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486 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings

Atmospheric marine aerosol particles impact Earth's albedo and climate. These particles can be primary or secondary and come from a variety of sources, including sea salt, dissolved organic matter, volatile organic compounds, and sulfur-containing compounds. Dimethylsulfide (DMS) marine emissions contribute greatly to the global biogenic sulfur budget, and its oxidation products can contribute to aerosol mass, specifically as sulfuric acid and methanesulfonic acid (MSA). Further, sulfuric acid is a known nucleating compound, and MSA may be able to participate in nucleation when bases are available. As DMS emissions, and thus MSA and sulfuric acid from DMS oxidation, may have changed since pre-industrial times and may change in a warming climate, it is important to characterize and constrain the climate impacts of both species. Currently, global models that simulate aerosol size distributions include contributions of sulfate and sulfuric acid from DMS oxidation, but to our knowledge, global models typically neglect the impact of MSA on size distributions. In this study, we use the GEOS-Chem-TOMAS (GC-TOMAS) global aerosol microphysics model to determine the impact on aerosol size distributions and subsequent aerosol radiative effects from including MSA in the size-resolved portion of the model. The effective equilibrium vapor pressure of MSA is currently uncertain, and we use the Extended Aerosol Inorganics Model (E-AIM) to build a parameterization for GC-TOMAS of MSA's effective volatility as a function of temperature, relative humidity, and available gas-phase bases, allowing MSA to condense as an ideally nonvolatile or semivolatile species or too volatile to condense. We also present two limiting cases for MSA's volatility, assuming that MSA is always ideally nonvolatile (irreversible condensation) or that MSA is always ideally semivolatile (quasi-equilibrium condensation but still irreversible condensation). We further present simulations in which MSA participates in binary and ternary nucleation with the same efficacy as sulfuric acid whenever MSA is treated as ideally nonvolatile. When using the volatility parameterization described above (both with and without nucleation), including MSA in the model changes the global annual averages at 900 hPa of submicron aerosol mass by 1.2 %, N3 (number concentration of particles greater than 3 nm in diameter) by -3.9 % (non-nucleating) or 112.5 % (nucleating), N80 by 0.8 % (non-nucleating) or 2.1 % (nucleating), the cloud-albedo aerosol indirect effect (AIE) by -8.6 mW m -2 (non-nucleating) or -26 mW m -2 (nucleating), and the direct radiative effect (DRE) by -15 mW m -2 (non-nucleating) or -14  mW m -2 (nucleating). The sulfate and sulfuric acid from DMS oxidation produces 4–6 times more submicron mass than MSA does, leading to an ~10 times stronger cooling effect in the DRE. But the changes in N80 are comparable between the contributions from MSA and from DMS-derived sulfate/sulfuric acid, leading to comparable changes in the cloud-albedo AIE. Model–measurement comparisons with the Heintzenberg et al. (2000) dataset over the Southern Ocean indicate that the default model has a missing source or sources of ultrafine particles: the cases in which MSA participates in nucleation (thus increasing ultrafine number) most closely match the Heintzenberg distributions, but we cannot conclude nucleation from MSA is the correct reason for improvement. Model–measurement comparisons with particle-phase MSA observed with a customized Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) from the ATom campaign show that cases with the MSA volatility parameterizations (both with and without nucleation) tend to fit the measurements the best (as this is the first use of MSA measurements from ATom, we provide a detailed description of these measurements and their calibration). However, no one model sensitivity case shows the best model–measurement agreement for both Heintzenberg and the ATom campaigns. As there are uncertainties in both MSA's behavior (nucleation and condensation) and the DMS emissions inventory, further studies on both fronts are needed to better constrain MSA's past, current, and future impacts upon the global aerosol size distribution and radiative forcing.

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

Summer Aerosol and Trace Gas Observations in Houston, Texas Using an Adaptable Mobile Facility

