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At least 325 records · Page 18

New Particle Formation and Growth Dynamics for α-Pinene Ozonolysis in a Smog Chamber and Implications for Ambient Environments

Secondary organic aerosol (SOA) plays an important role in the Earth’s energy balance and air quality. Understanding the formation of SOA accompanying the oxidation of volatile organic compounds (VOCs) remains incomplete because of the complex reactions and partitioning mechanisms. In this study, we investigated new particle formation (NPF) of SOA derived from α-pinene ozonolysis in the Harvard Environmental Chamber using the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the condensing species as two products, one of lower volatility (LVOC, 0.01 μg m –3 ) and one of higher volatility (SVOC, 1.0 μg m –3 ). A module for the classical nucleation theory was included. The surface tension (σ), bulk diffusivity (D b ), and mass accommodation coefficient (α) were varied until convergence between the simulated and observed particle number size distributions. α of LVOC was constrained as 0.03–0.1 with the reported σ of α-pinene-ozonolysis-derived SOA and Tolman surface correction (~23.0–27.5 mN m –1 ) and Db from 10 –15.5 to >10 –11 cm 2 s –1 . The observed particle number size distribution of α-pinene ozonolysis was well-simulated to derive the physical parameters, including σ, Db, and α, suggesting the possible application to group the reported complex oxidation products and further application for other atmospheric-related oxidations for quantifying NPF.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-boundary-layer-monsoon interactions amplify semi-direct effect of biomass smoke on low cloud formation in Southeast Asia

Low clouds play a key role in the Earth-atmosphere energy balance and influence agricultural production and solar-power generation. Smoke aloft has been found to enhance marine stratocumulus through aerosol-cloud interactions, but its role in regions with strong human activities and complex monsoon circulation remains unclear. Here we show that biomass burning aerosols aloft strongly increase the low cloud coverage over both land and ocean in subtropical southeastern Asia. The degree of this enhancement and its spatial extent are comparable to that in the Southeast Atlantic, even though the total biomass burning emissions in Southeast Asia are only one-fifth of those in Southern Africa. We find that a synergetic effect of aerosol-cloud-boundary layer interaction with the monsoon is the main reason for the strong semi-direct effect and enhanced low cloud formation in southeastern Asia.

54 ENVIRONMENTAL SCIENCES↗

Evaluation of the interactive stratospheric ozone (O3v2) module in the E3SM version 1 Earth system model

Stratospheric ozone affects climate directly as the predominant heat source in the stratosphere and indirectly through chemical reactions controlling other greenhouse gases. The U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1) implemented a new ozone chemistry module that improves the simulation of the sharp tropopause gradients, replacing a version based partly on long-term average climatologies that poorly represented heating rates in the lowermost stratosphere. The new O3v2 module extends seamlessly into the troposphere and preserves the naturally sharp cross-tropopause gradient, with 20 %–40 % less ozone in this region. Additionally, O3v2 enables the diagnosis of stratosphere–troposphere exchange flux of ozone, a key budget term lacking in E3SMv1. Here, we evaluate key features in ozone abundance and other closely related quantities in atmosphere-only E3SMv1 simulations driven by observed sea surface temperatures (SSTs, years 1990–2014), comparing them with satellite observations of ozone and also with the University of California, Irvine chemistry transport model (UCI CTM) using the same stratospheric chemistry scheme but driven by European Centre forecast fields for the same period. In terms of stratospheric column ozone, O3v2 shows reduced mean bias and improved northern midlatitude variability, but it is not quite as good as the UCI CTM. As expected, SST-forced E3SMv1 simulations cannot synchronize with observed quasi-biennial oscillations (QBOs), but they do show the typical QBO pattern seen in column ozone. This new O3v2 E3SMv1 model mostly retains the same climate state and climate sensitivity as the previous version, and we recommend its use for other climate models that still use ozone climatologies.

