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DOE OSTI2024

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

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

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Nature-based climate solutions can help mitigate the radiative forcing that follows deforestation

Widespread expansion of agriculture and forestry has altered the surface of the Earth, the composition of the atmosphere, and as a result, the climate. Here we quantify the radiative forcing caused by the historical deforestation of an ecoregion in the U.S. Upper Midwest and the adoption of eight nature-based climate solutions. We combined regional forest inventory data with over three decades of remote sensing and in situ data from a replicated land use change experiment. Deforestation of the region caused net global warming (1626 ± 44 µW m -2 ), mainly from the 76 % reduction of ecosystem carbon stocks, but also from the 84 % reduction of the soil methane sink and the 115 % increase in soil nitrous oxide emissions. The associated albedo increase offset 24 % of this greenhouse gas induced warming. For the adoption of nature-based climate solutions, we found that conservation agriculture can provide -39 to -76 ± 31 µW m -2 of climate mitigation over a 100-year time period while short/medium length forestry rotations can provide more at -296 to -881 ± 44 µW m -2 and natural forest regeneration can provide the most at -1555 ± 44 µW m -2 . As the impacts of climate change on nature and society intensify, consideration should be given to the climate mitigation, habitat, and ecosystem services that nature-based climate solutions can provide.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Assessing Radiative Feedbacks and Their Contribution to the Arctic Amplification Measured by Various Metrics

Arctic amplification (AA), characterized by a more rapid surface air temperature (SAT) warming in the Arctic than the global average, is a major feature of global climate warming. Various metrics have been used to quantify AA based on SAT anomalies, trends, or variability, and they can yield quite different conclusions regarding the magnitude and temporal patterns of AA. This study examines and compares various AA metrics for their temporal consistency in the region north of 70°N from the early twentieth to the early 21st century using observational data and reanalysis products. We also quantify contributions of different radiative feedback mechanisms to AA based on short-term climate variability in reanalysis and model data using the Kernel-Gregory approach. Albedo and lapse rate feedbacks are positive and comparable, with albedo feedback being the leading contributor for all AA metrics. The net cloud feedback, which has large uncertainties, depends strongly on the data sets and AA metrics used. By quantifying the influence of internal variability on AA and related feedbacks based on global climate model ensemble simulations, we find that water vapor and cloud feedbacks are most heavily affected by internal variability.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Changes in Aerosols, Meteorology, and Radiation in the Southeastern U.S. Warming Hole Region during 2000 to 2019

Abstract Surface air temperatures in the southeastern United States that did not change from the climatological mean from 1900 to 2000 have increased since the year 2000. Analyzed herein are factors modulating the surface air temperatures in the region for a 20-yr period (2000–19) using space- and surface-based observations, and output from a reanalysis model. The 20-yr period is segregated into two decades, 2000–09 and 2010–19, corresponding to different tropospheric chemical regimes. Changes in seasonal and decadal averages are examined. The later decade experienced higher average surface air temperatures with significant warming during summer and fall seasons. Decadal and seasonal averages of cloud properties, column water vapor, rain rates, and top-of-atmosphere outgoing longwave radiation did not exhibit statistically significant differences between the two decades. The region experienced strong warm and moist advection during the winter months and very weak advection during the summer months. The later decade exhibited higher low-level moisture advection during the winter months than the earlier decade with insignificant changes in the temperature advection between the two decades. The later decade had significantly lower aerosol dry and liquid water mass during all seasons, along with lower aerosol optical depth, higher single scattering albedo, and lower top-of-the-atmosphere outgoing shortwave radiation during cloud-free conditions in the summer season. Collectively, these results suggest that changes in the aerosol direct radiative forcing are responsible for warming during summer months that experience weak advection and highlight seasonal differences in the temperature controlling mechanisms in the region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Light-absorbing impurities accelerating glacial melting in southeastern Tibetan Plateau