An aerosol container featuring a shared inlet system was deployed to Houston, Texas in July 2022, enabling direct, high-time-resolution in situ measurements of aerosols and trace gases. The internal rack system and floorplan was designed for adaptable modularity to elucidate aerosol physicochemical processes at fine scales. The design allowed for the deployment of a core instrument suite and additional customized research grade instruments. A heterogeneous mixture of aerosols was observed during three regimes: (1) intermittent black carbon (BC) and diurnal variations in aerosol chemical composition, (2) observed particle growth associated with SO 2 , (3) transported supermicron dust. The high variability of observed particles and gases in high time resolution indicated a complex urban area with multiple local and regional sources and processes. Particle growth rates of 7–16 nm/hr were observed for submicron particles during periods when SO 2 was >0.5 ppbv. Two periods of multi-day long-range transport events of dust from the African Sahara were observed in the supermicron and submicron particle modes with total mass concentrations up to 30 μg m −3 . Aerosol scattering angstrom exponents and extinction coefficients (B ext ) increased with humidity as a function of particle composition. The measurements demonstrate collaborative capabilities that can be used to increase observations of aerosol processing, microphysical and optical properties, internal mixing state, and supermicron aerosol that are not parameterized or missing in global Earth energy system models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Cloud vertical distribution from combined surface and space radar–lidar observations at two Arctic atmospheric observatories

Abstract. Detailed and accurate vertical distributions of cloud properties (such as cloud fraction, cloud phase, and cloud water content) and their changes are essential to accurately calculate the surface radiative flux and to depict the mean climate state. Surface and space-based active sensors including radar and lidar are ideal to provide this information because of their superior capability to detect clouds and retrieve cloud microphysical properties. In this study, we compare the annual cycles of cloud property vertical distributions from space-based active sensors and surface-based active sensors at two Arctic atmospheric observatories, Barrow and Eureka. Based on the comparisons, we identify the sensors' respective strengths and limitations, and develop a blended cloud property vertical distribution by combining both sets of observations. Results show that surface-based observations offer a more complete cloud property vertical distribution from the surface up to 11 km above mean sea level (a.m.s.l.) with limitations in the middle and high altitudes; the annual mean total cloud fraction from space-based observations shows 25–40 % fewer clouds below 0.5 km than from surface-based observations, and space-based observations also show much fewer ice clouds and mixed-phase clouds, and slightly more liquid clouds, from the surface to 1 km. In general, space-based observations show comparable cloud fractions between 1 and 2 km a.m.s.l., and larger cloud fractions above 2 km a.m.s.l. than from surface-based observations. A blended product combines the strengths of both products to provide a more reliable annual cycle of cloud property vertical distributions from the surface to 11 km a.m.s.l. This information can be valuable for deriving an accurate surface radiative budget in the Arctic and for cloud parameterization evaluation in weather and climate models. Cloud annual cycles show similar evolutions in total cloud fraction and ice cloud fraction, and lower liquid-containing cloud fraction at Eureka than at Barrow; the differences can be attributed to the generally colder and drier conditions at Eureka relative to Barrow.

58 GEOSCIENCES↗
DOE OSTI2024

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Aerosol Chemical Speciation Monitor (ACSM) Composition-Dependent Collection Efficiency (CDCE) Value-Added Product Report

Aerosol particles influence the Earth’s radiation balance directly by absorbing and scattering light and indirectly by influencing cloud formation, properties, and lifetimes. Measurements of aerosol particle optical properties, mass loading, size distributions, microphysical properties, cloud formation properties, and chemical composition are important for understanding the aerosol life cycle and for validating earth system models that predict these quantities. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Aerosol Observing System (AOS) is a highly instrumented platform that measures many of these aerosol properties in situ. The Aerodyne aerosol chemical speciation monitor (ACSM) is a baseline instrument deployed in the AOS. The ACSM provides a quantitative measurement of aerosol particle chemical composition for non-refractory (operationally defined as components that evaporate on the 600ºC vaporizer) aerosol components in real time. Standard output is the mass concentration of particulate organics, nitrate, sulfate, chloride, and ammonium. One well-known limitation to the accuracy of the ACSM data is in evaluating the fraction of the ambient aerosol particles that are detected by the instrument. This quantity is referred to as the collection efficiency (CE) and is often less than unity. This is attributed to particles rebounding after impaction onto the heated vaporizer rather than being trapped, volatilized rapidly, and detected. Other factors, such as divergence of the aerosol particle beam, may also impact CE, but the particle rebound effect is the dominant factor. Scientists will sometimes assume CE = 0.5 (i.e., one half of sampled particles are detected) for ambient particles collected during field missions. However, parameterizations have been developed that express CE as a function of the measured chemical composition, referred to as the composition-dependent collection efficiency (CDCE). The physical explanation for a CDCE, supported by laboratory studies, is that rebound from the vaporizer is a function of the particle phase, with liquid-like particles “sticking” to the vaporizer and solid-like or crystalline particles “bouncing” from the vaporizer. Thus, particles with compositions are liquids-like under the measurement conditions (e.g., certain organics, acidic particles, particles enriched in nitrate) have CE close to unity while crystalline or solid particles (e.g., deliquesced ammonium sulfate) have lower CE. This value-added product (VAP) implements the procedure described by Middlebrook et al. (2012) to correct the ACSM data for the composition-dependent collection efficiency. Applying this parameterization improves the accuracy of the ACSM data and brings them into better agreement with other co-located aerosol measurements.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Variability in Ice Nucleating Particles Across Greater Houston Texas

