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At least 55 records · Page 3

Semimicroscopic description of isoscalar giant multipole resonances in medium-mass closed-shell nuclei

Main properties of isoscalar giant multipole resonances (up to L=3), including L=0,and 2 overtones, in medium-mass closed-shell nuclei are described within the semimicroscopic particle-hole dispersive optical model. Further, main properties are characterized by the energy-averaged strength distribution, projected (one-body) transition density, and probabilities of direct one-nucleon decay. Calculation results obtained for characteristics of the mentioned resonances in the 48 Ca, 90 Zr, and 132 Sn nuclei are compared with available experimental data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Intensive aerosol properties of boreal and regional biomass burning aerosol at Mt. Bachelor Observatory: larger and black carbon (BC)-dominant particles transported from Siberian wildfires

We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8–14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σ scat ), aerosol light-absorbing coefficients (σ abs ), fine particulate matter (PM 1 ), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσ scat /ΔPM 1 ), and a bimodal aerosol size distribution with a higher geometric mean diameter (D g ). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region.

54 ENVIRONMENTAL SCIENCES↗

Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets

Aerosol particles represent unique chemical environments because of their high surface area-to-volume ratio that promotes the effects of interfacial chemistry in confined environments. Properties such as viscosity, diffusivity, water content, pH, and morphology—following liquid–liquid phase separation—can strongly alter how a particle interacts with condensable vapors and reactive trace gases, thus modifying its continual evolution and environmental effects. Our understanding of this chemical evolution of atmospheric particulate matter and its environmental impacts is largely limited by our ability to directly observe how these critical particle properties respond to the addition or reactive uptake of new chemical components. Aerosol optical tweezers (AOT) stably trap particles in focused laser beams, providing positional control and the retrieval of many of these critical properties required to understand and predict the chemistry of aerosolized microdroplets. The analytical power of the AOT stems from the retrieval of the cavity-enhanced Raman spectrum induced by the trapping laser. Analysis of the whispering gallery modes (WGMs) that resonate as a standing wave around the droplet’s interface, provide high accuracy measurements of the droplet’s size, refractive index (and thus a measurement of composition), and can distinguish between core–shell, partially engulfed, and homogeneous morphologies. In this study, we have advanced the ability to determine the properties of the core and shell phases in biphasic droplets, including obtaining high-accuracy pH measurements. These capabilities were applied to perform AOT physical chemistry experiments on authentic secondary organic aerosol (SOA) produced directly in the AOT chamber by ozonolysis of terpene vapors. The propensity of the SOA to phase separate as a shell from a wide range of nonpolar to polar core phases was observed, along with the discovery of a stable emulsified state of SOA particles in an aqueous salt droplet. Micron-thick SOA shells did not impede the gain or loss of water or squalane from the core to the surrounding air, indicating no significant diffusional limitations to condensational growth or partitioning even under dry conditions. These experiments formed the foundation of a new framework that predicts how the phase-separated morphology of complex aerosols containing organic carbon evolves during continual atmospheric oxidation processes. Increases in oxidation state will quickly drive conversion from a partially engulfed to core–shell morphology that has dramatically different chemical reactivity since the core phase is completely concealed by the shell. The recent advances in the experimental capabilities of the AOT technique such as presented here enable novel experimental methodologies that provide insights into the chemistry and multidimensional properties of aerosol microdroplets, and how these coevolve and respond to continual chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Optical Properties of Individual Tar Balls in the Free Troposphere

Tar balls are brown carbonaceous particles, highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are believed to have a significant impact on the Earth’s radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory “Ottavio Vittori” on Mt. Cimone, Italy (2165 meters above sea level) using multi-modal micro-spectroscopy. Our results show that tar balls contributed 50% of carbonaceous particles by number in the size range from 0.25 to 1.8 µm. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average refractive index of inhomogeneously and homogenously mixed tar balls (1.40 - 0.03i, and 1.36 - 0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model (SBDART) and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 Wm-2 (on a clear sky day) to 9.5 Wm-2 (when clouds are below the aerosol layer). In conclusion, understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

54 ENVIRONMENTAL SCIENCES↗

Monitoring and characterization of particle contamination in the pulse compression chamber of the OMEGA EP laser system

The laser-damage performance of optics is known to be negatively affected by microscale particle contamination induced by the operational environment. This work investigates the properties of particles accumulating in various locations near critical optics inside the OMEGA EP grating compressor chamber during quarterly operational periods over a 2-year duration. The particles found were characterized using optical microscopy, scanning electron microscopy and energy dispersive X-ray spectroscopy. The analysis indicates significant concentrations of micrometer- to nanometer-scale particles inside the vacuum chamber, with higher values observed near the port leading to the OMEGA EP target chamber. The distribution of the chemical composition of these particles varies between collection periods. Although understanding of the mechanisms of particle generation and transport remains uncertain, the hypothesis is that this particle load represents a risk for contaminating the surfaces of high-value optics located inside the chamber, including the compression gratings and deformable mirrors, and therefore affecting their laser-damage resistance and overall operational lifetime.