Deposition of light-absorbing particles on glacier surfaces poses a series of adverse impacts on the cryospheric environment, climate and human health. Broad attention of the scientific community has been paid on insoluble light-absorbing impurities (ILAIs) in snow and ice on glaciers over the Tibetan Plateau (TP). However, systematic investigation of ILAIs in snowpack of glaciers on the TP is scarce. In this study, the properties and darkening effect of ILAIs in snowpack on glaciers are extensively investigated in the southeast of TP. Results show that ILAIs concentrations in multiple types of snow and ice samples were significantly different. Snowpit depths varied substantially from one profile to another during May and June 2016. The average concentrations of ILAIs in snowpits increase as snow melting progresses. Black carbon (BC) and dust cause snow albedo reduction more in snow with larger grain size Re. Based on a radiative transfer model calculation, the average albedo reduction induced by BC in the snowpack was 0.141 ± 0.02, and associated daily maximum radiative forcing (RF) was 72.97 ± 12.7 W m-2. BC is a controlling light-absorbing factor in snowpack and causes substantial albedo reduction and thus the associated daily maximum RF. The maximum reduction of snow cover duration was 4.56 ± 0.71 days caused by BC and dust in snowpack in southeastern TP. The average mass absorption cross-section (MAC) of BC from multiple snowpits was 3.26 ± 0.46 m2 g-1, which represents a typical value of MAC in snow on glaciers, but it is type-dependent of snow/ice samples. Tropospheric aerosols vertically extended up to 8 km over the TP and its surrounding areas, which indicates the transport of aerosols from remote sources through elevated pathways. A large amount of carbon stored in the brittle glaciers can be potentially released with meltwater runoff under a warming climate. This study provides a new insight for investigating carbonaceous and light-absorbing particles in glacierization areas.

Niu, Hewen↗
DOE OSTI2026

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗
DOE OSTI2020

Dust dominates high-altitude snow darkening and melt over high-mountain Asia

Westerly-driven, long-range transportation of dust particles in elevated aerosol layers (EALs) is a persistent phenomenon during spring and summer over the Indian subcontinent. During the snow accumulation season, EALs transport substantial dust to the snow-covered slopes of high-mountain Asia (HMA). Here we use multiple satellite-based estimates to demonstrate a robust physical association between the EALs and dust-induced snow darkening over HMA. Results from a fully-coupled atmosphere-chemistry-snow model support these observations, revealing a signature of increasing dust-induced snow darkening with surface elevation over HMA that peaks near 4500 m. Moreover, the influence of dust on snow darkening is greater than that of black carbon above 4000 m. Our findings suggest a discernable role of dust in the observed spatial heterogeneity of snowmelt and snowline trends over HMA and highlight an increasing contribution of dust to snowmelt as the snowline rises with warming.

Elevated aerosol layers (EAL), Light absorbing par↗
DOE OSTI2021

Contrasting characteristics of open- and closed-cellular stratocumulus cloud in the eastern North Atlantic

Abstract. Extensive regions of marine boundary layer cloud impact the radiative balance through their significant shortwave albedo while having little impact on outgoing longwave radiation. Despite this importance, these cloud systems remain poorly represented in large-scale models due to difficulty in representing the processes that drive their life cycle and coverage. In particular, the mesoscale organization and cellular structure of marine boundary clouds have important implications for the subsequent cloud feedbacks. In this study, we use long-term (2013–2018) observations from the Atmospheric Radiation Measurement (ARM) Facility's Eastern North Atlantic (ENA) site on Graciosa Island, Azores, Portugal, to identify cloud cases with open- or closed-cellular organization. More than 500 h of each organization type are identified. The ARM observations are combined with reanalysis and satellite products to quantify the cloud, precipitation, aerosol, thermodynamic, and large-scale synoptic characteristics associated with these cloud types. Our analysis shows that both cloud organization populations occur during similar sea surface temperature conditions, but the open-cell cases are distinguished by stronger cold-air advection and large-scale subsidence compared to the closed-cell cases, consistent with their formation during cold-air outbreaks. We also find that the open-cell cases were associated with deeper boundary layers, stronger low-level winds, and higher rain rates compared to their closed-cell counterparts. Finally, raindrops with diameters larger than 1 mm were routinely recorded at the surface during both populations, with a higher number of large drops during the open-cellular cases. The similarities and differences noted herein provide important insights into the environmental and cloud characteristics during varying marine boundary layer cloud mesoscale organization and will be useful for the evaluation of model simulations for ENA marine clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Sensitivity of surface temperature to oceanic forcing via q-Flux Green’s function experiments. Part III: asymmetric response to warming and cooling