The concentration and cloud-forming potential of a region's ice nucleating particle (INP) population have uncertain impacts on deep convective clouds. Specifically, ice nucleating particles (INPs) may affect various cloud properties related to the formation, lifetime, and precipitation of deep convective clouds. As part of the U.S. Department of Energy's TRacking Aerosol and Convection interaction ExpeRiment (TRACER) campaign, researchers from Texas A&M University deployed three Davis Rotating-drum Universal-size-cut Monitoring (DRUM) samplers throughout Greater Houston, Texas from June through September 2022. Ambient particles, collected at the surface with the DRUM samplers in four aerodynamic diameter size ranges (>3, 3–1.2, 1.2–0.34, and 0.34–0.15 μm), were analyzed in offline cold-stage ice nucleation experiments. The INP population in Greater Houston is complex, varying by site and day, but can be generalized by a weak to moderately efficient mode of INPs at −24°C and an efficient mode at −15°C. Analysis reveals that supermicron particles are largely responsible for ice nucleation warmer than −20°C across the region while submicron particles dominate at temperatures colder than −20°C. Additionally, significant spatial diversity in the INP population was observed, with differences in mean nucleation temperature between sites for nearly every size cut. Although INP concentrations were typically ∼0.08 L −1 at −20°C throughout the campaign, a notable region-wide increase in INP concentration for particles freezing at temperatures warmer than −20°C occurred from mid-August to mid-September. This comprehensive characterization of Greater Houston's INP population, including spatial, temporal, and particle size variations, can help constrain ice microphysics parameterizations in weather and climate models.

Thompson, Seth A. [Texas A & M Univ., College Stat↗
DOE OSTI2025

Weak influence of anthropogenic emissions on aerosol, cloud, and rain in the wet season of the Amazon rainforest

Anthropogenic emissions have been shown to affect new particle formation, aerosol concentrations, and clouds. Such effects vary with region, environmental conditions, and cloud types. In the wet season of Amazonia, anthropogenic emissions emitted from Manaus, Brazil, can significantly increase the cloud condensation nuclei (CCN) concentrations compared to the background of mainly natural aerosols. However, the regional response of cloud and rain to anthropogenic emissions in Amazonia remains very uncertain. Here, we aim to quantify how aerosol concentration, cloud, and rain respond to changes in anthropogenic emissions through parameterized new particle formation and primary aerosol emission in the Manaus region and to understand the underlying mechanisms. We ran the atmosphere-only configuration of the HadGEM3 climate model with a nested regional domain that covers most of the rainforest region (720 km by 1200 km with 3 km resolution) under scaled regional emissions. The 7 d simulations show that, in the areas that are affected by anthropogenic emissions, when aerosol and precursor gas emissions are doubled from the baseline emission inventories, aerosol number concentrations increase by 13 %. The nucleation rate that involves sulfuric acid and biogenic compounds generally increases with pollution levels. However, nucleation is suppressed very close to the pollution source, resulting in lower nucleation and soluble Aitken mode aerosol number concentrations. We also found that doubling the anthropogenic emission can increase the cloud droplet number concentrations ( N d ) by 9 %, but cloud water and rain mass mixing ratios do not change significantly. Even very strong reductions in aerosol number concentrations by a factor of 4, which is an unrealistic condition, cause only a 4 % increase in rain over the domain. If we assume our simulation has a fine enough grid resolution and an accurate representation of the relevant atmospheric processes, the simulated weak and non-linear response of cloud and rain properties to linearly scaled anthropogenic emissions suggests that the interactions among aerosol, cloud, and precipitation in the Amazonian convective environment are buffered by microphysical processes. It also implies that the convective environment is resilient to the changes in Nd that occur in response to localized anthropogenic aerosol perturbations.

