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How convective boundary‐layer (CBL) processes modify fluxes of sensible (SH) and latent (LH) heat and CO₂(F_c) in the atmospheric surface layer (ASL) remains a recalcitrant problem. Here, large eddy simulations for the CBL show that whileSHin the ASL decreases linearly with height regardless of soil moisture conditions,LHandF_cdecrease linearly with height over wet soils but increase with height over dry soils. This varying flux divergence/convergence is regulated by changes in asymmetric flux transport between top‐down and bottom‐up processes. Such flux divergence and convergence indicate that turbulent fluxes measured in the ASL underestimate and overestimate the “true” surface interfacial fluxes, respectively. While the non‐closure of the surface energy balance persists across all soil moisture states, it improves over drier soils due to overestimatedLH. The non‐closure does not imply thatF_cis always underestimated;F_ccan be overestimated over dry soils despite the non‐closure issue.

 

Li‐rich rocksalt oxides are promising cathode materials for lithium‐ion batteries due to their large capacity and energy density, and their ability to use earth‐abundant elements. The excess Li in the rocksalt, needed to achieve good Li transport, reduces the theoretical transition metal redox capacity and introduces a labile oxygen state, both of which lead to increased oxygen oxidation and concomitant capacity loss with cycling. Herein, it is demonstrated that substituting the labile oxygen in Li‐rich cation‐disordered rocksalt materials with a vacancy is an effective strategy to inhibit oxygen oxidation. It is found that the oxygen vacancy in cation‐disordered lithium manganese oxide favors high Li coordination thereby reducing the concentration of unhybridized oxygen states, while increasing the theoretical Mn capacity. It is shown that in the vacancy‐containing compound, synthesized by ball milling, the Mn valence is lowered to less than +3, providing access to more than 300 mAh g⁻¹capacity from the Mn²⁺/Mn⁴⁺redox reservoir. The increased transition metal redox and decreased O oxidation are found to improve the capacity and voltage retention, indicating that oxygen vacancy creation to remove the most vulnerable oxygen ions and reduce transition metal valence provides a new opportunity for the design of high‐performance Li‐rich rocksalt cathodes.

 

Experimental evidence shows that temperature‐humidity () similarity in the atmospheric surface layer (ASL) is reduced as Bowen ratio () increases over land. However, underlying physical mechanisms remain not well understood. With large‐eddy simulations,dissimilarity is investigated in the steady‐state, convective boundary layer (CBL) over homogeneous landscape with varying. Asincreases from 0.4 to 2.0, the entrainment ratio forslightly decreases but that forqlargely increases. As a result, local production of humidity variance is substantially enhanced in the upper CBL and transported to the lower CBL by vigorous large eddies, contributing significantly to nonlocal fraction. However, the increased temperature variance in the ASL associated with strong heat flux is larger than that transported from the upper CBL. Such asymmetry in vertical diffusion induced by varying partitioning of surface fluxes strongly regulatesdissimilarity even under perfect conditions valid for Monin‐Obukhov similarity theory.

 

Abstract. Wildfire smoke is one of the most significant concerns ofhuman and environmental health, associated with its substantial impacts onair quality, weather, and climate. However, biomass burning emissions andsmoke remain among the largest sources of uncertainties in air qualityforecasts. In this study, we evaluate the smoke emissions and plumeforecasts from 12 state-of-the-art air quality forecasting systemsduring the Williams Flats fire in Washington State, US, August 2019, whichwas intensively observed during the Fire Influence on Regional to GlobalEnvironments and Air Quality (FIREX-AQ) field campaign. Model forecasts withlead times within 1 d are intercompared under the same framework basedon observations from multiple platforms to reveal their performanceregarding fire emissions, aerosol optical depth (AOD), surface PM2.5,plume injection, and surface PM2.5 to AOD ratio. The comparison ofsmoke organic carbon (OC) emissions suggests a large range of daily totalsamong the models, with a factor of 20 to 50. Limited representations of thediurnal patterns and day-to-day variations of emissions highlight the needto incorporate new methodologies to predict the temporal evolution andreduce uncertainty of smoke emission estimates. The evaluation of smoke AOD(sAOD) forecasts suggests overall underpredictions in both the magnitude andsmoke plume area for nearly all models, although the high-resolution modelshave a better representation of the fine-scale structures of smoke plumes.The models driven by fire radiativepower (FRP)-based fire emissions or assimilating satellite AODdata generally outperform the others. Additionally, limitations of thepersistence assumption used when predicting smoke emissions are revealed bysubstantial underpredictions of sAOD on 8 August 2019, mainly over thetransported smoke plumes, owing to the underestimated emissions on7 August. In contrast, the surface smoke PM2.5 (sPM2.5) forecastsshow both positive and negative overall biases for these models, with mostmembers presenting more considerable diurnal variations of sPM2.5.Overpredictions of sPM2.5 are found for the models driven by FRP-basedemissions during nighttime, suggesting the necessity to improve verticalemission allocation within and above the planetary boundary layer (PBL).Smoke injection heights are further evaluated using the NASA LangleyResearch Center's Differential Absorption High Spectral Resolution Lidar(DIAL-HSRL) data collected during the flight observations. As the firebecame stronger over 3–8 August, the plume height became deeper, with aday-to-day range of about 2–9 km a.g.l. However, narrower ranges arefound for all models, with a tendency of overpredicting the plume heights forthe shallower injection transects and underpredicting for the days showingdeeper injections. The misrepresented plume injection heights lead toinaccurate vertical plume allocations along the transects corresponding totransported smoke that is 1 d old. Discrepancies in model performance forsurface PM2.5 and AOD are further suggested by the evaluation of theirratio, which cannot be compensated for by solely adjusting the smoke emissionsbut are more attributable to model representations of plume injections,besides other possible factors including the evolution of PBL depths andaerosol optical property assumptions. By consolidating multiple forecastsystems, these results provide strategic insight on pathways to improvesmoke forecasts. 

Aerosols have significant and complex impacts on regional climate in East Asia. Cloud‐aerosol‐precipitation interactions (CAPI) remain most challenging in climate studies. The quantitative understanding of CAPI requires good knowledge of aerosols, ranging from their formation, composition, transport, and their radiative, hygroscopic, and microphysical properties. A comprehensive review is presented here centered on the CAPI based chiefly, but not limited to, publications in the special section named EAST‐AIRcpc concerning (1) observations of aerosol loading and properties, (2) relationships between aerosols and meteorological variables affecting CAPI, (3) mechanisms behind CAPI, and (4) quantification of CAPI and their impact on climate. Heavy aerosol loading in East Asia has significant radiative effects by reducing surface radiation, increasing the air temperature, and lowering the boundary layer height. A key factor is aerosol absorption, which is particularly strong in central China. This absorption can have a wide range of impacts such as creating an imbalance of aerosol radiative forcing at the top and bottom of the atmosphere, leading to inconsistent retrievals of cloud variables from space‐borne and ground‐based instruments. Aerosol radiative forcing can delay or suppress the initiation and development of convective clouds whose microphysics can be further altered by the microphysical effect of aerosols. For the same cloud thickness, the likelihood of precipitation is influenced by aerosols: suppressing light rain and enhancing heavy rain, delaying but intensifying thunderstorms, and reducing the onset of isolated showers in most parts of China. Rainfall has become more inhomogeneous and more extreme in the heavily polluted urban regions.