A strong statistical link between aerosol indirect effects and the self-similarity of rainfall distributions

We use convective-scale simulations of monsoonal clouds to reveal a self-similar probability density function that underpins surface rainfall statistics. This density is independent of cloud-droplet number concentration and is unchanged by aerosol perturbations. It therefore represents an invariant property of our model with respect to cloud-aerosol interactions. For a given aerosol concentration, if the dependence of at least one moment of the rainfall distribution on cloud-droplet number is a known input parameter, then the self-similar density can be used to reconstruct the entire rainfall distribution to a useful degree of accuracy. In particular, we present both single-moment and double-moment reconstructions that are able to predict the responses of the rainfall distributions to changes in aerosol concentration. In doing so we show that the seemingly high-dimensional space of possible aerosol-induced rainfall-distribution transformations can be parametrized by a surprisingly small (at most three) independent “degrees of freedom”: the self-similar density, and auxiliary information about two moments of the rainfall distribution. This suggests that, although aerosol-indirect effects on any specific hydro-meteorological system may be multifarious in terms of rainfall changes and physical mechanisms, there may, nevertheless, be a universal constraint on the number of independent degrees of freedom needed to represent the dependencies of rainfall on aerosols.

Coexistence of three liquid phases in individual atmospheric aerosol particles

Individual atmospheric particles can contain mixtures of primary organic aerosol (POA), secondary organic aerosol (SOA), and secondary inorganic aerosol (SIA). To predict the role of such complex multicomponent particles in air quality and climate, information on the number and types of phases present in the particles is needed. However, the phase behavior of such particles has not been studied in the laboratory, and as a result, remains poorly constrained. Here, we show that POA+SOA+SIA particles can contain three distinct liquid phases: a low-polarity organic-rich phase, a higher-polarity organic-rich phase, and an aqueous inorganic-rich phase. Based on our results, when the elemental oxygen-to-carbon (O:C) ratio of the SOA is less than 0.8, three liquid phases can coexist within the same particle over a wide relative humidity range. In contrast, when the O:C ratio of the SOA is greater than 0.8, three phases will not form. We also demonstrate, using thermodynamic and kinetic modeling, that the presence of three liquid phases in such particles impacts their equilibration timescale with the surrounding gas phase. Three phases will likely also impact their ability to act as nuclei for liquid cloud droplets, the reactivity of these particles, and the mechanism of SOA formation and growth in the atmosphere. These observations provide fundamental information necessary for improved predictions of air quality and aerosol indirect effects on climate.

Aerosol impacts on warm-cloud microphysics and drizzle in a moderately polluted environment

Climate is critically affected by aerosols, which alter cloud lifecycles and precipitation distribution through radiative and microphysical effects. In this study, aerosol and cloud property datasets from MODIS (Moderate Resolution Imaging Spectroradiometer), onboard the Aqua satellite, and surface observations, including aerosol concentrations, raindrop size distribution, and meteorological parameters, were used to statistically quantify the effects of aerosols on low-level warm-cloud microphysics and drizzle over northern Taiwan during multiple fall seasons (from 15 October to 30 November of 2005–2017). Our results indicated that northwestern Taiwan, which has several densely populated cities, is dominated by low-level clouds (e.g., warm, thin, and broken clouds) during the fall season. The observed effects of aerosols on warm clouds indicated aerosol indirect effects (i.e., increased aerosol loading caused a decrease in cloud effective radius (CER)), an increase in cloud optical thickness, an increase in cloud fraction, and a decrease in cloud-top temperature under a fixed cloud water path. Quantitatively, aerosol–cloud interactions (ACI=-∂ln⁡CER∂ln⁡α|CWP, changes in CER relative to changes in aerosol amounts) were 0.07 for our research domain and varied between 0.09 and 0.06 in the surrounding remote (i.e., ocean) and polluted (i.e., land) areas, respectively, indicating aerosol indirect effects were stronger in the remote area. From the raindrop size distribution analysis, high aerosol loading resulted in a decreased frequency of drizzle events, redistribution of cloud water to more numerous and smaller droplets, and reduced collision–coalescence rates. However, during light rain (≤1 mm h−1), high aerosol concentrations drove raindrops towards smaller droplet sizes and increased the appearance of drizzle drops. This study used long-term surface and satellite data to determine aerosol variations in northern Taiwan, effects on clouds and precipitation, and observational strategies for future research on aerosol–cloud–precipitation interactions.

