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DOE OSTI2022

Discovering faint and high apparent motion rate near-Earth asteroids using a deep learning program

ABSTRACT Although many near-Earth objects have been found by ground-based telescopes, some fast-moving ones, especially those near detection limits, have been missed by observatories. We developed a convolutional neural network for detecting faint fast-moving near-Earth objects. It was trained with artificial streaks generated from simulations and was able to find these asteroid streaks with an accuracy of 98.7 per cent and a false positive rate of 0.02 per cent on simulated data. This program was used to search image data from the Zwicky Transient Facility (ZTF) in four nights in 2019, and it identified six previously undiscovered asteroids. The visual magnitudes of our detections range from ∼19.0 to 20.3 and motion rates range from ∼6.8 to 24 deg d−1, which is very faint compared to other ZTF detections moving at similar motion rates. Our asteroids are also ∼1–51 m diameter in size and ∼5–60 lunar distances away at close approach, assuming their albedo values follow the albedo distribution function of known asteroids. The use of a purely simulated data set to train our model enables the program to gain sensitivity in detecting faint and fast-moving objects while still being able to recover nearly all discoveries made by previously designed neural networks which used real detections to train neural networks. Our approach can be adopted by any observatory for detecting fast-moving asteroid streaks.

Wang, Franklin (ORCID:0000000344887355)↗

DOE OSTI2022

Uncertainty Quantification of Bifacial Performance Modeling

Analysis on uncertainty in the annual energy of PV systems that can be attributed to parameters of particular importance to bifacial PV modules is presented. Monte Carlo simulations are used to evaluate the effect of uncertain module bifaciality factors, module transmission fractions, albedo values, and ground clearance. The analyses cover a wide spectrum of potential PV array archetypes through variation of installation parameters. The results of the Monte Carlo analysis reveal that the uncertainty is largely dependent on albedo uncertainty, but more simulations are needed to identify trends across system archetypes. The simulations are aimed at attributing an annual energy uncertainty factor for bifacial considerations that can be applied in post-processing of project probability of exceedance analysis.

energy modeling↗

DOE OSTI2025

Combining Eddy Covariance Towers, Field Measurements, and the MEMS 2 Ecosystem Model Improves Confidence in the Climate Impacts of Bioenergy With Carbon Capture and Storage

ABSTRACT Carbon dioxide removal technologies such as bioenergy with carbon capture and storage (BECCS) are required if the effects of climate change are to be reversed over the next century. However, BECCS demands extensive land use change that may create positive or negative radiative forcing impacts upstream of the BECCS facility through changes to in situ greenhouse gas fluxes and land surface albedo. When quantifying these upstream climate impacts, even at a single site, different methods can give different estimates. Here we show how three common methods for estimating the net ecosystem carbon balance of bioenergy crops established on former grassland or former cropland can differ in their central estimates and uncertainty. We place these net ecosystem carbon balance forcings in the context of associated radiative forcings from changes to soil N 2 O and CH 4 fluxes, land surface albedo, embedded fossil fuel use, and geologically stored carbon. Results from long term eddy covariance measurements, a soil and plant carbon inventory, and the MEMS 2 process‐based ecosystem model all agree that establishing perennials such as switchgrass or mixed prairie on former cropland resulted in net negative radiative forcing (i.e., global cooling) of −26.5 to −39.6 fW m −2 over 100 years. Establishing these perennials on former grassland sites had similar climate mitigation impacts of −19.3 to −42.5 fW m −2 . However, the largest climate mitigation came from establishing corn for BECCS on former cropland or grassland, with radiative forcings from −38.4 to −50.5 fW m −2 , due to its higher plant productivity and therefore more geologically stored carbon. Our results highlight the strengths and limitations of each method for quantifying the field scale climate impacts of BECCS and show that utilizing multiple methods can increase confidence in the final radiative forcing estimates.

