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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties

The scattering and backscattering enhancement factors (ƒ(RH) and ƒ b (RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles ƒ(RH) and ƒ b (RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of ƒ(RH) and ƒ b (RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher ƒ(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement ƒ b (RH) is consistently lower than ƒ(RH) at all sites, with the difference between ƒ(RH) and ƒ b (RH) increasing for aerosol with higher ƒ(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM 1 than PM 10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, ƒ(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of ƒ(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω 0 , and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω 0 and scattering Ångström exponent, α sp ) to parameterize ƒ(RH). The majority of sites (75 %) showed a consistent trend with ω 0 (higher ƒ(RH = 85 %) for higher ω 0 ), while no clear pattern was observed between ƒ(RH = 85 %) and αsp. This suggests that aerosol ω 0 is more promising than α sp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω 0 and ƒ(RH) could serve as a constraint on global model simulations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Identifying the sources of uncertainty in climate model simulations of solar radiation modification with the G6sulfur and G6solar Geoengineering Model Intercomparison Project (GeoMIP) simulations

We present here results from the Geoengineering Model Intercomparison Project (GeoMIP) simulations for the experiments G6sulfur and G6solar for six Earth system models participating in the Climate Model Intercomparison Project (CMIP) Phase 6. The aim of the experiments is to reduce the warming that results from a high-tier emission scenario (Shared Socioeconomic Pathways SSP5-8.5) to that resulting from a medium-tier emission scenario (SSP2-4.5). These simulations aim to analyze the response of climate models to a reduction in incoming surface radiation as a means to reduce global surface temperatures, and they do so either by simulating a stratospheric sulfate aerosol layer or, in a more idealized way, through a uniform reduction in the solar constant in the model. We find that over the final two decades of this century there are considerable inter-model spreads in the needed injection amounts of sulfate (29 ± 9 Tg-SO 2 /yr between 2081 and 2100), in the latitudinal distribution of the aerosol cloud and in the stratospheric temperature changes resulting from the added aerosol layer. Even in the simpler G6solar experiment, there is a spread in the needed solar dimming to achieve the same global temperature target (1.91 ± 0.44 %). The analyzed models already show significant differences in the response to the increasing CO 2 concentrations for global mean temperatures and global mean precipitation (2.05 K ± 0.42 K and 2.28 ± 0.80 %, respectively, for SSP5-8.5 minus SSP2-4.5 averaged over 2081–2100). With aerosol injection, the differences in how the aerosols spread further change some of the underlying uncertainties, such as the global mean precipitation response (–3.79 ± 0.76 % for G6sulfur compared to –2.07 ± 0.40 % for G6solar against SSP2-4.5 between 2081 and 2100). These differences in the behavior of the aerosols also result in a larger uncertainty in the regional surface temperature response among models in the case of the G6sulfur simulations, suggesting the need to devise various, more specific experiments to single out and resolve particular sources of uncertainty. The spread in the modeled response suggests that a degree of caution is necessary when using these results for assessing specific impacts of geoengineering in various aspects of the Earth system. However, all models agree that compared to a scenario with unmitigated warming, stratospheric aerosol geoengineering has the potential to both globally and locally reduce the increase in surface temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46°C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

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

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Contrasting aerosol effects on longwave cloud forcing in South East Asia and Amazon simulated with Community Atmosphere Model version 5.3

Aerosols modify cloud microphysical and radiative properties and thus impact the shortwave (SW) and longwave cloud forcing (LWCF). This study first reports the finding of contrasting aerosol effects on LWCF in South East Asia and Amazon in the Community Atmosphere Model version 5.3 (CAM5.3), which corresponds to the sum of LW indirect and semi-direct effects investigated in Ghan et al., (2012). A series of numerical experiments is conducted to decompose the complex aerosol effects on LWCF. Our analysis indicates that the cooling (negative aerosol effects on LWCF) in Amazon is due mainly to the aerosol effects on warm clouds and the inhibition of vertical motion by the aerosol-induced radiative cooling. In contrast, the warming (positive aerosol effects on LWCF) in South East Asia is due mainly to the aerosol effect on homogeneous freezing, thus reducing the ice particle size and prolonging the existence of ice cloud. Our results emphasize that a comprehensive analysis of integrated aerosol effects on both warm and ice clouds is necessary for better understanding the aerosol effects on LWCF.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Shortened Duration of Global Warming Slowdowns with Elevated Greenhouse Gas Emissions