Climate response is often assumed to be linear in climate sensitivity studies. However, by examining the surface temperature (TS) response to pairs of oceanic forcings of equal amplitude but opposite sign in a large set of local q-flux perturbation experiments with CAM5 coupled to a slab, we find strong asymmetry in TS responses to the heating and cooling forcings, indicating a strong nonlinearity intrinsic to the climate system examined. Regardless of where the symmetric forcing is placed, the cooling response to the negative forcing always exceeds the warming to the positive forcing, implying an intrinsic inclination towards cooling of our current climate. Thus, the ongoing global warming induced by increasing greenhouse gases may have already been alleviated by the asymmetric component of the response. The common asymmetry in TS response peaks in high latitudes, especially along sea ice edges, with notable seasonal dependence. Decomposition into different radiative feedbacks through a radiative kernel indicates that the asymmetry in the TS response is realized largely through lapse rate and albedo feedbacks. Further process interference experiments disabling the seasonal cycle and/or sea ice reveal that the asymmetry originates ultimately from the presence of the sea ice component and is further amplified by the seasonal cycle. The fact that a pair of opposite tropical q-flux forcings can excite very similar asymmetric response as a pair placed at 55°S strongly suggests the asymmetric response is a manifestation of an internal mode of the climate model system.

Liu, Fukai↗
DOE OSTI2023

Vertical Structure and Ice Production Processes of Shallow Convective Postfrontal Clouds over the Southern Ocean in MARCUS. Part I: Observational Study

A study of the vertical structure of postfrontal shallow clouds in the marine boundary layer over the Southern Ocean is presented here. The central question of this two-part study regards cloud phase (liquid/ice) of precipitation, and the associated growth mechanisms. In this first part, data from the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) field campaign are analyzed, starting with a 75-h case with continuous sea surface-based thermal instability, modest surface heat fluxes, an open-cellular mesoscale organization, and very few ice nucleating particles (INPs). The clouds are mostly precipitating and shallow (tops mostly around 2 km above sea level), with weak up- and downdrafts, and with cloud-top temperatures generally around –18° to –10°C. Further, the case study is extended to three other periods of postfrontal shallow clouds in MARCUS. While abundant supercooled liquid water is commonly present, an experimental cloud-phase algorithm classifies nearly two-thirds of clouds in the 0° to –5°C layer as containing ice (cloud ice, snow, or mixed phase), implying that much of the precipitation grows through cold-cloud processes. The best predictors of ice presence are cloud-top temperature, cloud depth, and INP concentration. Measures of convective activity and turbulence are found to be poor indicators of ice presence in the studied environment. The water-phase distribution in this cloud regime is explored through numerical simulations in Part II. Significance Statement: Climate models generally predict a lower albedo than observed over the Southern Ocean, and this is largely attributed to a lack of cloudiness, especially in the postfrontal cold sector of midlatitude cyclones. This in turn may be due to an excess of ice in these simulated clouds, resulting in rapid precipitation fallout and an overly brief cloud lifespan. The objective of this study is to examine whether shallow postfrontal clouds over the Southern Ocean are dominated by supercooled drops, or by snow and ice, using data collected by a U.S. Department of Energy Atmospheric Radiation Measurement Mobile Facility deployed aboard an Australian Antarctic supply vessel. We find that these clouds contain much supercooled liquid, even though cloud-top temperatures generally are around –18° to –8°C, and that about two-thirds of the clouds just above the freezing level contain ice. Much of the precipitation appears to grow through cold-cloud processes above the freezing level, rather than drizzle/rain. Updrafts and/or turbulence in convection or in cloud-top generating cells do not initiate much ice, compared to observations elsewhere in a similar temperature range. This may be attributable to the extremely low concentration of ice nucleating particles in this environment. Ultimately, the deepest clouds with the coldest cloud tops are most likely to be ice dominated.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Albedo susceptibility of northeastern Pacific stratocumulus: the role of covarying meteorological conditions

