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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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DOE OSTI2020

Radiative heating rate profiles over the southeast Atlantic Ocean during the 2016 and 2017 biomass burning seasons

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. Further uncertainties in the cloud structure arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean, where biomass burning aerosol is transported from the African continent. As the aerosol plume progresses across the southeast Atlantic Ocean, radiative heating within the aerosol layer has the potential to alter the thermodynamic environment and therefore the cloud structure; however, limited work has been done to quantify this along the trajectory of the aerosol plume in the region. The deployment of the first Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF1) in support of the Layered Atlantic Smoke Interactions with Clouds field campaign provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96° S, 14.35° W). Using observed profiles of temperature, humidity, and clouds from the field campaign alongside aerosol optical properties from Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), as input for the Rapid Radiation Transfer Model (RRTM), profiles of the radiative heating rate due to aerosols and clouds were computed. Radiative heating is also assessed across the southeast Atlantic Ocean using an ensemble of back trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. Idealized experiments using the RRTM with and without aerosols and a range of values for the single-scattering albedo (SSA) demonstrate that shortwave (SW) heating within the aerosol layer above Ascension Island can locally range between 2 and 8 K d -1 depending on the aerosol optical properties, though impacts of the aerosol can be felt elsewhere in the atmospheric column. When considered under clear conditions, the aerosol has a cooling effect at the TOA, and based on the observed cloud properties at Ascension Island, the cloud albedo is not large enough to overcome this. Shortwave radiative heating due to biomass burning aerosol is not balanced by additional longwave (LW) cooling, and the net radiative impact results in a stabilization of the lower troposphere. However, these results are extremely sensitive to the single-scattering albedo assumptions in models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

NeuralMie (v1.0): an aerosol optics emulator

The direct interactions of atmospheric aerosols with radiation significantly impact the Earth's climate and weather and are important to represent accurately in simulations of the atmosphere. This work introduces two contributions to enable a more accurate representation of aerosol optics in atmosphere models: (1) NeuralMie, a neural network Mie scattering emulator that can directly compute the bulk optical properties of a diverse range of aerosol populations and is appropriate for use in atmosphere simulations where aerosol optical properties are parameterized, and (2) TAMie, a fast Python-based Mie scattering code based on the Toon and Ackerman (1981) Mie scattering algorithm that can represent both homogeneous and coated particles. TAMie achieves speed and accuracy comparable to established Fortran Mie codes and is used to produce training data for NeuralMie. NeuralMie is highly flexible and can be used for a wide range of particle types, wavelengths, and mixing assumptions. It can represent core-shell scattering and, by directly estimating bulk optical properties, is more efficient than existing Mie code and Mie code emulators while incurring negligible error compared to existing aerosol optics parameterization schemes (0.08 % mean absolute percentage error).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

POPSnet-SGP: A Pilot Aerosol Microphysics Network for Targeting Climate Model Uncertainty Interim Field Campaign Report

Aerosols mediate the radiative fluxes in clear and cloudy skies and dominate the uncertainty in the radiative forcing of climate. Relatively dense networks of aerosol optical depth measurements have been used to effectively constrain simulated aerosol optical properties, but model diversity of aerosol microphysical properties is much larger (Mann et al. 2014, Myhre et al. 2009). A better understanding of aerosol microphysics is essential as they are the fundamental pieces of information required to convert aerosol emissions information to radiative and cloud-nucleating properties that drive radiative effects and forcing of climate. Model representation of aerosol microphysical properties has lagged in part due to their inherently greater spatial variability, but also due to a lack of available observations. This project – the Printed Optical Particle Spectrometer Network (POPSnet)-Southern Great Plains (SGP) Pilot – launched the first spatially dense network of aerosol size distribution measurements over an area the size of a global model grid cell and demonstrated its use in providing valuable information regarding the spatial variability of aerosol microphysical properties and its drivers for improving model constraints.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

Abstract. The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles is subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ∼10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth and its dependence on both size and RH.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

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aerosol optical properties for aoppsap1flynn1m.c1

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

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54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Aerosol and Cloud Optical Properties from the ARM Raman Lidars: The Feature Detection and Extinction (RLPROF-FEX) Value-Added Product