54 ENVIRONMENTAL SCIENCES↗

Effects of marine organic aerosols as sources of immersion-mode ice-nucleating particles on high-latitude mixed-phase clouds

Mixed-phase clouds are frequently observed in high-latitude regions and have important impacts on the surface energy budget and regional climate. Marine organic aerosol (MOA), a natural source of aerosol emitted over ~70 % of Earth's surface, may significantly modify the properties and radiative forcing of mixed-phase clouds. However, the relative importance of MOA as a source of ice-nucleating particles (INPs) in comparison to mineral dust, and MOA's effects as cloud condensation nuclei (CCN) and INPs on mixed-phase clouds are still open questions. In this study, we implement MOA as a new aerosol species into the Community Atmosphere Model version 6 (CAM6), the atmosphere component of the Community Earth System Model version 2 (CESM2), and allow the treatment of aerosol–cloud interactions of MOA via droplet activation and ice nucleation. CAM6 reproduces observed seasonal cycles of marine organic matter at Mace Head and Amsterdam Island when the MOA fraction of sea spray aerosol in the model is assumed to depend on sea spray biology but fails when this fraction is assumed to be constant. Model results indicate that marine INPs dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer, while dust INPs are more abundant elsewhere. By acting as CCN, MOA exerts a shortwave cloud forcing change of -2.78 W m-2 over the Southern Ocean in the austral summer. By acting as INPs, MOA enhances the longwave cloud forcing by 0.35 W m-2 over the Southern Ocean in the austral winter. The annual global mean net cloud forcing changes due to CCN and INPs of MOA are -0.35 and 0.016 W m-2, respectively. These findings highlight the vital importance for Earth system models to consider MOA as an important aerosol species for the interactions of biogeochemistry, hydrological cycle, and climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the dynamics and bottleneck of the key atmospheric SO 2 oxidation reaction by the hydroxyl radical

SO 2 (Sulfur dioxide) is the major precursor to the production of sulfuric acid (H 2 SO 4 ), contributing to acid rain and atmospheric aerosols. Sulfuric acid formed from SO 2 generates light-reflecting sulfate aerosol particles in the atmosphere. This property has prompted recent geoengineering proposals to inject sulfuric acid or its precursors into the Earth’s atmosphere to increase the planetary albedo to counteract global warming. SO 2 oxidation in the atmosphere by the hydroxyl radical HO to form HOSO 2 is a key rate-limiting step in the mechanism for forming acid rain. However, the dynamics of the HO + SO 2 → HOSO 2 reaction and its slow rate in the atmosphere are poorly understood to date. Herein, we use photoelectron spectroscopy of cryogenically cooled HOSO 2 – anion to access the neutral HOSO 2 radical near the transition state of the HO + SO 2 reaction. Spectroscopic and dynamic calculations are conducted on the first ab initio-based full-dimensional potential energy surface to interpret the photoelectron spectra of HOSO 2 – and to probe the dynamics of the HO + SO 2 reaction. In addition to the finding of a unique pre-reaction complex (HO⋯SO 2 ) directly connected to the transition state, dynamic calculations reveal that the accessible phase space for the HO + SO 2 → HOSO 2 reaction is extremely narrow, forming a key reaction bottleneck and slowing the reaction rate in the atmosphere, despite the low reaction barrier. This study underlines the importance of understanding the full multidimensional potential energy surface to elucidate the dynamics of complex bimolecular reactions involving polyatomic reactants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Year-round trace gas measurements in the central Arctic during the MOSAiC expedition

Despite the key role of the Arctic in the global Earth system, year-round in-situ atmospheric composition observations within the Arctic are sparse and mostly rely on measurements at ground-based coastal stations. Measurements of a suite of in-situ trace gases were performed in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. These observations give a comprehensive picture of year-round near-surface atmospheric abundances of key greenhouse and trace gases, i.e., carbon dioxide, methane, nitrous oxide, ozone, carbon monoxide, dimethylsulfide, sulfur dioxide, elemental mercury, and selected volatile organic compounds (VOCs). Redundancy in certain measurements supported continuity and permitted cross-evaluation and validation of the data. This paper gives an overview of the trace gas measurements conducted during MOSAiC and highlights the high quality of the monitoring activities. In addition, in the case of redundant measurements, merged datasets are provided and recommended for further use by the scientific community.

54 ENVIRONMENTAL SCIENCES↗

The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics

Abstract. Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and black carbon (BC) particulate emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as particulate phase sulfate (SO4) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m−2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models.

