and lifetime. We evaluate model predictions with a suite of surface, aircraft, and satellite observations that span the globe and the full troposphere. Simulations indicate that both a strong production (achieved here by multigenerational aging of SOA precursors that includes moderate functionalization) and a strong sink of SOA (especially in the middle upper troposphere, achieved here by adding particle-phase photolysis) are needed to reproduce the vertical distribution of organic aerosol (OA) measured during several aircraft field campaigns; without this sink, the simulated middle upper tropospheric OA is too large. Our results show that variations in SOA chemistry formulations change SOA wet removal lifetime by a factor of 3 due to changes in horizontal and vertical distributions of SOA. In all the SOA chemistry formulations tested here, an efficient chemical sink, that is, particle-phase photolysis, was needed to reproduce the aircraft measurements of OA at high altitudes. Globally, SOA removal rates by photolysis are equal to the wet removal sink, and photolysis decreases SOA lifetimes from 10 to ~3 days. A recent review of multiple field studies found no increase in net OA formation over and downwind biomass burning regions, so we also tested an alternative, empirical SOA treatment that increases primary organic aerosol (POA) emissions near source region and converts POA to SOA with an aging time scale of 1 day. Although this empirical treatment performs surprisingly well in simulating OA loadings near the surface, it overestimates OA loadings in the middle and upper troposphere compared to aircraft measurements, likely due to strong convective transport to high altitudes where wet removal is weak. The default improved model formulation (multigenerational aging with moderate fragmentation and photolysis) performs much better than the empirical treatment in these regions. Differences in SOA treatments greatly affect the SOA direct radiative effect, which ranges from -0.65 (moderate fragmentation and photolysis) to -2 W m-2 (moderate fragmentation without photolysis). Notably, most SOA formulations predict similar global indirect forcing of SOA calculated as the difference in cloud forcing between present-day and preindustrial simulations. © 2020. The Authors.