Aerosols and their interactions and influence on clouds are among the main sources of uncertainties in radiative direct and indirect forcing (IPCC 2013). Continuous height-resolved measurements of cloud and aerosol optical properties are needed to reduce these uncertainties. Here we describe the Raman Lidar Profiles – Feature detection and Extinction (RLPROF-FEX) Value-Added Product (VAP) derived using Raman lidar data at multiple U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility sites. RLPROF-FEX provides estimates of extinction, backscatter, and depolarization using the algorithm described by Thorsen et al. 2015 and Thorsen and Fu 2015. This document provides a description of the FEX algorithm, its input and output data, and related details about the Raman lidar (RL) system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of –0.2 and 1.5 W m –2 , respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Stratospheric aerosol forcing for CMIP7 – Part 1: optical properties for pre-industrial, historical, and scenario simulations

Stratospheric aerosols, most of which originate from explosive volcanic sulfur emissions into the stratosphere, are a key natural driver of climate variability. They are thus a forcing provided by the Coupled Model Intercomparison Project (CMIP) Climate Forcings Task Team to climate modelling groups participating in phase 7 of CMIP. For the historical period, we provide two datasets covering 1750–2023: (i) a volcanic upper tropospheric-stratospheric sulfur emission dataset, documented in a companion paper; and (ii) a stratospheric sulfate aerosol optical property dataset, documented in this paper. For the satellite era (from 1979 onwards), stratospheric aerosol optical properties are derived from the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) dataset. For the pre-satellite era (1750–1978), optical properties are derived from our volcanic SO 2 emission dataset using a new version of the reduced-complexity volcanic aerosol model Easy Volcanic Aerosol (Height) (EVA_H v2). A background, non-volcanic stratospheric aerosol climatology is derived from the 1998–2001 period with a trend over 1850–1978 accounting for increasing anthropogenic aerosols. A monthly stratospheric aerosol climatology is derived from the 1850–2021 average for both pre-industrial and scenario (future) simulations, with a 9-year ramp over 2022–2030 for scenario simulations to ensure a smooth transition from the historical period. CMIP7 simulations should use version 2.2.1 of our pre-industrial and historical datasets, and version 2.2.2 of our scenario dataset. Our methodology to produce historical aerosol optical properties significantly differs from CMIP6 for the pre-satellite era, and the resulting forcings in turn largely differ. In particular, the CMIP6 dataset was mostly based on the sparse and uncertain pyrheliometer record, which resulted in strongly underrepresented emissions from small-to-moderate magnitude eruptions. The resulting bias is addressed in CMIP7, which is entirely emission-derived in the pre-satellite era and uses more recent ice-core-based volcanic sulfur emission inventories than CMIP6. Our approach results in an overall larger volcanic aerosol forcing for CMIP7, with the 1850–2014 mean mid-visible global mean stratospheric aerosol optical depth (SAOD) in CMIP7 (0.0138) being 29 % higher than in CMIP6 (0.0107). The pre-industrial mean of the same variable is 26 % higher in CMIP7 (0.0135, derived from the historical 1850–2021) than CMIP6 (0.0107, derived from the historical 1850–2014 mean). Using a reduced-complexity climate model, we simulate a global mean surface temperature that is 0.07 °C colder for 1850–1900 when using the CMIP7 dataset instead of CMIP6, whereas 2000–2014 is 0.03 °C warmer in CMIP7. Our dataset also exhibits lower forcing for 1960–1980, resulting in temperatures 0.06 °C warmer when averaged over 1960–1990, a period for which CMIP6 climate models exhibit a cold bias. Given the large uncertainties characterizing the dataset, in particular for the pre-satellite era, we advise against treating the CMIP7 or CMIP6 dataset as uniquely superior for any specific year and highlight the need for further evaluation. We conclude the study by discussing sources of uncertainty for the dataset, future research avenues to improve it, as well as requirements to operationalize the production of the dataset, i.e. extend it and update it on an annual basis instead of every 5–7 years following CMIP cycles.