47 OTHER INSTRUMENTATION↗

Microphysical properties of atmospheric soot and organic particles: measurements, modeling, and impacts

Atmospheric soot and organic particles from fossil fuel combustion and biomass burning modify Earth’s climate through their interactions with solar radiation and through modifications of cloud properties by acting as cloud condensation nuclei and ice nucleating particles. Recent advancements in understanding their individual properties and microscopic composition have led to heightened interest in their microphysical properties. This review article provides an overview of current advanced microscopic measurements and offers insights into future avenues for studying microphysical properties of these particles. To quantify soot morphology and ageing, fractal dimension ( D f ) is a commonly employed quantitative metric which allows to characterize morphologies of soot aggregates and their modifications in relation to ageing factors like internal mixing state, core-shell structures, phase, and composition heterogeneity. Models have been developed to incorporate D f and mixing diversity metrics of aged soot particles, enabling quantitative assessment of their optical absorption and radiative forcing effects. The microphysical properties of soot and organic particles are complex and they are influenced by particle sources, ageing process, and meteorological conditions. Furthermore, soluble organic particles exhibit diverse forms and can engage in liquid–liquid phase separation with sulfate and nitrate components. Primary carbonaceous particles such as tar balls and soot warrant further attention due to their strong light absorbing properties, presence of toxic organic constituents, and small size, which can impact human health. Future research needs include both atmospheric measurements and modeling approaches, focusing on changes in the mixing structures of soot and organic particle ensembles, their effects on climate dynamics and human health.

54 ENVIRONMENTAL SCIENCES↗

Understanding Biases in Simulated Cloud Radiative Effects in E3SMv3

This study systematically investigates biases in cloud radiative effects (CREs) within the recently released Energy Exascale Earth System Model version 3 (E3SMv3). Compared to its previous version (E3SMv2), E3SMv3 shows excessively strong shortwave CRE over tropical and subtropical oceans, the Southern Ocean, and the Northern Hemisphere storm tracks, which is primarily caused by an overestimation of optically intermediate low clouds. The model also displays excessive longwave CRE over the Maritime Continent and other tropical deep convection regions, resulting from an overestimation of optically thick high clouds. Implementing the Predicted Particle Properties (P3) scheme for stratiform clouds played the most significant role in these cloud changes. In addition, using a double-moment scheme for convective clouds contributed to the increase in intermediate low clouds and optically thick clouds in tropical deep convection regions. Error metrics for total cloud amount (E TCA ), cloud properties (E ctp-τ ), and cloud properties weighted by their SW and LW radiative impacts (E SW and E LW ) indicate that E3SMv3's ability to reproduce observed cloud radiative effect of low, middle, and high clouds has not been improved compared to E3SMv2. Nevertheless, the performance of E3SMv3 remains well within the spread of CMIP6 models, with E SW and E LW values smaller than those in most CMIP6 models. This study underscores the importance of integrating diverse satellite observations for robust cloud evaluation and using cloud-radiation relationships as consistency check for model errors. It suggests that further model developments focus on improving cloud microphysics and their interactions with radiation.