Continuous emissions of anthropogenic greenhouse gases (GHGs) and aerosols in the last 160 years have resulted in an increasing trend of global mean surface temperatures (GMSTs). Due to interactions with natural variability, rates of the combined anthropogenically and naturally induced warming trends are characterized by significant slowdowns and speedups on decadal timescales. In this work, by analyzing observed and model-simulated data, we investigate how the duration of these episodes will change with different strengths of GHG and aerosol forcing. We found that the duration of warming slowdowns can be more than 30 yr with a slower rate of anthropogenic emissions but would shorten to about 5 yr with a higher one. This duration reduction depends on both the magnitude of the climate response to anthropogenic forcing and the strength of the internal variability. Moreover, the warming slowdowns can still occur even towards the end of this century under high emissions scenarios but with significantly shortened duration.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Contrasting Stratospheric Smoke Mass and Lifetime From 2017 Canadian and 2019/2020 Australian Megafires: Global Simulations and Satellite Observations

Stratospheric injections of carbonaceous aerosols and combustion gases by extreme wildfires have become increasingly common. Recent “megafires,” particularly large and intense fires, delivered particulate burdens to the lower stratosphere comparable to those of moderate volcanic eruptions. The 2017 Canadian megafire generated four large Pyrocumulonimbi (pyroCbs), injecting up to ≈0.3 Tg of smoke in the lower stratosphere. Even more extreme, the 2019/2020 Australian event produced a pyroCb activity resulting in stratospheric smoke intrusions of ≈1 Tg. To understand their contrasting behavior, we present global climate simulations of the atmospheric response to these events, applying smoke burdens informed by remote observations. Model outcomes, compared to satellite data of smoke transport, reproduce reasonably well the initial plume rise, at 0.2–0.3 km/day, attaining heights of ≈20 km in Canada and above 30 km in Australia. Global dispersal of the plume occurs within about 3 weeks in both cases, consistent with observations. Smoke removal timescales, ≈5 months for the Canadian megafire, agree with remote measurements. During the Australian megafire, observations indicate stratospheric injections three times as large, and models predict comparatively longer smoke lifetimes, ≈16 months. After the latter event, atmospheric optical depths and radiative cooling achieved values close to those measured following the Pinatubo eruption. Sensitivity tests of model assumptions indicate, in accord with prior studies, that smoke burden, injection heights, and black carbon content can determine plume evolution and possible climate impacts. An empirical relation between peak heights of stratospheric plumes and lifetimes is derived that can help assess megafire impacts on the stratosphere, climate and the Earth system

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Cloud condensation nuclei concentrations derived from the CAMS reanalysis

Determining number concentrations of cloud condensation nuclei (CCN) is one of the first steps in the chain in analysis of cloud droplet formation, the direct microphysical link between aerosols and cloud droplets, and a process key for aerosol–cloud interactions (ACI). However, due to sparse coverage of in situ measurements and difficulties associated with retrievals from satellites, a global exploration of their magnitude, source as well as temporal and spatial distribution cannot be easily obtained. Thus, a better representation of CCN numbers is one of the goals for quantifying ACI processes and achieving uncertainty-reduced estimates of their associated radiative forcing. Here, we introduce a new CCN dataset which is derived based on aerosol mass mixing ratios from the latest Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA) in a diagnostic model that uses CAMSRA aerosol properties and a simplified kappa-Köhler framework suitable for global models. The emitted aerosols in CAMSRA are not only based on input from emission inventories using aerosol observations, they also have a strong tie to satellite-retrieved aerosol optical depth (AOD) as this is assimilated as a constraining factor in the reanalysis. Furthermore, the reanalysis interpolates for cases of poor or missing retrievals and thus allows for a full spatiotemporal quantification of CCN numbers. The derived CCN dataset captures the general trend and spatial and temporal distribution of total CCN number concentrations and CCN from different aerosol species. A brief evaluation with ground-based in situ measurements demonstrates the improvement of the modelled CCN over the sole use of AOD as a proxy for CCN as the overall correlation coefficient improved from 0.37 to 0.71. However, we find the modelled CCN from CAMSRA to be generally high biased and find a particular erroneous overestimation at one heavily polluted site which emphasises the need for further validation. The CCN dataset (https://doi.org/10.26050/WDCC/QUAERERE_CCNCAMS_v1, Block, 2023), which is now freely available to users, features 3-D CCN number concentrations of global coverage for various supersaturations and aerosol species covering the years 2003–2021 with daily frequency. This dataset is one of its kind as it offers lots of opportunities to be used for evaluation in models and in ACI studies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