Wang, Xuemei [University of Leeds (United Kingdom)↗
DOE OSTI2019

Microphysical and Dynamical Effects of Mixed-Phase Hydrometeors in Convective Storms Using a Bin Microphysics Model: Melting

Abstract The dynamics of convective systems are inherently linked to microphysical processes through phase changes that result in warming or cooling. This is especially true of near-surface cooling via evaporation and melting of falling hydrometeors. In most numerical simulations, the melting of frozen hydrometeors (e.g., hail, graupel, snow) is computed within parameterized bulk microphysics schemes, many of which lack the ability to accurately represent mixed-phase hydrometeors (i.e., partially melted ice), which can affect hydrometeor sedimentation, melting, and evaporation of shed drops. To better understand the microphysical and dynamical effects of melting in convective storms, a bin microphysics scheme was used in the Weather Research and Forecasting Model for two idealized cases: a supercell storm and a squall line. Physically based predicted liquid fraction, instantaneous melting, and instantaneous shedding schemes were used to examine the role and importance of melting hydrometeors for these two storm modes. The results suggest that the amount of precipitation is dependent on the representation of melting. Moreover, the dynamic and thermodynamic characteristics of the simulated storms are found to differ substantially between the melting scenarios, resulting in varied storm system evolution; these differences are found to be dependent on the ambient aerosol concentration, although the differences induced by changing the representation of melting generally outweigh those of changing the aerosol loading. The results highlight the large role of melting in convective storm characteristics and suggest that further model improvements are needed in the near future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Implementation and Evaluation of Physics-Driven Dynamic Entrainment-Mixing Parameterization in a Climate Model and Its Impact on Low-Cloud Simulation

The turbulent entrainment-mixing process in the Community Earth System Model version 1.2 (CESM1.2) is assumed to follow the extremely inhomogeneous entrainment-mixing. However, different entrainment-mixing scenarios can occur in real clouds. To address this deficiency, a unifying parameterization that represents different entrainment-mixing processes is implemented and evaluated in CESM1.2. The results indicate that the homogeneous mixing degree values simulated by the new parameterization in CESM1.2 are predominantly greater than 50%, suggesting a tendency toward homogeneous mixing. Compared to the extremely inhomogeneous mixing mechanism, the new parameterization increases the cloud droplet number concentration (Nc). More importantly, the new parameterization improves low-cloud fraction (CLDLOW) simulation in Northwest Pacific (NWP) and Southeast Pacific (SEP) regions, with relative improvements of 2.95% and 4.17%, respectively. Furthermore, the improvements reach up to 44.6% and 16.2% in the NWP and SEP regions, respectively, when considering the relationship between N c and CLDLOW. Further analysis reveals that the new parameterization enhances cloud optical depth, longwave radiative cooling effect, net condensation rate, cloud water mixing ratio, lower-troposphere stability, and CLDLOW by increasing N c . Additionally, these results underscore the importance of improving entrainment-mixing parameterization in climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

Prediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol–ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on collocated measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, which are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol–ice formation closure. Furthermore, the closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions.

58 GEOSCIENCES↗
DOE OSTI2020

Reconciling Contrasting Relationships Between Relative Dispersion and Volume-Mean Radius of Cloud Droplet Size Distributions

Cloud droplet spectral relative dispersion is critical to parameterizations of cloud radiative properties, warm-rain initiation, and aerosol-cloud interactions in models; however, there is no consistent relationship between relative dispersion and volume-mean radius in literature, which hinders improving relative dispersion parameterization and calls for physical explanation. Here we show, by analyzing aircraft observations of cumulus clouds during Routine AAF [Atmospheric Radiation Measurement (ARM) Aerial Facility] Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations, that the correlation between relative dispersion and volume-mean radius changes from positive to negative as volume-mean radius increases. With the new observation, we postulate that the sign of the correlation is determined by whether or not condensation (evaporation) occurs simultaneously with significant new activation (deactivation). The hypothesis is validated by simulations of both an adiabatic cloud parcel model and a parcel model accounting for entrainment-mixing. A new quantity, first bin strength, is introduced to quantify this new observation. Theoretical analysis of truncated gamma and modified gamma size distributions further supports the hypothesis and reconciles the contrasting relationships between relative dispersion and volume-mean radius, including the results in polluted fog observations. The results could shed new light on the so-called “twilight zone” between cloudy and cloud-free air, which in turn affects evaluation of aerosol-cloud interactions and retrieval of aerosol optical depth.

