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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Evaluation of a quasi-steady-state approximation of the cloud droplet growth equation (QDGE) scheme for aerosol activation in global models using multiple aircraft data over both continental and marine environments

This research introduces a numerically efficient aerosol activation scheme and evaluates it by using stratus and stratocumulus cloud data sampled during multiple aircraft campaigns in Canada, Chile, Brazil, and China. The scheme employs a quasi-steady-state approximation of the cloud droplet growth equation (QDGE) to efficiently simulate aerosol activation, the vertical profile of supersaturation, and the activated cloud droplet number concentration (CDNC) near the cloud base. The calculated maximum supersaturation values using the QDGE scheme were compared with multiple parcel model simulations under various aerosol and environmental conditions. The differences are all below 0.18 %, indicating good performance and accuracy of the QDGE scheme. We evaluated the QDGE scheme by specifying observed environmental thermodynamic variables and aerosol information from 31 cloud cases as input and comparing the simulated CDNC with cloud observations. The average of mean relative error ($\overline{MRE}$) of the simulated CDNC for cloud cases in each campaign ranges from 17.30 % in Brazil to 25.90 % in China, indicating that the QDGE scheme successfully reproduces observed variations in CDNC over a wide range of different meteorological conditions and aerosol regimes. Additionally, we carried out an error analysis by calculating the maximum information coefficient (MIC) between the MRE and input variables for the individual campaigns and all cloud cases. MIC values were then sorted by aerosol properties, pollution level, environmental humidity, and dynamic condition according to their relative importance to MRE. Based on the error analysis, we found that the magnitude of MRE is more relevant to the specification of input aerosol pollution level in marine regions and aerosol hygroscopicity in continental regions than to other variables in the simulation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Constraining Black Carbon Aging in Global Models to Reflect Timescales for Internal Mixing

The radiative effects of black carbon depend critically on its atmospheric lifetime, which is controlled by the rate at which freshly emitted combustion particles become internally mixed with other aerosol components. Global aerosol models strive to represent this process, but the timescale for aerosol mixing is not easily constrained using observations. In this study, we apply a timescale parameterization derived from particle‐resolved simulations to quantify, in a global aerosol model, the timescale for internal mixing. We show that, while highly variable, the average timescale for internal mixing is approximately 3 hr, which is much shorter than the 24‐hr aging timescale traditionally applied in bulk aerosol models. We then use the mixing timescale to constrain the aging criterion in the Modal Aerosol Module. Our analysis reveals that, to best reflect timescales for internal mixing, modal models should assume that particles transition from the hydrophobic (fresh) to the hydrophilic (aged) class once they accumulate a coating thickness equal to four monolayers of sulfuric acid, as opposed to the model's current aging criterion of eight monolayers. We show that, in remote regions like the Arctic and Antarctic, predictions of black carbon loading and its seasonal variation are particularly sensitive to the model representation of aging. By constraining aging in global models to reflect mixing timescales simulated by the particle‐resolved model, we eliminate one of the free parameters governing black carbon's long‐range transport and spatiotemporal distribution.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Brown, Hunter York (ORCID:0000000218147874)↗
DOE OSTI2022

OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on clouds

Sea spray aerosol is one of the major sources of atmospheric particulate matter globally. It has increasingly been recognized that organic matter derived from ocean biological precursors contributes significantly to the composition of submicron sea spray and may modify sea spray aerosol impacts on clouds and climate. This paper describes the implementation of the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) parameterization for sea spray organic aerosol emissions in a global Earth system model, the Energy Exascale Earth System Model (E3SM). OCEANFILMS is a physically based model that links sea spray chemistry with ocean biogeochemistry using a Langmuir partitioning approach. We describe the implementation details of OCEANFILMS within E3SM, compare simulated aerosol fields with observations, and investigate impacts on simulated clouds and climate. Four sensitivity cases are tested, in which organic emissions either strictly add to or strictly replace sea salt emissions (in mass and number) and are either fully internally or fully externally mixed with sea salt. The simulation with internally mixed, added organics agrees reasonably well with observed seasonal cycles of organic matter in marine aerosol and has been selected as the default configuration of the E3SM. In this configuration, sea spray organic aerosol contributes an additional source of cloud condensation nuclei, adding up to 30 cm -3 to Southern Ocean boundary-layer cloud condensation nuclei concentrations (supersaturation = 0.1 %). The addition of this new aerosol source strengthens shortwave radiative cooling by clouds by -0.36 W m -2 in the global annual mean and contributes more than -3.5 W m -2 to summertime zonal mean cloud forcing in the Southern Ocean, with maximum zonal mean impacts of about -4 W m -2 around 50–60°S. This is consistent with a previous top-down, satellite-based empirical estimate of the radiative forcing by sea spray organic aerosol over the Southern Ocean. Through its mechanistic approach, OCEANFILMS offers a path towards improved understanding of the feedbacks between ocean biology, sea spray organic matter, and climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Assessing effective radiative forcing from aerosol–cloud interactions over the global ocean