Aubry, Thomas J. [Univ. of Exeter, Devon (United K↗
DOE OSTI2023

Influence of NaCl concentration on the optical scattering properties of water-based aerosols

We present the characterization of several atmospheric aerosol analogs in a tabletop chamber and an analysis of how the concentration of NaCl present in these aerosols influences their bulk optical properties. Atmospheric aerosols (e.g., fog and haze) degrade optical signal via light–aerosol interactions causing scattering and absorption, which can be described by Mie theory. This attenuation is a function of the size distribution and number concentration of droplets in the light path. These properties are influenced by ambient conditions and the droplet’s composition, as described by Köhler theory. It is therefore possible to tune the wavelength-dependent bulk optical properties of an aerosol by controlling droplet composition. We present experimentation wherein we generated multiple microphysically and optically distinct atmospheric aerosol analogs using salt water solutions with varying concentrations of NaCl. The results demonstrate that changing the NaCl concentration has a clear and predictable impact on the microphysical and optical properties of the aerosol.

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

Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products

Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

Doppler lidar, aerosols, convection↗
DOE OSTI2023

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land-surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land-atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow-to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land-atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N

Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σ sp ) and light absorption coefficient (σ ap ) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80° N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4° N from near the surface to 50 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm -1 , which represent 98% of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m 2 g -1 , the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g -1 ) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σ ap 2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm -1 . The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Application of machine learning approaches in the analysis of mass absorption cross-section of black carbon aerosols: Aerosol composition dependencies and sensitivity analyses

Physics-based models typically require an in-depth understanding of a phenomenon and assumptions of the underlying process(es), which are often hard to obtain in practice, whereas data-driven machine learning models learn the structure and patterns in the training data without any prior theoretical assumptions and then use inference to develop useful predictions. A novel machine learning-based algorithm has been previously developed for the prediction of black carbon mass absorption cross-section (MAC BC ) and applied to a variety of different atmospheric environments. In contrast to light scattering theories which require assumptions about the underlying physics, this algorithm uses time-series data of aerosol properties to estimate the temporally-varying MAC BC at 870 nm. Here, we analyze our algorithm and discuss the influence of aerosol optical properties (such as Ångström exponents and single scattering albedo) and chemical composition on the model outputs and the associated accuracy. Additionally, we conduct sensitivity analyses on our models to understand how the predictions change in response to different sets of input variables. Our support vector machine (SVM) for regression model is the least sensitive to variations in the input variables, although all models tend to exhibit a degradation to their accuracy when scattering Ångström exponents are less than one.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Radiative impact of record-breaking wildfires from integrated ground-based data

The radiative effects of wildfires have been traditionally estimated by models using radiative transfer calculations. Assessment of model-predicted radiative effects commonly involves information on observation-based aerosol optical properties. However, lack or incompleteness of this information for dense plumes generated by intense wildfires reduces substantially the applicability of this assessment. Here we introduce a novel method that provides additional observational constraints for such assessments using widely available ground-based measurements of shortwave and spectrally resolved irradiances and aerosol optical depth (AOD) in the visible and near-infrared spectral ranges. We apply our method to quantify the radiative impact of the record-breaking wildfires that occurred in the Western US in September 2020. For our quantification we use integrated ground-based data collected at the Atmospheric Measurements Laboratory in Richland, Washington, USA with a location frequently downwind of wildfires in the Western US. We demonstrate that remarkably dense plumes generated by these wildfires strongly reduced the solar surface irradiance (up to 70% or 450 Wm -2 for total shortwave flux) and almost completely masked the sun from view due to extremely large AOD (above 10 at 500 nm wavelength). We also demonstrate that the plume-induced radiative impact is comparable in magnitude with those produced by a violent volcano eruption occurred in the Western US in 1980 and continental cumuli.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Wildland Urban Interface (WUI) Emissions: Laboratory Measurement of Aerosol and Trace Gas from Combustion of Manufactured Building Materials

