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DOE OSTI2021

A Bimodal Diagnostic Cloud Fraction Parameterization. Part II: Evaluation and Resolution Sensitivity

A wide range of approaches exists to account for subgrid cloud variability in regional simulations of the atmosphere. This paper addresses the following questions: 1) Is there still benefit in representing subgrid variability of cloud in convection-permitting simulations? 2) What is the sensitivity to the cloud fraction parameterization complexity? 3) Are current cloud fraction parameterizations scale-aware across convection-permitting resolutions? These questions are addressed for regional simulations of a 6-week observation campaign in the U.S. southern Great Plains. Particular attention is given to a new diagnostic cloud fraction scheme with a bimodal subgrid saturation-departure PDF, described in Part I. The model evaluation is performed using ground-based remote sensing synergies, satellite-based retrievals, and surface observations. It is shown that not using a cloud fraction parameterization results in underestimated cloud frequency and water content, even for stratocumulus. The use of a cloud fraction parameterization does not guarantee improved cloud property simulations, however. Diagnostic and prognostic cloud schemes with a symmetric subgrid saturation-departure PDF underestimate cloud fraction and cloud optical thickness, and hence overestimate surface shortwave radiation. These schemes require empirical bias-correction techniques to improve the cloud cover. The new cloud fraction parameterization, introduced in Part I, improves cloud cover, liquid water content, cloud-base height, optical thickness, and surface radiation compared to schemes reliant on a symmetric PDF. Furthermore, cloud parameterizations using turbulence-based, rather than prescribed constant subgrid variances, are shown to be more scale-aware across convection-permitting resolutions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Theory of In-Cloud Activation of Aerosols and Microphysical Quasi-Equilibrium in a Deep Updraft

The microphysical quasi-equilibrium in an ascending adiabatic parcel is elucidated by an analytical theory in 0D with drastic simplifications. The theory predicts how in-cloud activation is most likely to be triggered by the onset of precipitation during sufficient ascent, with the ascent only needing to approach almost twice the cloud-base updraft speed aloft. The precipitation and cloud condensate mass fields are coupled in a closed system in a simplified version of the model. The initial state of no precipitation is unstable with respect to a perturbation. In the 2D phase space of both mass fields, there is a neutral line. Unstable growth of precipitation mass drives the system to cross the line into a regime of stability. An attractor is then approached consisting of precipitation mass balanced by accretion of cloud mass and fallout. The cloud-particle number concentration also approaches a stable equilibrium governed by the balance between in-cloud activation aloft from the inexorably increasing supersaturation during vertical acceleration and accretion of cloud droplets by precipitation. Dimensionless numbers characterizing the microphysical equilibria and their stability are derived mathematically, including a condensation–precipitation efficiency and an in-cloud activation efficiency. The theory explains common observations of the orders of magnitude of liquid water content in convective and stratiform clouds. Finally, sensitivity tests of the numerically integrated theoretical equations are documented with respect to variations in cloud condensation nucleus (CCN) aerosols and updraft speed. In conclusion, it is shown that this theory of in-cloud activation, with an increasing supersaturation during ascent, applies to both ice-only and liquid-only cloud.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Quasi‐Steady State Supersaturation: Do High Values Derived From ESCAPE Represent Real High Supersaturations and the Potential for Condensational Invigoration?