The Fall and Rise of the Global Climate Model

Abstract Global models are an essential tool for climate projections, but conventional coarse‐resolution atmospheric general circulation models suffer from errors both in their parameterized cloud physics and in their representation of climatically important circulation features. A notable recent study by Terai et al. (2020, https://doi.org/10.1029/2020ms002274) documents a global model capable of reproducing the regime‐based effect of aerosols on cloud liquid water path expected from observational evidence. This may represent a significant advance in cloud process fidelity in global models. Such models can be expected to give a better estimate of the effective radiative forcing of the climate. If this advance in cloud process representation can be matched by advances in the representation of circulation features such as monsoons, then such models may also be able to navigate the complex tangle between spatially heterogeneous aerosol–cloud interactions and regional circulation patterns. This tight link between aerosol and circulation results in anthropogenic perturbations of climate variables of societal importance, such as regional rainfall distributions. Upcoming global models with km‐scale resolution may improve the regional circulation and be able to take advantage of the Terai et al. (2020, https://doi.org/10.1029/2020ms002274) improvement in cloud physics. If so, an era of significantly improved regional climate projection capabilities may soon dawn. If not, then the improvement in cloud physics might spur intensified efforts on problems in model dynamics. Either way, based on the rapid changes in aerosol emissions in the near future, learning to make reliable projections based on biased models is a skill that will not go out of style.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Characterizing the Atmospheric Mn Cycle and Its Impact on Terrestrial Biogeochemistry

Abstract The role of manganese (Mn) in ecosystem carbon (C) biogeochemical cycling is gaining increasing attention. While soil Mn is mainly derived from bedrock, atmospheric deposition could be a major source of Mn to surface soils, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g., industrialization and land‐use change due to agriculture), transport, and deposition, remains uncertain. Here, we use compiled emission data sets for each identified source to model and quantify the atmospheric Mn cycle by combining an atmospheric model and in situ atmospheric concentration measurements. We estimated global emissions of atmospheric Mn in aerosols (<10 μm in aerodynamic diameter) to be 1,400 Gg Mn year −1 . Approximately 31% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened Mn “pseudo” turnover times in 1‐m‐thick surface soils (ranging from 1,000 to over 10,000,000 years) by 1–2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn‐to‐N ratio of the atmospheric deposition in non‐desert dominated regions (between 5 × 10 −5 and 0.02) across industrialized areas, but that was still lower than soil Mn‐to‐N ratio by 1–3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, consisting with atmospheric Mn deposition enhancing carbon respiration as seen in in situ biogeochemical studies.

Environmental Sciences & Ecology↗
DOE OSTI2023

Distinct regional meteorological influences on low-cloud albedo susceptibility over global marine stratocumulus regions