Wildfires are increasing in intensity and more often threatening the wildland urban interface (WUI) where buildings and homes coexist with the natural environment. WUI emissions have not been as well-studied as emissions from vegetation. Thus, there is a need to quantify the emissions of building materials used in home construction under flaming and smoldering conditions to study their impacts to human health, visibility, air quality, and climate. Here, in a controlled laboratory setting, we quantify emissions of aerosols and trace gases including formaldehyde, particulate matter, and black carbon. We focus on the combustion of traditional single-source wood-based construction fuels. Our results indicate that, similar to natural fuels, the aerosol optical properties were more related to combustion conditions than the fuel type. Overall, we observed significant variability in the gas and particle emissions. Consistent trends include high formaldehyde (HCHO) and carbon monoxide (CO) emissions for smoldering conditions and higher carbon dioxide (CO 2 ), nitrogen oxides (NO x ), and black carbon for flaming conditions. Finally, these observations highlight the need to better characterize emissions for materials in the built environment to assess large-scale climate and human health impacts of fires at the WUI.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Connecting the Radiative Influences of Aerosol upon the Mass Flux Profiles of Shallow Cumuli across the Southeast Atlantic Ocean Basin and its Boundaries (Final Report)

The Atlantic Ocean covers approximately 25% of Earth’s surface and the atmosphere above it is home to a complex array of clouds and aerosols that have important influences on regional and global weather and climate. These influences must be accurately depicted in short range, medium range, seasonal, and climate forecast models. Conditions over the tropical Atlantic are particularly complex due to continental scale plumes of dust from the Sahara Desert and smoke from agricultural burning in Africa that drift across the Atlantic Ocean basin toward the Americas. These plumes are often found meandering in the lower atmosphere above shallow tropical clouds that form above the ocean surface, presumably mingling with these clouds on occasion due to convective mixing processes. Elevated dust and smoke particles absorb incoming sunlight and substantially warm the marine atmosphere in the layer in which they are present. This warming may alter the thermal stability of the marine atmosphere and may throttle or enhance the development of clouds, change their internal structure and the rate at which they precipitate. Alternatively, it may isolate the lower atmosphere from drier layers above enabling water vapor to accumulate near the ocean surface potentially leading to the development of deeper convection. Our study was organized around the principal concept of determining the impact of African smoke and dust plumes upon cloud development at ASI and understanding how a popular shallow convection parameterization used in models responds to the presence of this aerosol. We analyzed observations collected during the US Department of Energy (DOE) Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign using the Atmospheric Radiation Measurement Program’s Mobile Facility #1 (AMF-1), which was deployed to Ascension Island (ASI) in Southeastern Atlantic for a one-year period. Ascension Island is immediately downwind from an African source of these plumes, but far enough removed to enable the lower atmosphere to have reacted to their presence. A main goal of our study was to compute radiative heating rate profiles over Ascension Island and along the trajectory from the biomass burning regions along coastal Africa to Ascension Island. To compute the radiative heating rate due to aerosols and clouds, we employed observed profiles of temperature, humidity, and clouds from LASIC alongside aerosol optical properties from the Modern-era Retrospective analysis for Research and Applications Version 2 (MERRA-2), as input for the Rapid Radiation Transfer Model (RRTM). Radiative heating was also assessed across the southeast Atlantic Ocean using an ensemble of back trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. We were successful in this effort and the resulting publication is already being cited despite its relatively short lifetime in the literature. The second part of our study involved the process-level representation of the clouds observed over the Southeastern Atlantic in models. Our initial task, upon which the balance of this portion of the study depended, was to evaluate the representativeness of the clouds observed by AMF-1. What orographic influence did Ascension Island have on the measured cloud structure? We set out to answer this question by trying to separate observations that were clearly indicative of orographic forcing from those that were representative of open ocean. The siting of AMF-1, which was 340-m above sea-level on the slope of a steep escarpment, proved demonstrably problematic for cloud process measurements. Despite considerable effort using multiple approaches including artificial intelligence (AI), we were unable to successfully compensate for the orographic forcing present at the AMF-1 site on ASI and, hence, produce process-level summaries of the convective mass flux representative of open ocean over the Southeastern Atlantic. Even though the project has officially ended, we are making a final attempt using two new types of clustering algorithm (i.e., AI) on the recommendation of a former student, who is an expert in this area. Since we have only recently begun to test these new AI schemes, the recommendations from the second part of our project outlined below are based on our experience at the time of this report.

54 ENVIRONMENTAL SCIENCES↗