Deep convective clouds were intensively sampled during the Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) with coordinated flights of the NRC Convair-580 and SPEC Learjet. A total of 219 updraft core segments were sampled over coastal Texas and Louisiana under diverse meteorological conditions. Median updraft properties included widths of ∼1 km, velocities of 4.8 m s −1 , droplet number concentrations of ∼400 cm −3 , and liquid water contents of 0.9 g m −3 . The limitations of using the quasi-steady state approximation to derive supersaturations were explored. Supersaturation (S QSS ) estimated from in situ observations under a quasi-steady state assumption averaged 0.4% but occasionally exceeded 2%, with values >1% (high supersaturations) identified as statistical outliers. Two case studies illustrated the conditions linked to high supersaturations. In a storm over the Gulf, median core S QSS reached 2.46% in the developing stage compared to 2.17% in the mature stage under similar thermodynamic conditions. In a storm over coastal Louisiana, S QSS peaked near 11% within a 13.7-m s −1 updraft, accompanied by predominantly supercooled liquid droplets at −13°C and exceptionally low diameter concentrations of 0.29 mm cm −3 . Bootstrap analysis of all sampled cores showed that high supersaturations are most probable in cold and mixed-phase regimes with moderate to strong updrafts and are strongly influenced by vertical velocity and droplet number concentrations. In conclusion, while extreme supersaturations (∼10%) were rare, their occurrence underscores the need for targeted multiplatform observations to resolve their spatiotemporal variability and assess their potential role in deep convective invigoration.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Bounding Global Aerosol Radiative Forcing of Climate Change

Abstract Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol‐radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol‐driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed‐phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of ‐1.6 to ‐0.6 W m −2 , or ‐2.0 to ‐0.4 W m −2 with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial‐era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Modeling Novel Aqueous Particle and Cloud Chemistry Processes of Biomass Burning Phenols and Their Potential to Form Secondary Organic Aerosols

Phenols emitted from biomass burning contribute significantly to secondary organic aerosol (SOA) formation through the partitioning of semivolatile products formed from gas-phase chemistry and multiphase chemistry in aerosol liquid water and clouds. The aqueous-phase SOA (aqSOA) formed via hydroxyl radical (˙OH), singlet molecular oxygen ( 1 O 2 *), and triplet excited states of organic compounds ( 3 C*), which oxidize dissolved phenols in the aqueous phase, might play a significant role in the evolution of organic aerosol (OA). However, a quantitative and predictive understanding of aqSOA has been challenging. Here, we develop a stand-alone box model to investigate the formation of SOA from gas-phase ˙OH chemistry and aqSOA formed by the dissolution of phenols followed by their aqueous-phase reactions with ˙OH, 1 O 2 *, and 3 C* in cloud droplets and aerosol liquid water. Here, we investigate four phenolic compounds, i.e., phenol, guaiacol, syringol, and guaiacyl acetone (GA), which represent some of the key potential sources of aqSOA from biomass burning in clouds. For the same initial precursor organic gas that dissolves in aerosol/cloud liquid water and subsequently reacts with aqueous phase oxidants, we predict that the aqSOA formation potential (defined as aqSOA formed per unit dissolved organic gas concentration) of these phenols is higher than that of isoprene-epoxydiol (IEPOX), a well-known aqSOA precursor. Cloud droplets can dissolve a broader range of soluble phenols compared to aqueous aerosols, since the liquid water contents of aerosols are orders of magnitude smaller than cloud droplets. Further, our simulations suggest that highly soluble and reactive multifunctional phenols like GA would predominantly undergo cloud chemistry within cloud layers, while gas-phase chemistry is likely to be more important for less soluble phenols. But in the absence of clouds, the condensation of low-volatility products from gas-phase oxidation followed by their reversible partitioning to organic aerosols dominates SOA formation, while the SOA formed through aqueous aerosol chemistry increases with relative humidity (RH), approaching 40% of the sum of gas and aqueous aerosol chemistry at 95% RH for GA. Our model developments of biomass-burning phenols and their aqueous chemistry can be readily implemented in regional and global atmospheric chemistry models to investigate the aqueous aerosol and cloud chemistry of biomass-burning organic gases in the atmosphere.