54 ENVIRONMENTAL SCIENCES↗

Improving the QBO Forcing by Resolved Waves With Vertical Grid Refinement in E3SMv2

Abstract The quasi‐biennial oscillation (QBO) is the dominate mode of variability in the tropical stratosphere and plays an important role in stratospheric dynamics and chemistry. The QBO is notably deficient in many climate models, including the Energy Exascale Earth System Model (E3SM) developed by the US Department of Energy. In this work, we refine the lower stratospheric vertical grid spacing from roughly 1 km to 500 m to facilitate more realistic equatorial wave activity in the lower stratosphere in E3SM version 2. The refinement results in a simulated QBO with a reasonable amplitude and easterly‐westerly transition in both directions, but still has a longer period than observed, slower easterly downward propagation speed, and shallower vertical depth. Similar refinement in the multi‐scale modeling framework configuration of E3SM yields similar improvements. By analyzing the forcing contributions from different wave types, we find that most of the QBO forcing still comes from parameterized gravity wave drag from convection. The improved QBO forcing contributions from resolved waves, especially equatorial Kelvin waves and resolved small scale waves, can be attributed to the grid refinement.

E3SM↗

Radiative Forcing of Nitrate Aerosols From 1975 to 2010 as Simulated by MOSAIC Module in CESM2-MAM4

In this work, we incorporate the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model Version 6 with interactive chemistry (CAM6-chem), and couple it with the four mode version of the Modal Aerosol Module (MAM4). The MOSAIC module is used to simulate the thermodynamics of the gas-aerosol mass exchange, with a special focus on simulating nitrate aerosol. By comparing against ground and satellite observations, we found that the MOSAIC/MAM4 scheme performs reasonably well in simulating spatiotemporal distributions of aerosols, including nitrate aerosol. We conducted a series of model experiments with and without nitrate aerosols, and examined the radiative effect (RE) associated with nitrate aerosols in 1975, 2000, and 2010, and accessed the radiative forcing (RF) of nitrate aerosols between the present day and pre-industrial periods. Comparing with the nitrate aerosol RE, we predicted relatively small RF of anthropogenic nitrate aerosol from aerosol-radiation interactions (RF ari : -0.014 W m -2 ) and large RF from aerosol-cloud interactions (RF aci : -0.219 W m -2 ). Regional signatures of nitrate RE/RF are noticeable and important: for instance, very small changes in RE ari in Europe and USA, but 2.8–3 times increases in RE ari in India and China from 1975 to 2010, while RE aci /RF aci in China is a warming effect due to the competing effect between sulfate and nitrate aerosols as cloud condensation nuclei.

54 ENVIRONMENTAL SCIENCES↗

Multi-campaign ship and aircraft observations of marine cloud condensation nuclei and droplet concentrations

In situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP 2 EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

54 ENVIRONMENTAL SCIENCES↗

Large Eddy Simulations of the Atmospheric Boundary Layer Over Satellite‐Sensed Sea Ice Maps

Surface heterogeneity in the marginal ice zone (MIZ) causes multiscale secondary atmospheric circulations that are challenging to model or observe. The absence or inadequate representation of these circulations in ocean‐atmosphere exchange schemes in climate models is partially responsible for the underestimation of Arctic sea ice loss. Observationally, such circulations obfuscate the interpretation of polar atmospheric chemistry measurements, among others. To address this open challenge, large‐eddy simulations are conducted over real‐world satellite‐sensed sea ice maps with an ice‐sea temperature contrast, as well as over idealizations of these maps that alter the ice pattern but conserve its fraction, showing that the ice fraction of a surface is not sufficient to predict the surface heat flux. In a second suite of simulations, three other heterogeneity metrics (representing the surface fragmentation, patch edge tortuosity, and patch size variability) are introduced to complement the ice fraction in describing the surface. Simulations varying these parameters suggest that they also significantly impact surface‐air interactions. A roughness contrast is then added to the surface temperature contrast, indicating that the contribution of roughness changes to the resulting atmospheric circulations is less pronounced than that of thermal heterogeneity. Based on these results, we illustrate, using a multi‐linear regression on these map features, that MIZ surface parameterizations in Earth Systems Models can be improved if they account for these various characteristics of the sea‐ice patterns.

