Global Distribution of the Phase State and Mixing Times within Secondary Organic Aerosol Particles in the Troposphere Based on Room-Temperature Viscosity Measurements
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The southern slope of the Tibetan Plateau (SSTP) is one of the rainiest regions in the world where geological hazards caused by extreme precipitation often occur. This study investigates the characteristics and mechanisms of extreme precipitation over SSTP from June to September during 2001–2020 using Global Precipitation Measurement satellite observation. The extreme precipitation days are defined as the days with top 5% of regional-mean daily precipitation over SSTP in this period, which has an average precipitation of 27.2 mm/d. Averaging over the extreme precipitation days, precipitation peaks at an altitude of about 300 m, coinciding with the climatological maximum precipitation, but with a much larger value of 37.2 mm/d than the climatology of 11.9 mm/d. Composite analysis of circulations on extreme days reveals significant circulation anomalies in both the lower and upper troposphere. Specifically, the lower-tropospheric circulations are characterized by significant westerly anomalies over northern India, and the upper-tropospheric circulations are characterized by northerly anomalies over the central Tibetan Plateau, which are statistically independent. The lower-tropospheric westerly anomalies blowing toward SSTP are blocked by the topography, favoring extreme precipitation over SSTP. The upper-tropospheric northerly anomalies, on the other hand, correspond to anomalous northeasterlies north of SSTP in the middle troposphere and southeasterlies to the south in the lower troposphere, and the convergence of these circulation anomalies favors extreme precipitation over SSTP. Lastly, the lower-tropospheric westerly and upper-tropospheric northerly anomalies, respectively, correspond to less precipitation over the South Asian monsoon region and the Tibetan Plateau.
Observed Madden-Julian Oscillation (MJO) events are examined with the aid of regional model simulations to understand the role of cloud radiative effects in the MJO development. The importance of this role is demonstrated by the absence of MJO in the model simulations that contain no cloud radiative effects. Comparisons of model simulations with and without the cloud radiative effects and observation help identify the major processes arising from those effects. Those processes develop essentially from heating in the upper-troposphere due to shortwave absorption within anvil clouds in the upper troposphere and the convergence of longwave radiation in the middle-upper troposphere, with a peak at 300-hPa, during deep convection. First, that heating adds extra buoyancy and accelerates the rising motion in the upper troposphere in deep convection. The vertical acceleration in the upper troposphere creates a vacuum effect and demands for more deep convection to develop. Second, in response to that demand and required by mass balance arises the large-scale horizontal and vertical mass, moisture, and energy convergence. It strengthens deep convection and, with the feedback from continuing cloud radiative effect, creates conditions that can perpetuate deep convection and MJO development. That perpetuation does not occur however because those processes arising from the cloud radiative heating in the upper troposphere stabilize the troposphere till it supports no further deep convection. Weakening deep convection reduces cloud radiative effects. The subsequent reduction of the vacuum effect in the upper troposphere diminishes deep convection completing an MJO cycle. These results advance our understanding of the development of the MJO in the radiative-convective system over warm waters in the tropics. They show that while the embryo of intraseasonal oscillation may exist in the system its growth/development is largely dependent on cloud radiative effects and feedbacks.