09 BIOMASS FUELS↗
DOE OSTI2024

Deriving cloud droplet number concentration from surface-based remote sensors with an emphasis on lidar measurements

Abstract. Given the importance of constraining cloud droplet number concentrations (Nd) in low-level clouds, we explore two methods for retrieving Nd from surface-based remote sensing that emphasize the information content in lidar measurements. Because Nd is the zeroth moment of the droplet size distribution (DSD), and all remote sensing approaches respond to DSD moments that are at least 2 orders of magnitude greater than the zeroth moment, deriving Nd from remote sensing measurements has significant uncertainty. At minimum, such algorithms require the extrapolation of information from two other measurements that respond to different moments of the DSD. Lidar, for instance, is sensitive to the second moment (cross-sectional area) of the DSD, while other measures from microwave sensors respond to higher-order moments. We develop methods using a simple lidar forward model that demonstrates that the depth to the maximum in lidar-attenuated backscatter (Rmax⁡) is strongly sensitive to Nd when some measure of the liquid water content vertical profile is given or assumed. Knowledge of Rmax⁡ to within 5 m can constrain Nd to within several tens of percent. However, operational lidar networks provide vertical resolutions of > 15 m, making a direct calculation of Nd from Rmax⁡ very uncertain. Therefore, we develop a Bayesian optimal estimation algorithm that brings additional information to the inversion such as lidar-derived extinction and radar reflectivity near the cloud top. This statistical approach provides reasonable characterizations of Nd and effective radius (re) to within approximately a factor of 2 and 30 %, respectively. By comparing surface-derived cloud properties with MODIS satellite and aircraft data collected during the MARCUS and CAPRICORN II campaigns, we demonstrate the utility of the methodology.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Insights into the relation between vertical cloud structure and dynamics of three polar lows: Observations from COMBLE

The vertical structure of three polar lows is described using profiling radar, lidar, and passive remote sensors deployed at a coastal site in northern Norway. The data were collected as part of the Cold-air Outbreaks in the Marine Boundary Layer Experiment (COMBLE). These data are examined in the context of satellite imagery, operational weather radar reflectivity imagery, and output from the AROME-Arctic model. A comparison to satellite images shows that AROME-Arctic captured the polar lows well. All three polar lows form in marine cold-air outbreaks and are surrounded by open-cellular convection typical of such outbreaks. Two of the lows form in a forward shear environment, and one under reverse shear. Initially, the three polar lows are comma-shaped; two of them transition to be more spirali-form at their mature stage and have mostly cloud-free warm cores. The warm cores are the result of a warm-seclusion process. All three lows have stratiform precipitation bands, marked by little cloud liquid water, and rather high surface precipitation rate. The vertical drafts and turbulence in these stratiform clouds are generally weak. In conclusion, all three lows also have convective clouds, which have stronger vertical drafts, stronger turbulence, and pockets of high liquid water content.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Relationships between Cloud Droplet Spectral Relative Dispersion and Entrainment Rate and Their Impacting Factors

Cloud microphysical properties are significantly affected by entrainment and mixing processes. However, it is unclear how the entrainment rate affects the relative dispersion of cloud droplet size distribution. Previously, the relationship between relative dispersion and entrainment rate was found to be positive or negative. To reconcile the contrasting relationships, the Explicit Mixing Parcel Model is used to determine the underlying mechanisms. When evaporation is dominated by small droplets, and the entrained environmental air is further saturated during mixing, the relationship is negative. However, when the evaporation of big droplets is dominant, the relationship is positive. Whether or not the cloud condensation nuclei are considered in the entrained environmental air is a key factor as condensation on the entrained condensation nuclei is the main source of small droplets. However, if cloud condensation nuclei are not entrained, the relationship is positive. If cloud condensation nuclei are entrained, the relationship is dependent on many other factors. High vertical velocity, relative humidity of environmental air, liquid water content, and low droplet number concentration are more likely to cause the negative relationship since new saturation is easier to achieve by evaporation of small droplets. Further, the signs of the relationship are not strongly affected by the turbulence dissipation rate, but the higher dissipation rate causes the positive relationship more significant for a larger entrainment rate. A conceptual model is proposed to reconcile the contrasting relationships. This work enhances the understanding of relative dispersion and lays a foundation for the quantification of entrainment-mixing mechanisms.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Coastal-Fog Microphysics Using In-Situ Observations and GOES-R Retrievals