Lu, Chunsong↗
DOE OSTI2022

Better calibration of cloud parameterizations and subgrid effects increases the fidelity of the E3SM Atmosphere Model version 1

Abstract. Realistic simulation of the Earth's mean-state climate remains a major challenge, and yet it is crucial for predicting the climate system in transition. Deficiencies in models' process representations, propagation of errors from one process to another, and associated compensating errors can often confound the interpretation and improvement of model simulations. These errors and biases can also lead to unrealistic climate projections and incorrect attribution of the physical mechanisms governing past and future climate change. Here we show that a significantly improved global atmospheric simulation can be achieved by focusing on the realism of process assumptions in cloud calibration and subgrid effects using the Energy Exascale Earth System Model (E3SM) Atmosphere Model version 1 (EAMv1). The calibration of clouds and subgrid effects informed by our understanding of physical mechanisms leads to significant improvements in clouds and precipitation climatology, reducing common and long-standing biases across cloud regimes in the model. The improved cloud fidelity in turn reduces biases in other aspects of the system. Furthermore, even though the recalibration does not change the global mean aerosol and total anthropogenic effective radiative forcings (ERFs), the sensitivity of clouds, precipitation, and surface temperature to aerosol perturbations is significantly reduced. This suggests that it is possible to achieve improvements to the historical evolution of surface temperature over EAMv1 and that precise knowledge of global mean ERFs is not enough to constrain historical or future climate change. Cloud feedbacks are also significantly reduced in the recalibrated model, suggesting that there would be a lower climate sensitivity when it is run as part of the fully coupled E3SM. This study also compares results from incremental changes to cloud microphysics, turbulent mixing, deep convection, and subgrid effects to understand how assumptions in the representation of these processes affect different aspects of the simulated atmosphere as well as its response to forcings. We conclude that the spectral composition and geographical distribution of the ERFs and cloud feedback, as well as the fidelity of the simulated base climate state, are important for constraining the climate in the past and future.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2014

The Impact of Microphysics and Planetary Boundary Layer Physics on Model Simulation of U.S. Deep South Summer Convection

Inspection of output from various configurations of high-resolution, explicit convection forecast models such as the Weather Research and Forecasting (WRF) model indicates significant sensitivity to the choices of model physics pararneterizations employed. Some of the largest apparent sensitivities are related to the specifications of the cloud microphysics and planetary boundary layer physics packages. In addition, these sensitivities appear to be especially pronounced for the weakly-sheared, multicell modes of deep convection characteristic of the Deep South of the United States during the boreal summer. Possible ocean-land sensitivities also argue for further examination of the impacts of using unique ocean-land surface initialization datasets provided by the NASA Short-term Prediction Research and Transition (SPoRn Center to select NOAAlNWS weather forecast offices. To obtain better quantitative understanding of these sensitivities and also to determine the utility of the ocean-land initialization data, we have executed matrices of regional WRF forecasts for selected convective events near Mobile, AL (MOB), and Houston, TX (HGX). The matrices consist of identically initialized WRF 24-h forecasts using any of eight microphysics choices and any of three planetary boWldary layer choices. The resulting 24 simulations performed for each event within either the MOB or HGX regions are then compared to identify the sensitivities of various convective storm metrics to the physics choices. Particular emphasis is placed on sensitivities of precipitation timing, intensity, and coverage, as well as amount and coverage oflightuing activity diagnosed from storm kinematics and graupel in the mixed phase layer. The results confirm impressions gleaned from study of the behavior of variously configured WRF runs contained in the ensembles produced each spring at the Center for the Analysis and Prediction of Storms, but with the benefit of more straightforward control of the physics package choices. The design of the experiments thus allows for more direct interpretation of the sensitivities to each possible physics combination. The results should assist forecasters in their efforts to anticipate and correct for possible biases in simulated WRF convection patterns, and help the modeling community refine their model parameterizations.