Falvo, Grant [Department of Plant, Soil and Microb↗

DOE OSTI2022

Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA)

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in-situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from June 21 to July 20, 2017 and January 15 to February 18, 2018 in the Azores. The flights were designed to maximize the synergy between in-situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Lastly, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

North Slope of Alaska Black Carbon Loadings and Mixing State for MOSAiC Field Campaign Report

The Arctic represents a unique region to study global climate change in that it exhibits pronounced sensitivity towards aerosol radiative forcing, referred to as arctic amplification. Of the aerosol species that are expected to contribute to this aerosol forcing, black carbon (BC) is arguably at the top of the list. Black carbon has this distinction because it exerts two radiative forcing influences that can be characterized as atmospheric and non-atmospheric. As an atmospheric forcer, BC behaves much as it does in the mid-latitudes – through the direct effect and semi-direct effects – collectively causing surface dimming with subsequent surface cooling and mid-altitude warming affecting cloud cover. As a terrestrial forcer, which is unique to the cryosphere, the deposition of BC on the surface can readily decrease polar surface albedo that, in turn, can activate a positive feedback wherein the increased surface absorption leads to further snow melt causing still further reduction in surface albedo.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Volumetrically Absorbing Thermal Insulator (VATI) for High-temperature Receivers

This project seeks to exploit volumetric absorption of concentrated solar irradiation in a thin, high-temperature, thermally conductive medium. High efficiency thermal conversion is achieved by volumetric absorption of both incoming solar irradiation (short wavelength) and emitted irradiation (long wavelength), demonstrating a volumetrically absorbing thermally insulating (VATI) effect. The thermalized energy is conducted to the back wall, enclosing the working fluid (molten salt or supercritical CO 2 ). Reliance on conductive thermal transport requires a thermally conductive medium, in the absence of which large temperature gradients drive losses due to emission. The project’s outcomes are important to realize a cost-effective approach to reduce optical and thermal losses from CSP receivers at high temperatures (720°C). High-temperature stable and commercially available porous SiC structures (open-cell foams) were explored as a volumetrically absorbing and thermally insulating layer. To the best of our knowledge, the current state-of-the-art for industrially deployed coatings is Pyromark. However, Pyromark suffers degradation at 700+°C and diurnal temperature changes. This necessitates periodic recoating, and the downtime increases the overall levelized cost of energy (LCOE) production. On the other hand, contemporary research activities have generated significant advances in the development of selective emitter coatings, which present challenges with costs, scalability, and stability. The pursued approach alleviates these concerns by developing a receiver that utilizes the inherent structure of high-temperature stable porous materials to enable robust and cost-effective receivers which require no periodic maintenance downtimes. The overall goal of the project is to experimentally demonstrate a figure of merit (FOM) of 0.92 at a temperature of 720°C and solar irradiation of 1000x concentration with porous receivers. The relevant crystallographic (phase) optical and thermal properties of porous SiC were first characterized. Second, the 3-D geometry of the porous SiC was analyzed using micro-X-ray tomography and converted to CAD data using image processing analysis. Utilizing this 3-D geometry and relevant optical/thermal properties, Monte Carlo- Ray Tracing (MCRT) analysis was performed to extract important parameters governing solar-thermal energy conversion such as extinction coefficient (β, 1/m), scattering albedo (ω) and the scattering phase function (Φ). These properties were then integrated into an in-house radiative and conduction transport model to solve for temperature and transport fluxes characterizing the solar-thermal energy conversion. This model was utilized to predict the FOM for various SiC porous geometries and to identify the highest possible FOM. Testing of the optimized porous structures will be accomplished with a custom-built high-accuracy (< ±4%) FOM measurement test-stand and a 1000x solar concentrator. When neglecting convective losses and resistance at the open boundary and the back wall, the optimized SiC foam leads to a FOM of 0.84. This FOM does not surpass the performance of Pyromark 2500. Yet, conversely to Pyromark 2500, SiC is stable at high temperatures and does not degrade over time. Also, it is possible to boost the FOM of SiC by engineering its effective thermal conductivity and its scattering albedo. A FOM of 0.92 is predicted for an optimized foam by accounting for convective losses and resistance at the open boundary and the back wall. This largely exceeds the FOM of Pyromark 2500 (~0.86) predicted by neglecting convective losses and resistance. Therefore, further engineering of the foam could lead to unprecedented FOMs.