Here, the objective of this work is to evaluate GOES-R based fog conditions occurred during the C-FOG (Toward Improving Coastal Fog Prediction) field campaign. C-FOG is designed to advance understanding of fog formation, development, and dissipation over coastal environments to improve its predictability. The project took place along coastlines and open water environments of Eastern Canada (Nova Scotia, NS and the Island of Newfoundland, NL) during August-October of 2018 where environmental conditions play an important role for late season’s fog formation. During the C-FOG field campaign, instruments were located at the Ferryland Supersite, NL, with 2 main sites, and five satellite sites, as well as on the Research Vessel (R/V) Hugh R. Sharp. Key measurement instruments included a Gondola carrying a CDP (cloud droplet probe) and a BCP (backscatter cloud probe) was used for measuring droplet spectra from 1-75 µm on the R/V. A LPM (laser precipitation monitor) with 100 µm-1 cm size range and an OPC (optical particle counter) with 0.3-17 µm at 16 spectral channels provided information for fog and drizzle discrimination. Remote sensing platforms (e.g. profiling microwave radiometer, PMWR), Ceilometer, Lidar), meteorological towers, tethered balloons, and GOES-R products (e.g. fog coverage and droplet size and liquid water path) were used to evaluate fog over horizontal and vertical dimensions. Results suggest that effective radius, phase, liquid water path, and liquid water content values obtained from GOES-R and PMWR were comparable to ground based in-situ observations. It is concluded that integration of observations and nowcasting products may help improve short term local fog predictions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Analysis of Coastal Fog from a Ship During the C-FOG Campaign

This work presents ship-based measurements of fog off St John’s Newfoundland on 13 September 2018 during the Coastal Fog (C-FOG) field campaign. The measurements included cloud-particle spectra, cloud-base height and aerosol backscatter, radiation, turbulence, visibility, and sea surface temperature. Radiosonde soundings were made at intervals less than 2 hours. Fog occurred in two episodes under the center of eastward-moving synoptic low-pressure system. The boundary layer structure during the first fog episode consisted of 3 layers, separated by 2 saturated air temperature inversions and capped by a subsidence inversion. The lowest layer was fog and the upper layers were cloud. The second fog episode consisted of one well-mixed fog layer capped by a subsidence inversion. Low wind speeds and stable stratification maintained low surface-layer turbulence during fog. Droplet size distributions had typical bimodal distributions. The visibility correlated with the droplet number concentration and liquid water content. The air temperature was higher than the sea surface temperature for the first 30 minutes of the first fog episode but was colder than the sea for the remainder of all fog. The sensible heat flux was upward, from sea to air, for the first 62 % of the first fog episode and then reversed to downward, from air to sea, for the remainder of the first fog episode and the second fog episode. Here, the counter-gradient heat fluxes observed (i.e., opposite to what is expected from the instantaneous air-sea temperature difference) appear to be related to turbulence, entrainment and stratification in the fog layer that overwhelmed the influence of air-sea temperature difference. While the synoptic-scale dynamics preconditioned the area for fog formation, the final step of fog appearance in this case was nuanced by stratification-turbulence interactions, local advective processes and microphysical environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Depth-specific distribution of bacterial MAGs in permafrost active layer in Ny Ålesund, Svalbard (79°N)