Abstract. Quantification of the radiative adjustment of marine low clouds to aerosol perturbations, regionally and globally, remains the largest source of uncertainty in assessing current and future climate. One of the important steps towards quantifying the role of aerosol in modifying cloud radiative properties is to quantify the susceptibility of cloud albedo and liquid water path (LWP) to perturbations in cloud droplet number concentration (Nd). We use 10 years of spaceborne observations from the polar-orbiting Aqua satellite to quantify the albedo susceptibility of marine low clouds to Nd perturbations over the northeast (NE) Pacific stratocumulus (Sc) region. Mutual information analysis reveals a dominating control of cloud state (e.g., LWP and Nd) on low-cloud albedo susceptibility, relative to the meteorological states that drive these cloud states. Through a LWP–Nd space decomposition of albedo susceptibilities, we show clear separation among susceptibility regimes (brightening or darkening), consistent with previously established mechanisms through which aerosol modulates cloud properties. These regimes include (i) thin non-precipitating clouds (LWP < 55 g m−2) that exhibit brightening (occurring 37 % of the time), corresponding to the Twomey effect; (ii) thicker non-precipitating clouds, corresponding to entrainment-driven negative LWP adjustments that manifest as a darkening regime (36 % of the time); and (iii) another brightening regime (22 % of the time) consisting of mostly precipitating clouds, corresponding to precipitation-suppression LWP positive adjustments. Overall, we find an annual-mean regional low-cloud brightening potential of 20.8±2.68 W m−2 ln(Nd)−1, despite an overall negative LWP adjustment for non-precipitating marine stratocumulus, owing to the high occurrence of the Twomey–brightening regime. Over the NE Pacific, clear seasonal covariabilities among meteorological factors related to the large-scale circulation are found to play an important role in grouping conditions favorable for each susceptibility regime. When considering the covarying meteorological conditions, our results indicate that for the northeastern Pacific stratocumulus, clouds that exhibit the strongest brightening potential occur most frequently within shallow marine boundary layers over a cool ocean surface with a stable atmosphere and a dry free troposphere above. Clouds that exhibit a darkening potential associated with negative LWP adjustments occur most frequently within deep marine boundary layers in which the atmospheric instability and the ocean surface are not strong and warm enough to produce frequent precipitation. Cloud brightening associated with warm-rain suppression is found to preferably occur either under unstable atmospheric conditions or humid free-tropospheric conditions that co-occur with a warm ocean surface.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Evaluation and improvement of the parameterization of aerosol hygroscopicity in global climate models using in-situ surface measurements (Final Report)

Aerosols are tiny particles suspended on the atmosphere that can interact with incoming solar radiation and affect the Earth radiative budget. They do so by scattering and absorbing solar radiation, and these properties vary depending on the aerosol size and chemical composition. Moreover, by taking up water from the surrounding air, hygroscopic aerosol particles will grow in size and change their chemical composition, thus modifying their optical properties (scattering and absorption) and their final impact on radiative forcing calculations. An accurate knowledge of aerosol hygroscopicity is crucial for estimating the net radiative impact of aerosols. We took a three-pronged approach to improve our understanding of aerosol hygroscopicity and how it is implemented in Earth system models. In the first part of our project, we developed a benchmark dataset from existing aerosol hygroscopic growth measurements made by tandem nephelometer humidogram systems. We analyzed, using a standardized methodology, observations from 26 in-situ stations around the globe. Measurement data was collected from multiple data providers, reviewed and harmonized to create a consistent dataset of the scattering enhancement factor due to aerosol water uptake. This dataset is archived in several publicly available databases for use by interested researchers. In the second part of the project, we used the benchmark hygroscopicity dataset to perform a global study on aerosol hygroscopicity and aerosol optical properties. Measurements show a global picture of scattering enhancement with larger values for Arctic and marine sites and lower for urban and desert sites. We assessed the RH dependence of aerosol radiative forcing and showed that the overall effect of aerosol hygroscopicity on DARF is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 compared to dry conditions (RH<40%). Finally, we explored using aerosol single scattering albedo (SSA) and scattering Angstrom exponent (SAE) as possible proxies for aerosol hygroscopicity. SSA showed more promise as a surrogate for the scattering enhancement factor than SAE, but neither was ideal. In the third part of the project we evaluated the output of ten Earth system models (ESMs) against the benchmark hygroscopicity dataset. ESMs utilize various schemes for aerosol hygroscopicity which had not been previously tested against observations on a global scale. We found that ESMs currently overestimate scattering enhancement due to hygroscopic growth. Model parameterizations of hygroscopicity and model chemistry are two main factors driving the observed diversity in hygroscopicity simulations among the models. In addition, our study makes several suggestions for modelers, including improving the parameterizations of organic and sea salt aerosol hygroscopicity. Future hygroscopicity model evaluation experiments should include the model data related to particles size which was not available for our study.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Perovskite Solar Cells Go Bifacial—Mutual Benefits for Efficiency and Durability

Bifacial solar cells hold the potential to achieve a higher power output per unit area than conventional monofacial devices without significantly increasing manufacturing costs. However, efficient bifacial designs are challenging to implement in inorganic thin-film solar cells because of their short carrier lifetimes and high rear surface recombination. The emergence of perovskite photovoltaic (PV) technology creates a golden opportunity to realize efficient bifacial thin-film solar cells, owing to their outstanding optoelectronic properties and unique features of device physics. More importantly, transparent conducting oxide electrodes can prevent electrode corrosion by halide ions, mitigating one major instability issue of the perovskite devices. Here, the theory of bifacial PV devices is summarized and the advantages of bifacial perovskite solar cells, such as high power output, enhanced device durability, and low economic and environmental costs, are reviewed. The limitations and challenges for bifacial perovskite solar cells are also discussed. Lastly, the awareness of bifacial solar cells as a feasible commercialization pathway of perovskite PV for mainstream solar power generation and building-integrated PV is advocated and future research directions are suggested.