Abstract. The mean altitude of the smoke loading over the southeast Atlantic moves from the boundary layer in July to the free troposphere by October. This study details the month-by-month changes in cloud properties and the large-scale environment as a function of the biomass burning aerosol loading at Ascension Island (8∘ S, 14.5∘ W) from July to October, based on island measurements, satellite retrievals, and reanalysis. In July and August, the smoke loading predominantly varies within the boundary layer. During both months, the low-cloud fraction is less and is increasingly cumuliform when more smoke is present, with the exception of a late morning boundary layer deepening that encourages a short-lived cloud development. The meteorology varies little, suggesting aerosol–cloud interactions explain the cloudiness changes. September marks a transition month during which midlatitude disturbances can intrude into the Atlantic subtropics, constraining the free tropospheric aerosol closer to the African coast. Stronger boundary layer winds on cleaner days help deepen, dry, and cool much of the marine boundary layer compared to that on days with high smoke loadings, with stratocumulus reducing everywhere but at the northern deck edge. The September free troposphere is better mixed on smoky days compared to October. Longwave cooling rates, generated by a sharp water vapor gradient at the aerosol layer top, encourage a small-scale vertical mixing that could help maintain the well-mixed smoky September free troposphere. The October meteorology primarily varies as a function of the strength of the free tropospheric winds advecting aerosol offshore. The free tropospheric aerosol loading is less than in September, and the moisture variability is greater. Low-level clouds increase and are more stratiform in October when the smoke loadings are higher. The increased free tropospheric moisture can help sustain the clouds through a reduction in evaporative drying during cloud-top entrainment. Enhanced subsidence above the coastal upwelling region, increasing cloud droplet number concentrations, may further prolong cloud lifetime through microphysical interactions. Reduced subsidence underneath stronger free tropospheric winds at Ascension Island supports slightly higher cloud tops during smokier conditions. Overall, the monthly changes in the large-scale aerosol and moisture vertical structure act to amplify the seasonal cycle in low-cloud amount and morphology. This is climatically important, as cloudiness changes dominate changes in the top-of-atmosphere radiation budget.
Aerosol‐cloud interactions are a persistent source of uncertainty in climate research. This study presents findings from a model intercomparison project examining the impact of aerosols on clouds and climate in convection‐permitting radiative‐convective equilibrium (RCE) simulations. Specifically, 11 different modeling teams conducted RCE simulations under varying aerosol concentrations, domain configurations, and sea surface temperatures (SSTs). We analyze the response of domain‐mean cloud and radiative properties to imposed aerosol concentrations across different SSTs. Additionally, we explore the potential impact of aerosols on convective aggregation and large‐scale circulation in large‐domain simulations. The results reveal that the cloud and radiative responses to aerosols vary substantially across models. However, a common trend across models, SSTs, and domain configurations is that increased aerosol loading tends to suppress warm rain formation, enhance cloud water content in the mid‐troposphere, and consequently increase mid‐tropospheric humidity and upper‐tropospheric temperature, thereby impacting static stability. The warming of the upper troposphere can be attributed to reduced lateral entrainment effects due to the higher environmental humidity in the mid‐troposphere. However, models do not agree on aerosol impacts on convective updraft velocity based on the preliminary examination of high‐percentiles of vertical velocity at a single mid‐troposheric layer (500 hPa). In large‐domain simulations, where convection tends to self‐organize, aerosol loading does not consistently influence self‐organization but tends to reduce the intensity of large‐scale circulation forming between convective clusters and dry regions. This reduction in circulation intensity can be explained by the increase in static stability due to the upper tropospheric warming.
Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.
Abstract. Previous studies have found that low-level Arctic clouds often persist for long periods even in the face of very low surface cloud condensation nuclei (CCN) concentrations. Here, we investigate whether these conditions could occur due to continuous entrainment of aerosol particles from the free troposphere (FT). We use an idealized large eddy simulation (LES) modeling framework, where aerosol concentrations are low in the boundary layer (BL) but increased up to 50× in the free troposphere. We find that the tests with higher tropospheric aerosol concentrations simulated clouds, which persisted for longer and maintained higher liquid water paths (LWPs). This is due to direct entrainment of the tropospheric aerosol into the cloud layer, which results in a precipitation suppression from the increase in cloud droplet number and in stronger cloud-top radiative cooling, which causes stronger circulations maintaining the cloud in the absence of surface forcing. Together, these two responses result in a more well-mixed boundary layer with a top that remains in contact with the tropospheric aerosol reservoir and can maintain entrainment of those aerosol particles. The surface aerosol concentrations, however, remained low in all simulations. The free-tropospheric aerosol concentration necessary to maintain the clouds is consistent with concentrations that are frequently seen in observations.