Arctic soil microbial communities may shift with increasing temperatures and water availability from climate change. We examined temperature and volumetric liquid water content (VWC) in the upper 80 cm of permafrost-affected soil over 2 years (2018–2019) at the Bayelva monitoring station, Ny Ålesund, Svalbard. We show VWC increases with depth, whereas in situ temperature is more stable vertically, ranging from -5°C to 5°C seasonally. Prokaryotic metagenome-assembled genomes (MAGs) were obtained at 2–4 cm vertical resolution collected while frozen in April 2018 and at 10 cm vertical resolution collected while thawed in September 2019. The most abundant MAGs were Acidobacteriota, Actinomycetota, and Chloroflexota. Actinomycetota and Chloroflexota increase with depth, while Acidobacteriota classes Thermoanaerobaculia Gp7-AA8, Blastocatellia UBA7656, and Vicinamibacteria Vicinamibacterales are found above 6 cm, below 6 cm, and below 20cm, respectively. All MAGs have diverse carbon-degrading genes, and Actinomycetota and Chloroflexota have autotrophic genes. Further, genes encoding β -glucosidase, N-acetyl-β-D-glucosaminidase, and xylosidase increase with depth, indicating a greater potential for organic matter degradation with higher VWC. Acidobacteriota dominate the top 6 cm with their classes segregating by depth, whereas Actinomycetota and Chloroflexota dominate below ~6 cm. This suggests that Acidobacteriota classes adapt to lower VWC at the surface, while Actinomycetota and Chloroflexota persist below 6cm with higher VWC. This indicates that VWC may be as important as temperature in microbial climate change responses in Arctic mineral soils. Here we describe MAG-based Seqcode type species in the Acidobacteriota, Onstottus arcticum, Onstottus frigus, and Gilichinskyi gelida and in the Actinobacteriota, Mayfieldus profundus.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Analytical advances to study the air – water interfacial chemistry in the atmosphere

Formation of aqueous secondary organic aerosol (aqSOA) at the air – liquid interface recently has attracted a lot of attention in atmospheric chemistry. The discrepancies in mass distributions, aerosol oxidative capacity, liquid water content, hygroscopic growth of aerosols, and formation of clouds and fogs suggest that interfacial chemistry play a more important role than previously deemed. However, detailed mechanisms at the air–water interface remain unclear owing to the lack of comprehensive understanding that underpins complicated interfacial phenomena, which are not easily measurable from field campaigns, laboratory measurements, or computational simulations. Here, this review highlights relevant and recent technical advancement employed to study aqSOA encompassing spectroscopy and mass spectrometry. The current knowledge on the aqSOA processes is digested with an emphasis on recent research of interfacial aqSOA formation including laboratory studies and model simulations. Finally, future directions of the interfacial chemistry are recommended for field and laboratory studies as well as theoretical efforts to resolve interfacial challenges in atmospheric chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Simulating Droplet-Resolved Haze and Cloud Chemistry Forming Secondary Organic Aerosols in Turbulent Conditions within Laboratory and Cloud Parcels

Most of our existing knowledge of cloud chemistry in regards to forming secondary organic aerosols (SOA) is based on measurements in bulk aqueous solutions. However, SOA reaction kinetics derived from bulk solution measurements might differ from the kinetics in actual cloud droplets, since turbulent mixing and ionic strengths, and ratio of surface area to volume in individual cloud droplets might vary substantially from bulk solutions in the real atmosphere. Three-dimensional models at various scales have been used to simulate aqueous chemistry. However, most of these models do not resolve turbulence down to the smallest length scales of 1 mm and do not simulate cloud chemistry in individual cloud droplets due to large computational costs. Here we incorporate the formation of isoprene epoxydiol SOA (IEPOX-SOA) in individual droplets within a one-dimensional explicit mixing parcel model (EMPM-Chem). We apply EMPM-Chem to simulate turbulence and droplet-resolved IEPOX-SOA formation using a configuration based on the Michigan Tech Pi chamber. We find that the dissolution of IEPOX gases is weighted more towards larger cloud droplets due to their large liquid water content (compared to smaller droplets), while the conversion of dissolved IEPOX to IEPOX-SOA is much greater within smaller deliquesced haze particles due to their higher acidity and ionic strengths compared to cloud droplets. We also find that as droplet residence times increase in the chamber, e.g., due to increasing ammonium bisulfate seed aerosol injection rates and/or increasing heights of the chamber, formation of IEPOX-SOA increases substantially. Thus, our EMPM-Chem model could be used to design future cloud chambers to maximize SOA production from cloud chemistry. We also apply the EMPM-Chem model to simulate how IEPOX-SOA formation evolves in individual cloud droplets within rising cloudy parcels in the atmosphere. We find that as subsaturated air is entrained into and turbulently mixed with the cloud parcel, evaporation causes a reduction in droplet sizes, which leads to corresponding increases in per droplet ionic strength and acidity. Increased droplet acidity in turn greatly accelerates the kinetics of IEPOX-SOA formation. In conclusion, our results provide key insights into single-cloud-droplet chemistry, suggesting that entrainment mixing may be an important process that increases SOA formation in the real atmosphere.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The Role of Ice Splintering on Microphysics of Deep Convective Clouds Forming Under Different Aerosol Conditions: Simulations Using the Model With Spectral Bin Microphysics