14 SOLAR ENERGY↗

DOE OSTI2023

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. 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/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Monolithic Bifacial Halide Perovskite-Cadmium Selenide Telluride (CST) Tandem Thin-Film Solar Cells (Final Technical Report)

In this project, we develop a bifacial tandem design for monolithic metal halide perovskite-cadmium selenide telluride (CST) tandem solar cells. The bifacial tandem design not only enables the monolithic integration of perovskite-CST tandems but also delivers high efficiency by harvesting the albedo light. It also allows better current match and thus enables higher power output of the tandem devices than conventional tandem cells. We worked on understanding the critical factors limiting bifacial CST cells and developing strategies to improve their bifaciality. We also developed efficient wide-bandgap perovskite subcells and interconnecting layers that enable the monolithic perovskite-CST tandem solar cells. We successfully demonstrated prototype monolithic bifacial perovskite-CST tandem solar cells with bifacial equivalent efficiencies of more than 25% under an albedo of 0.4. Additionally, we optimized the wide-bandgap perovskite to realize four-terminal perovskite-CST tandem devices with efficiencies of 25.5% under monofacial illumination. The team disseminated these results to stakeholders in the PV academic and industry and discussed the challenges and major technical barriers for their market entry. The technologies developed in the project are promising but are not yet ready for immediate commercialization. Future fundamental study and R&D work are needed to advance these promising technologies.

14 SOLAR ENERGY↗

DOE OSTI2022

Combining Particle Tracking with Electromagnetic Radiation Showers: Merging GPT and Geant4 with Visualization

Field emitted electrons can seriously affect the operation of high-field, high-duty factor electron accelerators. Accelerated field emission can result in high average power beams which can radiation damage beamline components. In addition, localized losses generate thermal hot spots whose outgassing degrades the ultra-high vacuum required in photoinjectors and cryomodules. However, despite their importance, the effects of field emission are rarely included in the design and engineering of electron injectors. This work attempts to remedy this situation by combining two well-known and well-documented programs, GPT and Geant4, to track electrons and their losses in an injector beamline. This paper describes a system of programs which simulates electron paths and losses along the beamline. In addition, the tracking results can be zoomed and panned along and about the beampipe envelope using an open-source 3D CAD program. The scattering albedo calculations of the combined program, GPT-Geant4, are shown to be in good agreement with the literature albedos. The paper concludes with a dark current simulation for the LCLS-II injector from the cathode to the collimator at 1.5 m from the cathode.

Dowell, David H.↗

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 OSTI2020

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

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 OSTI2022

Quantifying the effects of mixing state on aerosol optical properties

Abstract. Calculations of the aerosol direct effect on climate rely on simulated aerosol fields. The model representation of aerosol mixing state potentially introduces large uncertainties into these calculations, since the simulated aerosol optical properties are sensitive to mixing state. In this study, we systematically quantified the impact of aerosol mixing state on aerosol optical properties using an ensemble of 1800 aerosol populations from particle-resolved simulations as a basis for Mie calculations for optical properties. Assuming the aerosol to be internally mixed within prescribed size bins caused overestimations of aerosol absorptivity and underestimations of aerosol scattering. Together, these led to errors in the populations' single scattering albedo of up to −22.3 % with a median of −0.9 %. The mixing state metric χ proved useful in relating errors in the volume absorption coefficient, the volume scattering coefficient and the single scattering albedo to the degree of internally mixing of the aerosol, with larger errors being associated with more external mixtures. At the same time, a range of errors existed for any given value of χ. We attributed this range to the extent to which the internal mixture assumption distorted the particles' black carbon content and the refractive index of the particle coatings. Both can vary for populations with the same value of χ. These results are further evidence of the important yet complicated role of mixing state in calculating aerosol optical properties.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Inferring the photolysis rate of NO 2 in the stratosphere based on satellite observations

NO and NO 2 (NO x ) play major roles in both tropospheric and stratospheric chemistry. This paper provides a novel method to obtain a global and accurate photolysis rate for NO 2 based on satellite data. The photolysis rate J(NO 2 ) dominates the daytime diurnal variation of NO x photochemistry. Here the spatial variation of J(NO 2 ) at 50–90°S in December from 20–40km is obtained using data from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) experiment. Because NO and NO 2 rapidly exchange with one another in the daytime, J(NO 2 ) can be attained assuming steady state, and the results are shown to be consistent with model results. The J(NO 2 ) value decreases as the solar zenith angle increases and has a weak altitude dependence. A key finding is that satellite-derived J(NO 2 ) increases in the polar regions, in good agreement with model predictions, due to the effects of ice and snow on surface albedo. Thus, the method presented here provides an observation-based check on the role of albedo in driving polar photochemistry.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Natural marine cloud brightening in the Southern Ocean