Abstract. This study assesses the relative importance of time integration error in present-day climate simulations conducted with the atmosphere component of the Energy Exascale Earth System Model version 1 (EAMv1) at 1∘ horizontal resolution. We show that a factor-of-6 reduction of time step size in all major parts of the model leads to significant changes in the long-term mean climate. Examples of changes in 10-year mean zonal averages include the following: up to 0.5 K of warming in the lower troposphere and cooling in the tropical and subtropical upper troposphere, 1 %–10 % decreases in relative humidity throughout the troposphere, and 10 %–20 % decreases in cloud fraction in the upper troposphere and decreases exceeding 20 % in the subtropical lower troposphere. In terms of the 10-year mean geographical distribution, systematic decreases of 20 %–50 % are seen in total cloud cover and cloud radiative effects in the subtropics. These changes imply that the reduction of temporal truncation errors leads to a notable although unsurprising degradation of agreement between the simulated and observed present-day climate; to regain optimal climate fidelity in the absence of those truncation errors, the model would require retuning. A coarse-grained attribution of the time step sensitivities is carried out by shortening time steps used in various components of EAM or by revising the numerical coupling between some processes. Our analysis leads to the finding that the marked decreases in the subtropical low-cloud fraction and total cloud radiative effect are caused not by the step size used for the collectively subcycled turbulence, shallow convection, and stratiform cloud macrophysics and microphysics parameterizations but rather by the step sizes used outside those subcycles. Further analysis suggests that the coupling frequency between the subcycles and the rest of EAM significantly affects the subtropical marine stratocumulus decks, while deep convection has significant impacts on trade cumulus. The step size of the cloud macrophysics and microphysics subcycle itself appears to have a primary impact on cloud fraction in the upper troposphere and also in the midlatitude near-surface layers. Impacts of step sizes used by the dynamical core and the radiation parameterization appear to be relatively small. These results provide useful clues for future studies aiming at understanding and addressing the root causes of sensitivities to time step sizes and process coupling frequencies in EAM. While this study focuses on EAMv1 and the conclusions are likely model-specific, the presented experimentation strategy has general value for weather and climate model development, as the methodology can help researchers identify and understand sources of time integration error in sophisticated multi-component models.
Abstract Mechanical forcing by orography affects precipitating convection across many tropical regions, but controls on the intensity and horizontal extent of the orographic precipitation peak and rain shadow remain poorly understood. A recent theory explains this control of precipitation as arising from modulation of lower-tropospheric temperature and moisture by orographic mechanical forcing, setting the distribution of convective rainfall by controlling parcel buoyancy. Using satellite and reanalysis data, we evaluate this theory by investigating spatiotemporal precipitation variations in six mountainous tropical regions spanning South and Southeast Asia, and the Maritime Continent. We show that a strong relationship holds in these regions between daily precipitation and a measure of convective plume buoyancy. This measure depends on boundary layer thermodynamic properties and lower-free-tropospheric moisture and temperature. Consistent with the theory, temporal variations in lower-free-tropospheric temperature are primarily modulated by orographic mechanical lifting through changes in cross-slope wind speed. However, winds directed along background horizontal moisture gradients also influence lower-tropospheric moisture variations in some regions. The buoyancy measure is also shown to explain many aspects of the spatial patterns of precipitation. Finally, we present a linear model with two horizontal dimensions that combines mountain wave dynamics with a linearized closure exploiting the relationship between precipitation and plume buoyancy. In some regions, this model skillfully captures the spatial structure and intensity of rainfall; it underestimates rainfall in regions where time-mean ascent in large-scale convergence zones shapes lower-tropospheric humidity. Overall, these results provide new understanding of fundamental processes controlling subseasonal and spatial variations in tropical orographic precipitation.