Observations during the Ice in Clouds Experiment-Tropical (ICE-T) field experiment show that the ice particles concentration in a developing deep convective clouds at the level of T = -15 °C reached about 500 L -1 , that is, many orders higher than that of ice-nucleating particle. To simulate microphysics of these clouds, the 2-D Hebrew University Cloud model (HUCM) with spectral bin microphysics was used in which two main types of ice multiplication mechanisms were included in addition to the Hallet-Mossop mechanism. In the first ice multiplication mechanism ice splinters form by drop freezing and drop-ice collisions. Ice multiplication of this type dominates during developing stage of cloud evolution, when liquid water content is significant. At later stage when clouds become nearly glaciated, ice crystals are produced largely by ice splintering during ice-ice collisions (the second ice multiplication mechanism). Simulations show that droplet size distributions, as well as size distributions of ice particles, agree well with the measurements during ICE-T. Simulations with different cloud condensation nuclei concentrations show the existence of the “optimum” cloud condensation nuclei concentration (or droplet concentration), at which concentration of ice splinters reaches maximum. In these simulations ice nucleation caused by the direct formation of ice crystals upon ice-nucleating particles, as well as the Hallett-Mossop process, has a negligible contribution to the ice crystal concentration.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Statistical Characteristics of Raindrop Size Distributions and Parameters in Central China during the Meiyu Seasons

The rain parameters measured by the laser OTT Parsivel raindrop disdrometer (Parsivel), the two-dimensional video disdrometer (2DVD) and DZZ5 tipping-bucket rain gauge (RG) during the Integrative Monsoon Frontal Rainfall Experiment (IMFRE) in summer 2018 are compared. The total rain amounts observed by Parsivel, 2DVD, and RG during IMFRE are 178.07 mm, 176.76 mm and 182.5 mm, while their total rainy hours are 113, 113 and 90. The mean Dm (mass-weighted mean diameter) and liquid water content values derived from Parsivel and 2DVD are 0.9 mm and 1.02 mm, and 0.247 g m-3 and 0.223 g m-3, respectively, and Parsivel is more sensitive to small raindrops (< 1 mm) than 2DVD. The raindrop spectra measured by Parsivel and 2DVD have excellent agreement for both convective rain (CR) and stratiform rain (SR) within a range of Dm from 1 to 3.5 mm. The rain samples from six Parsivel sites over the middle reaches of the Yangtze River during the 2016–2018 meiyu seasons have been collected and processed. The frequency occurrences for rain rates (RR) < 5 and > 10 mm h-1 are 83.9% and 7.4%, respectively, but they contribute 30.5% and 52.1 % of the total accumulated rainfall. Comparing the results with those over the lower reaches, the RR and total accumulated rainfall over the middle reaches are greater, especially for heavy rainfall. The rain drop size distributions (DSDs) in this study are wider and have higher number concentration than those from the lower reaches.