54 ENVIRONMENTAL SCIENCES↗

Overestimated natural biological nitrogen fixation translates to an exaggerated CO 2 fertilization effect in Earth system models

CO 2 fertilization of the terrestrial biosphere is limited by nitrogen. Biological nitrogen fixation (BNF) is the dominant natural nitrogen source to the terrestrial biosphere and can alleviate nitrogen limitation but is poorly constrained in Earth system models (ESMs). Here, in this study, we compare terrestrial BNF from an ensemble of ESMs of the 6th Coupled Model Intercomparison Project to a new global synthesis of observations across natural and agricultural biomes. We find that compared to observations, ESMs underestimate agricultural BNF but overestimate natural BNF in the present day by over 50%. Natural BNF is overestimated in the most productive ecosystems that contribute most to the terrestrial carbon sink (forests and grasslands). ESMs with different BNF representations yield a range of BNF responses to CO 2 enrichment. Some ESMs with phenomenological representations of BNF predict a natural BNF increase in response to a doubling of CO 2 that aligns with a meta-analysis of CO 2 enrichment experiments (31% increase) but fail to account for the substantial carbon cost of BNF. In contrast, ESMs with mechanistic representations of BNF account for its carbon cost as well as its regulation by nitrogen limitation but overestimate the BNF response to a doubling of CO 2 (135% increase). Overall, all current BNF representations in ESMs fall short of fully capturing its response to rising atmospheric CO 2 . Finally, we find a positive correlation between modeled present-day natural BNF and the CO 2 fertilization effect across ESMs, suggesting that overestimated natural BNF translates to an exaggerated CO 2 fertilization effect of approximately 11% in ESMs.

Biological nitrogen fixation↗

Nitrogen Deposition Weakens Soil Carbon Control of Nitrogen Dynamics Across the Contiguous United States

ABSTRACT Anthropogenic nitrogen (N) deposition is unequally distributed across space and time, with inputs to terrestrial ecosystems impacted by industry regulations and variations in human activity. Soil carbon (C) content normally controls the fraction of mineralized N that is nitrified ( ƒ nitrified ), affecting N bioavailability for plants and microbes. However, it is unknown whether N deposition has modified the relationships among soil C, net N mineralization, and net nitrification. To test whether N deposition alters the relationship between soil C and net N transformations, we collected soils from coniferous and deciduous forests, grasslands, and residential yards in 14 regions across the contiguous United States that vary in N deposition rates. We quantified rates of net nitrification and N mineralization, soil chemistry (soil C, N, and pH), and microbial biomass and function (as beta‐glucosidase (BG) and N ‐acetylglucosaminidase (NAG) activity) across these regions. Following expectations, soil C was a driver of ƒ nitrified across regions, whereby increasing soil C resulted in a decline in net nitrification and ƒ nitrified . The ƒ nitrified value increased with lower microbial enzymatic investment in N acquisition (increasing BG:NAG ratio) and lower active microbial biomass, providing some evidence that heterotrophic microbial N demand controls the ammonium pool for nitrifiers. However, higher total N deposition increased ƒ nitrified , including for high soil C sites predicted to have low ƒ nitrified , which decreased the role of soil C as a predictor of ƒ nitrified . Notably, the drop in contemporary atmospheric N deposition rates during the 2020 COVID‐19 pandemic did not weaken the effect of N deposition on relationships between soil C and ƒ nitrified . Our results suggest that N deposition can disrupt the relationship between soil C and net N transformations, with this change potentially explained by weaker microbial competition for N. Therefore, past N inputs and soil C should be used together to predict N dynamics across terrestrial ecosystems.

Nieland, Matthew A. [Stockbridge School of Agricul↗

Bedrock weathering rates, reactive nitrogen influxes and effluxes, and nitrous oxide emissions rates from the Pumphouse Hillslope, East River Watershed, Colorado

Atmospheric nitrous oxide contributes directly to global warming, yet models of the nitrogen cycle do not account for bedrock, the largest pool of terrestrial nitrogen, as a source of nitrous oxide. Although it is known that release rates of nitrogen from bedrock are large, there is an incomplete understanding of the connection between bedrock-hosted nitrogen and atmospheric nitrous oxide. Here, we quantify nitrogen fluxes and mass balances at a hillslope underlain by marine shale. We found that at this site bedrock weathering contributes 78% of the subsurface reactive nitrogen, while atmospheric sources (commonly regarded as the sole sources of reactive nitrogen in pristine environments) account for only the remaining 22%. About 56% of the total subsurface reactive nitrogen denitrifies, including 14% emitted as nitrous oxide. The remaining reactive nitrogen discharges in porewaters to a floodplain where additional denitrification likely occurs. We also found that the release of bedrock nitrogen occurs primarily within the zone of the seasonally fluctuating water table and suggest that the accumulation of nitrate in the vadoes zone, often attributed to fertilization and soil leaching, may also include contributions from weathered nitrogen-rich bedrock. Our hillslope study suggests that under oxygenated and moisture-rich conditions, weathering of deep, nitrogen-rich bedrock makes an important contribution to the nitrogen cycle. The data files are in Excel, which can be accessed using Microsoft Office, and consist of many data sets from the Pumphouse Hillslope PLM (Pumphouse Lower Montane) 1, 2, 3, and 4. They include soil to rock (0-10 meters) solid phase minerals and elements compositions; time- and depth-resolved pore-water chemistry and pore-gas compositions; time- and depth-resolved water table depths and water fluxes; subsurface weathering rates; nitrogen influxes and effluxes and mass balance. The attached paper is in a Word document, which can be accessed using Microsoft Office, and in pdf format.