Environmental sciences↗

Characterization of carbonaceous aerosols during TRACER-CAT

Absorbing aerosols (AA) have an important impact on the global radiation budget and cloud properties. The composition and properties of AA can vary substantially throughout the atmosphere, depending on the particle source and the influence of chemical aging. Uncertainties associated with the radiative effects of AA remain substantial. A key contributor to this uncertainty is understanding the extent to which coatings in general, and water uptake especially, alters absorption by AA particles and how this depends on particle composition. We deployed new and existing experimental tools during the Tracking Aerosol Convection Interactions Experiment (TRACER) campaign in Houston, TX as part of the Carbonaceous Aerosols Thrust (CAT) to provide detailed characterization of aerosol optical, chemical, and physical properties. Our TRACER-CAT measurements complemented and expanded on the planned TRACER instrumentation, allowing for more detailed characterization of aerosol properties of relevance to cloud development (a core focus of TRACER), such as the composition of particles that can act as cloud condensation nuclei, than would otherwise be available. Our measurements have allowed for assessment of the relationship(s) between AA optical properties (with a focus on absorption) and the chemical and physical characteristics (including the mixing state of black carbon (BC) containing particles). These field observations occurred in collaboration with Los Alamos National Laboratory in summer 2022 during the TRACER intensive operating period. The instrumentation we co-deployed provided for measurement of (i) multi-wavelength dry aerosol absorption, scattering, and extinction, (ii) the size-dependent composition and abundance of sub-micron aerosol, differentiating between those particles that do and do not contain BC, (iii) BC-specific concentrations and size distributions, (iv) particle size, and (v) the first field measurements at an ARM site of the influence of RH on multi-wavelength absorption by ambient AA. We have leveraged the natural variability of the atmosphere and of aerosol sources in the Houston region to (i) specifically disentangle contributions to light absorption from BC, absorbing organic carbon (brown carbon), and coatings on BC, (ii) characterize the mixing state of BC and assess the factors that give rise to compositional differences between BC-containing and BC-free aerosol, and (iii) establish how water uptake influences absorption and how any such effect depends on particle composition and BC mixing state. Overall, our study contributed to the mission of the Atmospheric System Research program in multiple ways. Through the deployment of complementary, advanced instrumentation for characterization of a wide range of aerosol properties our work helped to maximize the scientific impact of the TRACER campaign. Our work also allowed for development of new insights into the relationship(s) between aerosol composition, hygroscopicity, and the mixing state of BC with aerosol optical properties. Through this, our work has provided knowledge that can improve understanding and model representation of aerosol processes as they affect the Earth’s radiation budget.

54 ENVIRONMENTAL SCIENCES↗

Properties of isoscalar giant multipole resonances in medium-heavy closed-shell nuclei: A semimicroscopic description

The semimicroscopic particle-hole dispersive optical model (PHDOM) is implemented to describe main properties of Isoscalar Giant Multipole Resonances (up to L=3) in medium-heavy closed-shell nuclei. Here, the main properties are characterized by the strength distribution, transition density, partial and total probabilities of direct one-nucleon decay. Calculation results obtained for the 208 Pb nucleus are compared with available experimental data.

190 ≤ A ≤ 219↗

Density Functional Tight Binding Insights into Plasmonic Silver–Platinum Nanoparticles and Alloys for Enhanced Photocatalysis

Developing accurate and efficient Slater-Koster (SK) tight-binding parameter sets is essential for quantum plasmonic studies of alloyed metal nanoparticles, as conventional time dependent density functional theory (TD-DFT) calculations are computationally prohibitive for larger clusters. In this work, we develop and validate density functional tight binding (DFTB) parameter sets for both ground state (GS-SK) and excited state (ES-SK) calculations to study the structural, electronic, and optical properties of silver (Ag), platinum (Pt), and Ag–Pt nanoalloys. Our investigation of the ground state properties demonstrates that the GS-SK parameters enable DFTB to closely reproduce the electronic structures of platinum clusters with diverse sizes and geometries – showing qualitative agreement with DFT for density of states (DOS) profiles and energy levels. The ES-SK parameters accurately describe excited-state properties compared to TD-DFT reference calculations, including the broad, featureless absorption profiles of Pt that are dominated by interband transitions. Using the ES-SK parameters within a real-time TD-DFTB framework, we compute size-dependent optical absorption spectra of Ag, Pt and Ag-Pt nanocubes containing up to 1099 atoms (size ∼4.18 nm). A detailed study of Ag–Pt and Pt-Ag core–shell nanoparticles shows quenching of the Ag plasmon resonance even at monolayer coverage for Ag-Pt, but not for Pt-Ag. We also show how to define submonolayer Ag-core Pt-shell cubic structures that have similar optical properties to those generated experimentally for much larger particles, which offers potential for describing plasmon-enhanced photocatalysis. Collectively, the GS-SK and ES-SK parameter sets provide an accurate, computationally efficient approach for modeling the complex optical and electronic behavior of noble–transition metal nanostructures and their alloys.