Raindrop size distribution, Meiyu front, disdromet↗
DOE OSTI2021

Consideration of Initial Cloud Droplet Size Distribution Shapes in Quantifying Different Entrainment-Mixing Mechanisms

Entrainment-mixing process significantly affects cloud micro/macrophysics and the evaluation of aerosol indirect effects. However, it remains an open question as to how to quantify entrainment-mixing mechanism for broad cloud droplet size distributions (CDSDs). Here, CDSDs with different spectral widths are used to initialize the Explicit Mixing Parcel Model to address this problem, and microphysical properties are compared for different CDSD widths. For relatively broad CDSDs, as the number concentration and liquid water content decrease, the volume-mean radius and mean radius increase, which is opposite to the scenario for relatively narrow CDSDs and the homogeneous/inhomogeneous conceptual model. For the relatively broad CDSDs, such relationships could be mistaken as inhomogeneous mixing with subsequent ascent in analysis of the conventional microphysical mixing diagram. This then causes traditional homogenous mixing degrees to be unrealistically negative and not applicable for relatively broad CDSDs. New measures are introduced to explicitly account for the effect of CDSD spectral shapes on quantifying entrainment-mixing mechanism. The new measures yield reasonable ranges of values that conform to the dynamical measures such as the Damköhler and transitional scale numbers, and their temporal variation can be explained physically. This study extends the measures of homogeneous mixing degrees from narrow to broad CDSDs, and sheds new light on the consideration of CDSD shapes in parameterizations of entrainment-mixing mechanism.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Observed Relationships Between Cloud Droplet Effective Radius and Biogenic Gas Concentrations in Summertime Marine Stratocumulus Over the Eastern North Atlantic

Abstract Biogenic gases are a prominent component of the summertime marine boundary layer (MBL) over the Eastern North Atlantic. One of these gases, dimethyl sulfide (DMS), can produce sulfate cloud condensation nuclei (CCN) that, in theory, can brighten clouds through photolysis, and produces a reaction product, methane sulfonic acid (MSA). It is also possible that DMS can interact with sea‐salt or other marine aerosols changing their CCN activation spectrum, which could also modify cloud microphysical structure. Data collected aboard the G1 aircraft during the Aerosol Cloud Experiment Eastern North Atlantic (ACE‐ENA) in well‐mixed and decoupled marine boundary layers (MBLs) were used to examine relationships between the cloud droplet effective radii, , and the concentrations of DMS and MSA in constant cloud liquid water content (LWC) bins. A weak but statistically significant negative correlation was observed between CCN concentration and in most LWC bins, regardless of the source of the CCN, while a weak but statistically significant positive correlation between and DMS was observed. No correlation between the cloud droplet number concentration and DMS was found. The presence of MSA indicated that DMS‐to‐sulfate photolysis was likely occurring, but data sparsity prevented a statistically significant conclusion regarding the relationship between MSA and . Data sparsity in decoupled conditions also prevented statistically significant conclusions. To properly address biogenic gas impacts on cloud microphysics, it is recommended that aircraft data be supplemented by long‐term biogenic gas measurements at the surface in marine locations with appropriate remote and in‐situ cloud sensing capabilities, and the analysis limited to well‐mixed MBL's.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

The Relation of Environmental Conditions With Charge Structure in Central Argentina Thunderstorms

In this study we explored the environmental conditions hypothesized to induce a dominant charge structure in thunderstorms in the province of Cordoba, Argentina, during the RELAMPAGO-CACTI (Remote sensing of Electrification, Lightning, And Mesoscale/microscale Processes with Adaptive Ground Observations-Clouds, Aerosols, Complex Terrain Interactions) field campaigns. Hypothesized environmental conditions are thought to be related to small warm cloud residence time and warm rain growth suppression, which lead to high cloud liquid water contents in the mixed-phase zone, contributing to positive charging of graupel and anomalous charge structure storms. Data from radiosondes, a cloud condensation nuclei (CCN) ground-based instrument and reanalysis were used to characterize the proximity inflow air of storms with anomalous and normal charge structures. Consistent with the initial hypothesis, anomalous storms had small warm cloud depth caused by dry low-level humidity and low 0°C height. Anomalous storms were associated with lower CCN concentrations than normal storms, an opposite result to the initial expectation. High CAPE is not an important condition for the development of anomalous storms in Argentina, as no clear pattern could be found among the different parameters calculated for updraft proxy that would be consistent with the initial hypothesis.

54 ENVIRONMENTAL SCIENCES↗