Global-scale Aircraft Observations and Simulations of Cirrus Clouds and Aerosol Indirect Effects

<p>Cirrus clouds have widespread coverage over Earth's surface area. Cirrus cloud radiative forcings are directly affected by the microphysical properties of cirrus clouds, including ice water content (IWC), ice crystal number concentration (Nice), and mean diameter (Dice). In this work, in-situ observations obtained from seven flight campaigns funded by the U.S. National Science Foundation are used to examine key factors controlling the formation and evolution of cirrus clouds. These key factors include thermodynamic conditions (i.e., temperature and relative humidity), dynamic conditions (i.e., vertical velocity), and aerosol indirect effects from larger and smaller aerosols (> 500 nm and > 100 nm, respectively). After isolating the effects from thermodynamic and dynamic conditions, we found that when aerosol number concentrations (Na<sub>500</sub> and Na<sub>100</sub>) increase, IWC, Nice and Dice all increase. In particular, IWC and Nice increase significantly when Na is about 3 – 10 times larger than the average Na conditions (Patnaude and Diao, GRL, 2020).</p><p>Simulations of cirrus clouds by a global climate model – the U.S. National Center for Atmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6) are evaluated against in-situ observations (Patnaude, Diao, Liu and Chu, ACP, accepted). Observations show higher Nice in the northern hemisphere (NH) midlatitude than southern hemisphere (SH) midlatitude. CAM6 simulations show “too many” and “too small” ice crystals in most of the regions except NH midlatitude, where simulations show lower Nice than the observations. Weaker aerosol indirect effects on cirrus clouds are also seen in the simulations compared with observations.</p>

Changes in TOA SW Fluxes over Marine Clouds When Estimated via Semi-Physical Angular Distribution Models

Top-of-atmosphere (TOA) shortwave (SW) angular distribution models (ADMs) approximate – per angular direction of an imagined upward hemisphere – the intensity of sunlight scattered back from a specific Earth-atmosphere scene. ADMs are, thus, critical when converting satellite-borne broadband radiometry into estimated radiative fluxes. This paper applies a set of newly developed ADMs with a more refined scene definition and demonstrates tenable changes in estimated fluxes compared to currently operational ADMs. Newly developed ADMs use a semi-physical framework to consider cloud-top effective radius, , and above-cloud water vapor, ACWV, in addition to accounting for surface wind speed and clouds’ phase, fraction, and optical depth. In effect, instantaneous TOA SWfluxes for marine liquid-phase clouds had the largest flux differences (of up to 25 W m−2) for lower solar zenith angles and cloud optical depth greater than 10 due to extremes in or ACWV. In regions where clouds had persistently extreme levels of (here mostly for <7μm and >15μm) or ACWV, instantaneous fluxes estimated from Aqua, Terra, and Meteosat 8 and 9 satellites using the two ADMs differed systematically, resulting in significant deviations in daily mean fluxes (up to ±10 W m−2) and monthly mean fluxes (up to ±5 W m−2). Flux estimates using newly developed, semi-physical ADMs may contribute to a better understanding of solar fluxes over low-level clouds. It remains to be seen whether aerosol indirect effects are impacted by these updates.

Aerosol impacts on warm-cloud microphysics and drizzle in a moderately polluted environment

Climate is critically affected by aerosols, which can alter cloud lifecycles and precipitation distribution through radiative and microphysical effects. In this study, aerosol and cloud properties datasets from MODIS onboard Aqua satellite and surface observations, including aerosol concentrations, raindrop size distribution, and meteorological parameters, were used to statistically quantify the effects of aerosols on low-level warm cloud microphysics and drizzle over northern Taiwan during fall seasons (from October 15 to November 30 of 2005–2017). Results indicated that clouds in northwestern Taiwan, which with active human activity is dominated by low-level clouds (e.g. warm, thin, and broken clouds). The observed effects of aerosols on warm clouds indicated aerosol indirect effects; increasing aerosol loading caused a decrease in cloud effective radius (CER), an increase in cloud optical thickness, an increase in cloud fraction, and a decrease in cloud top temperature under a fixed cloud water path. A quantitative value of aerosol–cloud interactions (ACI = (δ ln⁡ CER)/(δ ln⁡ α), changes in CER depend on changes in aerosols) were calculated to be 0.07 for our research domain. ACI values varied between 0.09 and 0.06 in surrounding clean and heavily polluted areas, respectively, which indicated that aerosol indirect effects were more sensitive in the clean area. Analysis of raindrop size distribution observations during high aerosol loading resulted in a decreased frequency of drizzle events, redistributed cloud water to more numerous and smaller droplets, and reduced collision–coalescence rates. However, in the scenario of light precipitation (&amp;leq; 1 mm h−1), high aerosol concentrations drive raindrops towards smaller droplet sizes and increase the appearance of drizzle drops. This study used long-term surface and satellite data to determine aerosol variations in northern Taiwan, effects on the clouds and precipitations, and applications to observational strategy planning for future research on aerosol–cloud–precipitation interactions.