54 ENVIRONMENTAL SCIENCES↗

Investigating Material Behavior in Atmospheric Entry Conditions: Arc-Jet Testing Insights from Meteorite Ablation to High-Temperature Coatings.

Arc-jet testing is an indispensable tool in elucidating the complex interactions materials undergo when subjected to the extreme thermal and mechanical stresses of atmospheric entry. By replicating these harsh conditions, arc-jets enable researchers to explore critical phenomena such as ablation, melting, and spallation, generating invaluable data that informs the development of sophisticated, physics-based models. These models are pivotal not only in predicting material performance for spacecraft re-entry systems but also in assessing the threat posed by celestial bodies as they encounter Earth’s atmosphere. One of the leading facilities for such investigations is the Hypersonic Materials Environmental Test System (HyMETS) at NASA’s Langley Research Center. A pioneering test campaign conducted at HyMETS focused on unraveling the ablation mechanisms of an ordinary chondrite meteorite (Tamdakht H5) and a terrestrial analog (basalt). These studies unveiled distinct material behaviors: Tamdakht demonstrated a remarkably stable melt flow, with mass loss primarily driven by the volatilization of elements such as iron and sodium, whereas basalt exhibited more aggressive surface degradation due to the rapid decomposition of hydrated minerals, culminating in significant spallation and surface material ejection. Beyond meteorite analysis, HyMETS has also been integral in the exploration of advanced Thermal Protection Systems (TPS) such as Phenolic Impregnated Carbon Ablator (PICA), a material with extensive flight heritage in missions like Stardust, Mars Science Laboratory, Mars 2020, and Osiris-REx. PICA, when coated with NuSil CV-1144-0—a polysiloxane resin designed to prevent particle shedding—undergoes a remarkable transformation upon heating. The resin pyrolyzes to form a thin, oxidation-resistant silicon oxycarbide layer that profoundly influences the material’s thermal response through a sophisticated four-stage process. Initially, the silicon oxycarbide acts as a formidable barrier, impeding reactive interactions with the PICA char and effectively suppressing surface temperature rise and material recession. However, as the heating persists, the protective layer decomposes via carbothermal reduction, exposing the underlying char, which in turn leads to a dramatic spike in surface temperature and accelerated material erosion. In the final stage, equilibrium is reached, with recession rates aligning with those of the virgin material. This intricate understanding of PICA-NuSil behavior under extreme conditions offers valuable insights, enhancing material response models and advancing the development of next-generation TPS for space exploration.

Chemistry↗

Pooling Data Improves Multimodel IDF Estimates over Median-Based IDF Estimates: Analysis over the Susquehanna and Florida

Traditional multimodel methods for estimating future changes in precipitation intensity, duration, and frequency (IDF) curves rely on mean or median of models’ IDF estimates. Such multimodel estimates are impaired by large estimation uncertainty, shadowing their efficacy in planning efforts. Here, assuming that each climate model is one representation of the underlying data generating process, i.e., the Earth system, we propose a novel extension of current methods through pooling model data: (i) evaluate performance of climate models in simulating the spatial and temporal variability of the observed annual maximum precipitation (AMP), (ii) bias-correct and pool historical and future AMP data of reasonably performing models, and (iii) compute IDF estimates in a nonstationary framework from pooled historical and future model data. Pooling enhances fitting of the extreme value distribution to the data and assumes that data from reasonably performing models represent samples from the “true” underlying data generating distribution. Through Monte Carlo simulations with synthetic data, we show that return periods derived from pooled data have smaller biases and lesser uncertainty than those derived from ensembles of individual model data. We apply this method to NA-CORDEX models to estimate changes in 24-h precipitation intensity–frequency (PIF) estimates over the Susquehanna watershed and Florida peninsula. Our approach identifies significant future changes at more stations compared to median-based PIF estimates. The analysis suggests that almost all stations over the Susquehanna and at least two-thirds of the stations over the Florida peninsula will observe significant increases in 24-h precipitation for 2–100-yr return periods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