How clouds respond to anthropogenic sulfate aerosols is one of the largest sources of uncertainty in the radiative forcing of climate over the industrial era. This uncertainty limits our ability to predict equilibrium climate sensitivity (ECS)—the equilibrium global warming following a doubling of atmospheric CO 2 . Here, we use satellite observations to quantify relationships between sulfate aerosols and low-level clouds while carefully controlling for meteorology. We then combine the relationships with estimates of the change in sulfate concentration since about 1850 to constrain the associated radiative forcing. We estimate that the cloud-mediated radiative forcing from anthropogenic sulfate aerosols is − 1.11 ± 0.43 W m −2 over the global ocean (95% confidence). This constraint implies that ECS is likely between 2.9 and 4.5 K (66% confidence). Our results indicate that aerosol forcing is less uncertain and ECS is probably larger than the ranges proposed by recent climate assessments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Global organic and inorganic aerosol hygroscopicity and its effect on radiative forcing

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵ org ) and inorganic ions (ϵ inorg ) through a linear combination, κ = ϵ org · κ org + ϵ inorg · κ inorg . In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κ org = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κ org and κ inorg is small, we constrain a critically important aspect of global climate modelling.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Unexpected Changes of Aerosol Burdens With Decreased Convection in the Context of Scale-Aware Convection Schemes

Atmospheric aerosols in global climate models (GCMs) can be removed by both large-scale and convective precipitation. As the horizontal resolution of GCMs increases, it is expected that large-scale precipitation increases and convective precipitation decreases if scale-aware convection schemes are well developed. Here, to explore its impact on aerosol burdens, this study develops a novel method and applies it to the National Center for Atmospheric Research Community Atmosphere Model version 5.3 to mimic the behavior of scale-aware convective schemes. Surprisingly, it is found that aerosol burden increases globally as convective precipitation decreases and large-scale precipitation increases, which can be attributed to the reduced light rain. In the light-rain intensity category, the decreased frequency of convective precipitation is not offset by the increased frequency of large-scale precipitation. Therefore, for aerosol simulations in high-resolution GCMs using scale-aware convection schemes, subgrid convection and large-scale condensation should be coordinated to assure light rain stays the same.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Updating and Evaluating Anthropogenic Emissions for NOAA’s Global Ensemble Forecast Systems for Aerosols (GEFS-Aerosols): Application of an SO 2 Bias-Scaling Method

We updated the anthropogenic emissions inventory in NOAA’s operational Global Ensemble Forecast for Aerosols (GEFS-Aerosols) to improve the model’s prediction of aerosol optical depth (AOD). We used a methodology to quickly update the pivotal global anthropogenic sulfur dioxide (SO 2 ) emissions using a speciated AOD bias-scaling method. The AOD bias-scaling method is based on the latest model predictions compared to NASA’s Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA2). The model bias was subsequently applied to the CEDS 2019 SO 2 emissions for adjustment. The monthly mean GEFS-Aerosols AOD predictions were evaluated against a suite of satellite observations (e.g., MISR, VIIRS, and MODIS), ground-based AERONET observations, and the International Cooperative for Aerosol Prediction (ICAP) ensemble results. The results show that transitioning from CEDS 2014 to CEDS 2019 emissions data led to a significant improvement in the operational GEFS-Aerosols model performance, and applying the bias-scaled SO 2 emissions could further improve global AOD distributions. The biases of the simulated AODs against the observed AODs varied with observation type and seasons by a factor of 3~13 and 2~10, respectively. The global AOD distributions showed that the differences in the simulations against ICAP, MISR, VIIRS, and MODIS were the largest in March–May (MAM) and the smallest in December–February (DJF). When evaluating against the ground-truth AERONET data, the bias-scaling methods improved the global seasonal correlation (r), Index of Agreement (IOA), and mean biases, except for the MAM season, when the negative regional biases were exacerbated compared to the positive regional biases. The effect of bias-scaling had the most beneficial impact on model performance in the regions dominated by anthropogenic emissions, such as East Asia. However, it showed less improvement in other areas impacted by the greater relative transport of natural emissions sources, such as India. The accuracies of the reference observation or assimilation data for the adjusted inputs and the model physics for outputs, and the selection of regions with less seasonal emissions of natural aerosols determine the success of the bias-scaling methods. A companion study on emission scaling of anthropogenic absorbing aerosols needs further improved aerosol prediction.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

An Improved Convection Parameterization with Detailed Aerosol–Cloud Microphysics for a Global Model