Abstract. Marine stratocumuli cool the Earth effectively due to their high reflectance of incoming solar radiation and persistent occurrence. The susceptibility of cloud albedo to droplet number concentration perturbations depends strongly on large-scale meteorological conditions. Studies focused on the meteorological dependence of cloud adjustments often overlook the covariability among meteorological factors and their geographical and temporal variability. We use 8 years of satellite observations sorted by day and geographical location to show the global distribution of marine low-cloud albedo susceptibility. We find an overall cloud brightening potential for most marine warm clouds, which is more pronounced over subtropical coastal regions. A weak cloud darkening potential in the annual mean is evident over the remote SE Pacific and SE Atlantic. We show that large-scale meteorological fields from the ERA5 reanalysis data, including lower-tropospheric stability, free-tropospheric relative humidity, sea surface temperature, and boundary layer depth, have distinct covariabilities over each of the eastern subtropical ocean basins where marine stratocumuli prevail. This leads to a markedly different annual cycle in albedo susceptibility over each basin. Moreover, we find that basin-specific regional relationships between key meteorological factors and albedo susceptibilities are absent in a global analysis. Our results stress the importance of considering the geographical distinctiveness of temporal meteorological covariability when scaling up the local-to-global response of cloud albedo to aerosol perturbations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Large spatiotemporal variability in aerosol properties over central Argentina during the CACTI field campaign

Abstract. Few field campaigns with extensive aerosol measurements have been conducted over continental areas in the Southern Hemisphere. To address this data gap and better understand the interactions of convective clouds and the surrounding environment, extensive in situ and remote sensing measurements were collected during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign conducted between October 2018 and April 2019 over the Sierras de Córdoba range of central Argentina. This study describes measurements of aerosol number, size, composition, mixing state, and cloud condensation nuclei (CCN) collected on the ground and from a research aircraft during 7 weeks of the campaign. Large spatial and multiday variations in aerosol number, size, composition, and CCN were observed due to transport from upwind sources controlled by mesoscale to synoptic-scale meteorological conditions. Large vertical wind shears, back trajectories, single-particle measurements, and chemical transport model predictions indicate that different types of emissions and source regions, including biogenic emissions and biomass burning from the Amazon and anthropogenic emissions from Chile and eastern Argentina, contribute to aerosols observed during CACTI. Repeated aircraft measurements near the boundary layer top reveal strong spatial and temporal variations in CCN and demonstrate that understanding the complex co-variability of aerosol properties and clouds is critical to quantify the impact of aerosol–cloud interactions. In addition to quantifying aerosol properties in this data-sparse region, these measurements will be valuable to evaluate predictions over the midlatitudes of South America and improve parameterized aerosol processes in local, regional, and global models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Satellite-based evaluation of AeroCom model bias in biomass burning regions

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by –93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

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

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

09 BIOMASS FUELS↗
DOE OSTI2023

Pluminate: Quantifying aerosol injection behavior from simulation, experimentation and observations

Marine aerosol injections are a key component in further understanding of both the potentials of deliberate injection for marine cloud brightening (MCB), a potential climate intervention (CI) strategy, and key aerosol-cloud interaction behaviors that currently form the largest uncertainty in global climate model (GCM) predictions of our climate. Since the rate of spread of aerosols in a marine environment directly translates to the effectiveness and ability of aerosol injections in impacting cloud radiative forcing, it is crucial to understand the spatial and temporal extent of injected-aerosol effects following direct injection into marine environments. The ubiquity of ship-injected aerosol tracks from satellite imagery renders observational validation of new parameterizations possible in 2D, however, 3D compatible data is more scarce, and necessary for the development of subgrid scale parameterizations of aerosol-cloud interactions in GCMs. This report introduces two novel parameterizations of atmospheric aerosol injection behavior suitable for both 3D (GCM-compatible) and 2D (observation-related) modeling. Their applicability is highlighted using a wealth of different observational data: small and larger scale salt-aerosol injection experiments conducted at SNL, 3D large eddy simulations of ship-injected aerosol tracks and 2D satellite images of ship tracks. The power of experimental data in enhancing knowledge of aerosol-cloud interactions is in particular emphasized by studying key aerosol microphysical and optical properties as observed through their mixing in cloud-like environments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

A Multivariate Space‐Time Dynamic Model for Characterizing the Atmospheric Impacts Following the Mt. Pinatubo Eruption