McCaul, Eugene W., Jr.↗
DOE OSTI2022

Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Influence of Superparameterization and a Higher-Order Turbulence Closure on Rainfall Bias Over Amazonia in Community Atmosphere Model Version 5

In this work, we evaluate the Community Atmosphere Model Version 5 (CAM5) with a higher-order turbulence closure scheme, named Cloud Layers Unified By Binomials (CLUBB), and a Multiscale Modeling Framework (MMF) with two different microphysics configurations to investigate their influences on rainfall simulations over Southern Amazonia. The two different microphysics configurations in MMF are the one-moment cloud microphysics without aerosol treatment (SAM1MOM) and two-moment cloud microphysics coupled with aerosol treatment (SAM2MOM). Results show that both MMF-SAM2MOM and CLUBB effectively reduce the low biases of rainfall, mainly during the wet season. The CLUBB reduces low biases of humidity in the lower troposphere with further reduced shallow clouds. The latter enables more surface solar flux, leading to stronger convection and more rainfall. MMF, especially MMF-SAM2MOM, unstablizes the atmosphere with more moisture and higher atmospheric temperatures in the atmospheric boundary layer, allowing the growth of more extreme convection and further generating more deep convection. MMF-SAM2MOM significantly increases rainfall in the afternoon, but it does not reduce the early bias of the diurnal rainfall peak; LUBB, on the other hand, delays the afternoon peak time and produces more precipitation in the early morning, due to more realistic gradual transition between shallow and deep convection. MMF appears to be able to realistically capture the observed increase of relative humidity prior to deep convection, especially with its two-moment configuration. In contrast, in CAM5 and CAM5 with CLUBB, occurrence of deep convection in these models appears to be a result of stronger heating rather than higher relative humidity.

58 GEOSCIENCES↗
DOE OSTI2022

Convective and Turbulent Motions in Nonprecipitating Cu. Part II: LES Simulated Cloud Represented by a Starting Plume

The dynamic structure of a small trade wind cumulus (Cu) is analyzed using a novel approach. Cu developing in a shear-free environment is simulated by 10-m-resolution LES model with spectral bin microphysics. The aim is to clarify the dynamical nature of cloud updraft zone (CUZ) including entrainment and mixing in growing Cu. The validity of concept stating that a cloud at developing state can be represented by a parcel or a jet is tested. To investigate dynamical entrainment in CUZ performed by motions with scales larger than the turbulence scales, the modeled fields of air velocity were filtered by wavelet filter that separated convective motions from turbulent ones. Two types of objects in developing cloud were investigated: small volume ascending at maximal velocity (point parcel) and CUZ. It was found that the point parcel representing the upper part of cloud core is adiabatic. The motion of the air in this parcel ascending from cloud base determines cloud-top height. The top-hat (i.e., averaged) values of updraft velocity and adiabatic fraction in CUZ are substantially lower than those in the point parcel. Evaluation of the terms in the dynamical equation typically used in 1D cloud parcel models show that this equation can be applied for calculation of vertical velocities at the developing stage of small Cu, at least up to the heights of the inversion layer. Dynamically, the CUZ of developing cloud resembles the starting plume with the tail of nonstationary jet. Both the top-hat vertical velocity and buoyancy acceleration linearly increase with the height, at least up to the inversion layer. An important finding is that lateral entrainment of convective (nonturbulent) nature has a little effect on the top-hat CUZ velocity and cannot explain the vertical changes of conservative variables qt and θl. In contrast, entrained air lifting inside CUZ substantially decreases top-hat liquid water content and its adiabatic fraction. Possible reasons of these effects are discussed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Processing of Ice Cloud In Situ Data Collected by Bulk Water, Scattering, and Imaging Probes: Fundamentals, Uncertainties, and Efforts toward Consistency

Abstract In situ observations of cloud properties made by airborne probes play a critical role in ice cloud research through their role in process studies, parameterization development, and evaluation of simulations and remote sensing retrievals. To determine how cloud properties vary with environmental conditions, in situ data collected during different field projects processed by different groups must be used. However, because of the diverse algorithms and codes that are used to process measurements, it can be challenging to compare the results. Therefore it is vital to understand both the limitations of specific probes and uncertainties introduced by processing algorithms. Since there is currently no universally accepted framework regarding how in situ measurements should be processed, there is a need for a general reference that describes the most commonly applied algorithms along with their strengths and weaknesses. Methods used to process data from bulk water probes, single-particle light-scattering spectrometers and cloud-imaging probes are reviewed herein, with emphasis on measurements of the ice phase. Particular attention is paid to how uncertainties, caveats, and assumptions in processing algorithms affect derived products since there is currently no consensus on the optimal way of analyzing data. Recommendations for improving the analysis and interpretation of in situ data include the following: establishment of a common reference library of individual processing algorithms, better documentation of assumptions used in these algorithms, development and maintenance of sustainable community software for processing in situ observations, and more studies that compare different algorithms with the same benchmark datasets.

54 ENVIRONMENTAL SCIENCES↗