14 SOLAR ENERGY↗
DOE OSTI2022

Brown Carbon Fuel and Emission Source Attributions to Global Snow Darkening Effect

Snow and ice albedo reduction due to deposition of absorbing particles (i.e., snow darkening effect (SDE)) warms the Earth system and is largely attributed to black carbon (BC) and dust. Absorbing organic aerosol (BrC) also contributes to SDE but has received less attention due to uncertainty and challenges in model representation. This work incorporates the SDE of absorbing organic aerosol (BrC) from biomass burning and biofuel sources into the Snow Ice and Aerosol Radiative (SNICAR) model within a variant of the Community Earth System Model (CESM). Additionally, 12 different emission regions of BrC and BC from biomass burning and biofuel sources are tagged to quantify the relative contribution to global and regional SDE. BrC global SDE (0.021–0.056 Wm -2 ) is larger than other model estimates, corresponding to 37%–98% of the SDE from BC. When compared to observations, BrC simulations have a range in median bias (-2.5% to +21%), with better agreement in the simulations that include BrC photochemical bleaching. The largest relative contributions to global BrC SDE are traced to Northern Asia (23%–31%), Southeast Asia (16%–21%), and South Africa (13%–17%). Transport from Southeast Asia contributes nearly half of the regional BrC SDE in Antarctica (0.084–0.3 Wm -2 ), which is the largest regional input to global BrC SDE. Lower latitude BrC SDE is correlated with snowmelt, in-snow BrC concentrations, and snow cover fraction, while polar BrC SDE is correlated with surface insolation and snowmelt. This indicates the importance of in-snow processes and snow feedbacks on modeled BrC SDE.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Parallax-corrected VISST-derived pixel-level products from satellite GOES-16

The NASA Langley group led by William Smith produced GOES-16 satellite cloud retrievals over an approximate 10 by 10 degree region over the CACTI field campaign location. These retrievals are described here: https://www.arm.gov/capabilities/vaps/visst and are available for download here . They use algorithms historically called VISST that are now referred to as SatCORPS. More information can be found in Trepte et al. (2019), Minnis et al. (2021), and Yost et al. (2021). If using this dataset, please cite these references, the CACTI VISST dataset DOI found at the download link above, and this dataset’s DOI. The CACTI VISST pixel-level retrievals are on a 2 km spatial grid and available every 15 minutes (every 10 minutes late in the campaign), producing 21,765 files for the entire field campaign between October 2018 and April 2019. They are not corrected for parallax error, which is an offset in the actual geographical location of a cloud above the surface due to the satellite viewing the cloud partly from the side off nadir. This dataset applies a correction for parallax using the location relative to the satellite and the retrieved cloud top height above the surface, which allows the dataset to be geo-located with surface-based observations. The parallax correction for each location depends on the longitude, latitude and cloud top height above ground level (AGL) for that longitude and latitude in the original VISST files. The cloud top height AGL requires first computing the surface elevation at each VISST grid point. Data from the Advanced Spaceborne Thermal Emission and Reflection (ASTER) Global Digital Elevation Map Version 3 at 30-m resolution is projected onto the VISST grid using conservative coarsening (conserving surface elevation) in the xESMF Python package. The surface elevation is then subtracted from the VISST-retrieved cloud top height above mean sea level. These cloud top heights AGL are then combined with longitude and latitude to estimate the latitude and longitude corrections. Due to variability in cloud top height, the parallax shifts produce an irregular grid of values since higher cloud tops are shifted further than lower cloud tops. A ball tree-based neighbor search with Haversine distance is performed using the Python-based scikit-learn library to find the nearest VISST grid point to each parallax correction-shifted point. The data value of the shifted point is then assigned to that VISST grid point. In this manner, the irregular geographical shifts to correct for parallax are projected back to the rectilinear VISST grid. Because relatively higher clouds should obscure lower clouds, the variable values for the highest cloud top are preferentially chosen if two or more values are assigned to a grid point. The parallax correction should be viewed as an improved but still imperfect estimation of the cloud top locations, largely because the cloud top height is an imperfect retrieval. Please see the attached README document for further information. Users are encouraged to contact the authors with any additional questions.

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