The June 1991 Mt. Pinatubo eruption resulted in a massive increase of sulfate aerosols in the atmosphere, absorbing radiation and leading to global changes in surface and stratospheric temperatures. A volcanic eruption of this magnitude serves as a natural analog for stratospheric aerosol injection, a proposed solar radiation modification method to combat a warming climate. The impacts of such an event are multifaceted and region-specific. Our goal is to characterize the multivariate and dynamic nature of the atmospheric impacts following the Mt. Pinatubo eruption. We developed a multivariate space-time dynamic linear model to understand the full extent of the spatially- and temporally-varying impacts. Specifically, spatial variation is modeled using a flexible set of basis functions for which the basis coefficients are allowed to vary in time through a vector autoregressive (VAR) structure. This novel model is cast in a Dynamic Linear Model (DLM) framework and estimated via a customized MCMC approach. We demonstrate how the model quantifies the relationships between key atmospheric parameters prior to and following the Mt. Pinatubo eruption with reanalysis data from MERRA-2 and highlight when such a model is advantageous over univariate models.

Dynamic Linear Model↗
DOE OSTI2020

Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

The southeast Atlantic is home to well-defined smoke outflow from Africa coinciding vertically with extensive marine boundary-layer cloud decks, both reaching their climatological maxima in spatial extent around September. A framework is put forth for evaluating the performance of a range of global and regional aerosol models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. The sparse airborne observations are first aggregated into 2o grid boxes and into three vertical layers: the cloud-topped marine boundary layer (MBL), the layer from cloud top to 3 km, and the 3-6 km layer. Aerosol extensive properties simulated for the entire study region for all September suggest that the 2016 ORACLES observations are reasonably representative of the regional monthly average, with systematic deviations of 30% or less. All six models typically place the bottom of the smoke layer at lower altitudes than do the airborne lidar observations by 300-1400 m, whereas model aerosol top heights are within 0-500 m of the observations. All but one of the models that report carbonaceous aerosol masses underestimate the ratio of particulate extinction to the masses, a proxy for mass extinction efficiency, in 3-6 km. Notable findings on individual models include that WRF-CAM5 predicts the mass of black carbon and organic aerosols with minor (~10% or less) biases. GEOS-5 overestimates the carbonaceous particle masses in the MBL by a factor of 3-6. Extinction coefficients in the free troposphere (FT) and above-cloud aerosol optical depth (ACAOD) are 10-30% lower in WRF-CAM5, 30-50% lower in GEOS-5, 10-40% higher in GEOS-Chem, 10-20% higher in EAM-E3SM except for the practically unbiased 3-6 km extinction, and 20-70% lower in the Unified Model, than the airborne in situ, lidar and sunphotometer measurements. ALADIN-Climate also underestimates the ACAOD, by 30%. GEOS-5 and GEOS-Chem predict carbon monoxide in the MBL with small (10% or less) negative biases, despite their overestimates of carbonaceous aerosol masses. Overall, this study highlights a new approach to utilizing airborne aerosol measurements for model diagnosis.

Shinozuka, Yohei↗
DOE OSTI2022

Fine Ash-Bearing Particles as a Major Aerosol Component in Biomass Burning Smoke

Biomass burning (BB) events are occurring globally with increasing frequency, and their emissions are having more impacts on human health and climate. Large ash particles are recognized as a BB product with major influences on soil and water environments. However, fine-ash particles, which have diameters smaller than several microns and characteristic morphologies and compositions (mainly Ca and Mg carbonates), have not yet been explicitly considered as a major BB aerosol component either in field observations or climate models. This study measured BB aerosol samples using transmission electron microscopy (TEM) and ion chromatography during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. We show that significant amounts of fine ash-bearing particles are transported >100 km from their fire sources. Our environmental chamber experiments suggest that they can act as cloud condensation and ice nuclei. We also found considerable amounts of fine ash-bearing particles in the TEM samples collected during previous campaigns (Biomass Burning Observation Project and Megacity Initiative: Local and Global Research Observations). These ash particles are commonly mixed with organic matter and make up ~8% and 5% of BB smoke by number and mass, respectively, in samples collected during the FIREX-AQ campaign. The measured ash-mass concentrations are approximately five times and six times greater than those of BB black carbon and potassium, respectively, scaling to an estimated global emission of 11.6 Tg yr -1 with a range of 8.8–16.3 Tg yr -1 . Better characterization and constraints on these fine ash-bearing particles will improve BB aerosol measurements and strengthen assessments of BB impacts on human health and climate.

54 ENVIRONMENTAL SCIENCES↗