High-Order Methods in NASA’s Next Generation of Computational Fluid Dynamics Tools

The missions of the National Aeronautics and Space Administration (NASA) routinely produce unique requirements and challenges for development and application of Computational Fluid Dynamics (CFD) methods. NASA presently embodies four distinct Mission Directorates: Aeronautics Research, Exploration Systems, Science, and Space Operations. These missions generate requirements for systems that operate in a wide variety of environments. They range from the high-speed flight of aerodynamically optimized vehicles operating in the earth’s atmosphere to spacecraft designed for missions that don’t favor aerodynamic optimization, some operating in the atmosphere of planets and planetary moons such as Mars and Venus or Saturn’s moon Titan. Systems supporting these vehicles, such as rocket and jet propulsion, reaction control systems, fluid and thermal transfer systems, etc. can also generate their own unique set of flow phenomena that challenge today’s CFD methodology. Through the NASA Engineering and Safety Center (NESC), NASA annually conducts state-of-the-discipline assessments in fifteen distinct engineering disciplines. These assessments are performed by the NASA Technical Fellows that lead Technical Discipline Teams (TDT) of recognized experts in these fifteen areas. In the Aerosciences discipline, three topics have been identified as the top challenges for the discipline: aero-plume interaction prediction, unsteady separated flows, and aerothermodynamic prediction. These challenge areas are defined by the Agency’s high-risk projects and problems on which the NESC is requested to perform independent testing, analysis, and assessments. When viewed as a whole, these tests, analyses, and assessments provide a clear view of the recurring technical challenges facing Agency engineers and researchers and can be used to guide future research and technology development. The present state-of-the-art in the application of CFD at NASA is the use of Reynolds-Averaged Navier- Stokes (RANS) solvers, primarily executed in a steady-state mode of operation. In isolated cases, Unsteady RANS (URANS) solvers have been employed when steady RANS solutions produce poorly converging or oscillating results or in cases, such as aeroelastic analysis, which require unsteady aerodynamic simulation. For most traditional external and internal aerodynamic flows, structured overset grids or unstructured grids are employed to minimize geometric modeling and grid generation times. Grid adaptation, primarily as a series of coarse-grain intermediate processing steps is also seeing use on particularly complex flow problems and configurations. In the case of aerothermodynamic flows, engineers have been forced to continue to employ structured grid techniques as the present unstructured grid methodology has proven inadequate in the prediction of surface heating. In the area of aero-plume interaction modeling, two-gas, frozen chemistry simulation is generally the state-of-the- art, with some production solvers capable of predicting flows with only a single gas component. Prediction of flows falling into the afore-mentioned top Aerosciences technical challenges have severely stressed the present state-of-the-art in CFD prediction and for some problems, such as unsteady separated flows and aero-plume interaction cases, engineers have begun employing Large Eddy Simulation (LES) and Hybrid RANS/LES techniques. In some isolated aero-propulsion interaction cases, chemically reacting flow simulations have been applied. These methods are highly evolutionary and engineers have little experience in their application, so they cannot be heavily relied upon in today’s application environment. Therefore, this leads one to muse over which numerical technologies will be included in the CFD tools that will be employed 30 years in the future. This presentation will describe specific technical problems that have stressed NASA’s traditional CFD methods to their breaking point and will link these issues to the Agency’s top Aerosciences technical challenges. The discussion will then shift to the characteristics of future CFD solvers that will be required to attack these challenges and how these characteristics differ from the present state-of-the- art. High-order methods certainly appear to have a place in the development of future CFD tools and some of the physical characteristics of our most challenging problems suggest that high-order methods are the only way to effectively solve them. But there are some relatively severe implementation issues that face these methods, particularly in the area of general applicability and robust operation as an engineering tool. Desired characteristics of next-generation CFD solvers will be discussed and the author’s view of which emerging numerical technologies might be employed to address these attributes will also be presented

David M Schuster↗