Abstract A new microphysical treatment that includes aerosol–cloud interactions and secondary ice production (SIP) mechanisms is implemented in the convection scheme of the Community Atmosphere Model, version 6 (CAM6). The approach is to embed a 1D Lagrangian parcel model in the bulk convective plume of the existing deep convection parameterization. Aerosol activation, growth processes including collision/coalescence, and three processes of SIP mechanisms, two of which are normally overlooked in atmospheric models, are represented in this embedded parcel model. These microphysical processes are treated with a hybrid bin/bulk scheme and a high spatial and temporal resolution for the integration of the embedded parcel in 1D, allowing vertical velocity to determine the microphysical evolution following the in-cloud motion during ascent. Simulations of an observed case (Midlatitude Continental Convective Clouds Experiment) of a mesoscale convective system in Oklahoma, United States, with a single-column model (SCAM) version of CAM, are compared with aircraft in situ and ground-based observations of microphysical properties from the convection and precipitation. Results from the validation show the new microphysical scheme has a good representation of the ice initiation in the bulk convective plume, including the known and empirically quantified pathways of primary and secondary initiation, with benefits for the accuracy of properties of its supercooled cloud liquid. The sensitivity simulations and use of tagging tracers for the validated simulation confirm that the newly included SIP mechanisms are of paramount importance for convective microphysics and can be successfully treated in the global model.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Global source apportionment of aerosols into major emission regions and sectors over 1850–2017

Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM 2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM 2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM 2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM 2.5 burden by 1.7 mg m -2 and the sources from the Europe were also responsible for the PM 2.5 burden increase in East Asia and South Asia by about 1.0 mg m -2 . During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mg m -2 in the PM 2.5 burden in North America and Europe, while South Asia contributed about 0.3 mg m -2 . During 2010–2017, the contributions from East Asia to the PM 2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mg m -2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERF ari ). During 1980–2010, a decline in North American aerosols resulted in a positive ERF ari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERF ari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERF ari (cooling) changes in South Asia, Southeast Asia, and southern China.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Global Simulations Suggest Biomass Burning Aerosol Emissions From Grassland Fires Could Be Important Ice Nucleating Particles

Ice nucleating particles (INP) capable of nucleating ice crystals via immersion freezing at temperatures above approximately −35°C may strongly influence cloud glaciation, with implications for global precipitation and climate feedback. In addition to mineral dust, soil dust, and marine organics, laboratory and field measurements suggest biomass burning aerosols (BBA) can act as immersion-mode INP between around −30°C and −15°C. However, the contribution of BBA to the global INP budget remains poorly understood due to poor knowledge of which fuels yield INPs, uncertainties in global coverage of those fuels, and unknown size distributions of the INPs in the BBA. Nonetheless, with some understanding of these uncertainties from sensitivity studies, the relative importance of ice nucleation activity of BBA compared to other INP sources can be quantified. In this work, we investigate the potential global importance of BBA as INP using a global aerosol-climate model, specifically the UK Met Office Unified Model (UM). We evaluate the model using field campaign data sets. We examine potential uncertainties in fuel types and particle sizes on BBA-based INP concentrations. Averaged over June–September between 15°S and 50°S, BBA is a more important INP than dust and marine INP about 30% of the time at altitudes with temperatures between −30°C and −20°C. Our simulations therefore suggest BBA INPs may be at least as important as mineral dust and marine INP over the atmospheric regions and seasons where grassland fires are frequent.

Gohil, Kanishk [Carnegie Mellon University, Pittsb↗
DOE OSTI2021

Estimating Submicron Aerosol Mixing State at the Global Scale With Machine Learning and Earth System Modeling

Abstract This study integrates machine learning and particle‐resolved aerosol simulations to develop emulators that predict submicron aerosol mixing state indices from the Earth system model (ESM) simulations. The emulators predict aerosol mixing state using only quantities that are predicted by the ESM, including bulk aerosol species concentrations, which do not by themselves carry mixing state information. We used PartMC‐MOSAIC as the particle‐resolved model and NCAR's CESM as the ESM. We trained emulators for three different mixing state indices for submicron aerosol in terms of chemical species abundance ( χ a ), the mixing of optically absorbing and nonabsorbing species ( χ o ), and the mixing of hygroscopic and nonhygroscopic species ( χ h ). Our global mixing state maps show considerable spatial and seasonal variability unique to each mixing state index. Seasonal averages varied spatially between 13% and 94% for χ a , between 38% and 94% for χ o , and between 20% and 87% for χ h with global annual averages of 67%, 68%, and 56%, respectively. High values in one index can be consistent with low values in another index depending on the grouping of species and their relative abundance, meaning that each mixing state index captures different aspects of the population mixing state. Although a direct validation with observational data has not been possible yet, our results are consistent with mixing state index values derived from ambient observations. This work is a prototypical example of using machine learning emulators to add information to ESM simulations.

54 ENVIRONMENTAL SCIENCES↗