Motivated by recent discussions concerning differences of convective dynamics in polluted and pristine environments, the so-called convective invigoration in particular, this paper provides an analysis of factors affecting convective updraft buoyancy, such as the in-cloud supersaturation, condensate and precipitation loading, and entrainment. We use the deep convective period from simulations of daytime convection development over land discussed in our previous publications. An entraining parcel framework is used in the theoretical analysis. We show that for the specific case considered here, finite (positive) supersaturation noticeably reduces pseudo-adiabatic parcel buoyancy and cumulative convective available potential energy (cCAPE) in the lower troposphere. This comes from keeping a small fraction of the water vapor in a supersaturated state and thus reducing the latent heating. Such a lower-tropospheric impact is comparable to the effects of condensate loading and entrainment in the idealized parcel framework. For the entire tropospheric depth, loading and entrainment have a much more significant impact on the total CAPE. For the cloud model results, we compare ensemble simulations applying either a bulk microphysics scheme with saturation adjustment or a more comprehensive double-moment scheme with supersaturation prediction. We compare deep convective updraft velocities, buoyancies, and supersaturations from all ensembles. In agreement with the parcel analysis, the saturation-adjustment scheme provides noticeably stronger updrafts in the lower troposphere. For the simulations predicting supersaturation, there are small differences between pristine and polluted conditions below the freezing level that are difficult to explain by standard analysis of the in-cloud buoyancy components. By applying the piggybacking technique, we show that the lower-tropospheric buoyancy differences between pristine and polluted simulations come from a combination of temperature (i.e., latent heating) and condensate loading differences that work together to make polluted buoyancies and updraft velocities slightly larger when compared to their pristine analogues. Overall, the effects are rather small and contradict previous claims of a significant invigoration of deep convection in polluted environments.
Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.
Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (~1–2 K) and greatly enhanced moisture (>2 g kg -1 ) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.
We report that throughout the troposphere over the Amazon rainforest, isoprene epoxydiol-secondary organic aerosols (IEPOX-SOA) are key components of submicrometer particle mass. IEPOX-SOA is thought to form by multiphase chemical pathways in the atmosphere, but using detailed model simulations, we show that these pathways are strongly inhibited by the solid particle phase state prevailing in the upper troposphere. We find that 2-methyltetrol gases formed by in-plant biochemical oxidation pathways, their partitioning to fine particles, and dissolution in cloud droplets can explain over 90% of IEPOX-SOA mass concentrations in the upper troposphere. In agreement with previous PM10 chiral measurements, our simulations indicate that plant biochemical processes are the dominant source of particulate 2-methyltetrols in the lower troposphere as well (>70%). Our results imply that in-plant biochemistry plays a central but previously unidentified role in aerosol processes and atmosphere-biosphere-climate interactions over the rainforest.
Abstract The depth of convective clouds affects vertical transport of atmospheric constituents, influencing downstream weather and climate. Atmospheric controls on the maximum depth reached by moist convection are investigated with radar‐tracked convective cells tagged with sounding‐derived atmospheric parameters from a field campaign in central Argentina. Regression analyses show that narrow (<12‐km diameter) and wide (>16‐km diameter) cell depths respond to disparate factors, where cell areas are defined using composite reflectivity signatures. Undiluted lifted parcel indices including convective available potential energy (CAPE) and level of neutral buoyancy (LNB) are top predictors of wide cell maximum depth while mid‐tropospheric relative humidity is the top predictor of narrow cell maximum depth. Because narrow cells are more numerous than wide cells, the overall outcome of the full cell population does not strongly correlate with CAPE and LNB conditions. Tracked cells and atmospheric conditions in a simulation with 3‐km grid spacing covering the field campaign produce similar results to those observed. Narrow cells that are relatively deep have a cooler and moister mid‐troposphere with weaker free tropospheric subsidence, while relatively deep wide cells have much warmer and moister lower tropospheric conditions. These atmospheric differences are present 1 hr before cell initiation at both a fixed observing site and variable cell initiation locations. Simulated narrow cell maximum equivalent potential temperature decreases with height at a rate similar to the ambient vertical gradient, causing these cells to fall short of their LNB and supporting the view that entrainment‐driven dilution is a dominant control on their depth.