Abstract. The number of cloud droplets per unit volume (Nd) is a fundamentally important property of marine boundary layer (MBL) liquid clouds that, at constant liquid water path, exerts considerable controls on albedo. Past work has shown that regional Nd has a direct correlation to marine primary productivity (PP) because of the role of seasonally varying, biogenically derived precursor gases in modulating secondary aerosol properties. These linkages are thought to be observable over the high-latitude oceans, where strong seasonal variability in aerosol and meteorology covary in mostly pristine environments. Here, we examine Nd variability derived from 5 years of MODIS Level 2-derived cloud properties in a broad region of the summer eastern Southern Ocean and adjacent marginal seas. We demonstrate latitudinal, longitudinal and temporal gradients in Nd that are strongly correlated with the passage of air masses over high-PP waters that are mostly concentrated along the Antarctic Shelf poleward of 60∘ S. We find that the albedo of MBL clouds in the latitudes south of 60∘ S is significantly higher than similar liquid water path (LWP) clouds north of this latitude.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

The diurnal susceptibility of subtropical clouds to aerosols

The diurnal susceptibility of clouds and their radiative properties to aerosols is examined during their Lagrangian transition from subtropical stratocumulus to shallow cumulus regimes. Using large-eddy simulations, we analyze the six-day evolution of an air mass along a 3800 km observed trajectory from the coast of Peru toward the equator. Pristine and polluted scenarios are simulated with forcing imposed from weather reanalysis. The polluted scenario exhibits stronger diurnal variations in cloud water, cloud fraction, and albedo, with enhanced nighttime entrainment and suppressed precipitation. The overall response of cloud properties and outgoing shortwave radiation to droplet number concentration follows a distinct diurnal pattern: strong positive cloud adjustments dominate at night and in the morning, while weak negative adjustments prevail in the afternoon. This cycle is driven by the competition between precipitation suppression, which enhances cloud water and coverage, and entrainment drying, which depletes them. In polluted conditions, enhanced entrainment leads to a deeper and more decoupled boundary layer that cannot be sustained by surface fluxes in the afternoon, resulting in negative cloud adjustments. The enhanced entrainment rate under polluted conditions is caused by the reduced sedimentation of cloud and precipitation water from the entrainment zone. While the Twomey effect dominates the diurnal average albedo response, the diurnal variation in the competing cloud adjustments lead to a near-neutral net susceptibility in the afternoon, highlighting the critical role of diurnally varying processes in aerosol-cloud interactions.

Geosciences↗

DOE OSTI2020

Global ocean dimethyl sulfide climatology estimated from observations and an artificial neural network

Marine dimethyl sulfide (DMS) is important to climate due to the ability of DMS to alter Earth's radiation budget. Knowledge of the global-scale distribution, seasonal variability, and sea-to-air flux of DMS is needed in order to improve understanding of atmospheric sulfur, aerosol/cloud dynamics, and albedo. Here we examine the use of an artificial neural network (ANN) to extrapolate available DMS measurements to the global ocean and produce a global climatology with monthly temporal resolution. A global database of 82 996 ship-based DMS measurements in surface waters was used along with a suite of environmental parameters consisting of latitude–longitude coordinates, time of day, time of year, solar radiation, mixed layer depth, sea surface temperature, salinity, nitrate, phosphate, and silicate. Linear regressions of DMS against the environmental parameters show that on a global-scale mixed layer depth and solar radiation are the strongest predictors of DMS. These parameters capture ~9 % and ~7 % of the raw DMS data variance, respectively. Multilinear regression can capture more of the raw data variance (~39 %) but strongly underestimates DMS in high-concentration regions. In contrast, the artificial neural network captures ~66 % of the raw data variance in our database. Like prior climatologies our results show a strong seasonal cycle in surface ocean DMS with the highest concentrations and sea-to-air fluxes in the high-latitude summertime oceans. We estimate a lower global sea-to-air DMS flux (20.12±0.43 Tg S yr –1 ) than the prior estimate based on a map interpolation method when the same gas transfer velocity parameterization is used. Our sensitivity test results show that DMS concentration does not change unidirectionally with each of the environmental parameters, which emphasizes the interactions among these parameters. The ANN model suggests that the flux of DMS from the ocean to the atmosphere will increase with global warming. Given that larger DMS fluxes induce greater cloud albedo, this corresponds to a negative climate feedback.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Uncertainty Quantification of Bifacial Performance Modeling

bifacial↗