SPR↗

Midgap state requirements for optically active quantum defects

Abstract Optically active quantum defects play an important role in quantum sensing, computing and communication. The electronic structure and the single-particle energy levels of these quantum defects in the semiconducting host have been used to understand their optoelectronic properties. Optical excitations that are central for their initialization and readout are linked to transitions between occupied and unoccupied single-particle states. It is commonly assumed that only quantum defects introducing levels well within the band gap and far from the band edges are of interest for quantum technologies as they mimic an isolated atom embedded in the host. In this perspective, we contradict this common assumption and show that optically active defects with energy levels close to the band edges can display similar properties. We highlight quantum defects that are excited through transitions to or from a band-like level (bound exciton) such as the T center and Se S i + in silicon. We also present how defects such as the silicon split-vacancy in diamond can involve transitions between localized levels that are above the conduction band or below the valence band. Loosening the commonly assumed requirement on the electronic structure of quantum defects offers opportunities in quantum defects design and discovery especially in smaller band gap hosts such as silicon. We discuss the challenges in terms of operating temperature for photoluminescence or radiative lifetime in this regime. We also highlight how these alternative type of defects bring their own needs in terms of theoretical developments and fundamental understanding. This perspective clarifies the electronic structure requirement for quantum defects and will facilitate the identification and design of new color centers for quantum applications especially driven by first principles computations.

Xiong, Yihuang (ORCID:0000000178096047)↗

Influence of open ocean biogeochemistry on aerosol and clouds: Recent findings and perspectives

Aerosols and clouds are key components of the marine atmosphere, impacting the Earth’s radiative budget with a net cooling effect over the industrial era that counterbalances greenhouse gas warming, yet with an uncertain amplitude. Here we report recent advances in our understanding of how open ocean aerosol sources are modulated by ocean biogeochemistry and how they, in turn, shape cloud coverage and properties. We organize these findings in successive steps from ocean biogeochemical processes to particle formation by nucleation and sea spray emissions, further particle growth by condensation of gases, the potential to act as cloud condensation nuclei or ice nucleating particles, and finally, their effects on cloud formation, optical properties, and life cycle. We discuss how these processes may be impacted in a warming climate and the potential for ocean biogeochemistry—climate feedbacks through aerosols and clouds.

54 ENVIRONMENTAL SCIENCES↗

Optical and transport properties of plasma mixtures from ab initio molecular dynamics

Predicting the charged particle transport properties of warm dense matter/hot dense plasma mixtures is a challenge for analytical models. High accuracy ab initio methods are more computationally expensive, but can provide critical insight by explicitly simulating mixtures. In this work, we investigate the transport properties and optical response of warm dense carbon–hydrogen mixtures at varying concentrations under either conserved electronic pressure or mass density at a constant temperature. We compare options for mixing the calculated pure species properties to estimate the results of the mixtures. We find that a combination of the Drude model with the Matthiessen's rule works well for DC electron transport and low-frequency optical response. This breaks down at higher frequencies, where a volumetric mix of pure-species AC conductivities works better.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Liquid-induced topological transformations of cellular microstructures

The fundamental topology of cellular structures—the location, number and connectivity of nodes and compartments—can profoundly affect their acoustic, electrical5, chemical, mechanical and optical properties, as well as heat, fluid and particle transport. Approaches that harness swelling, electromagnetic actuation and mechanical instabilities in cellular materials have enabled a variety of interesting wall deformations and compartment shape alterations, but the resulting structures generally preserve the defining connectivity features of the initial topology. Achieving topological transformation presents a distinct challenge for existing strategies: it requires complex reorganization, repacking, and coordinated bending, stretching and folding, particularly around each node, where elastic resistance is highest owing to connectivity. Here we introduce a two-tiered dynamic strategy that achieves systematic reversible transformations of the fundamental topology of cellular microstructures, which can be applied to a wide range of materials and geometries. Our approach requires only exposing the structure to a selected liquid that is able to first infiltrate and plasticize the material at the molecular scale, and then, upon evaporation, form a network of localized capillary forces at the architectural scale that ‘zip’ the edges of the softened lattice into a new topological structure, which subsequently restiffens and remains kinetically trapped. Reversibility is induced by applying a mixture of liquids that act separately at the molecular and architectural scales (thus offering modular temporal control over the softening–evaporation–stiffening sequence) to restore the original topology or provide access to intermediate modes. Guided by a generalized theoretical model that connects cellular geometries, material stiffness and capillary forces, we demonstrate programmed reversible topological transformations of various lattice geometries and responsive materials that undergo fast global or localized deformations. In conclusion, we then harness dynamic topologies to develop active surfaces with information encryption, selective particle trapping and bubble release, as well as tunable mechanical, chemical and acoustic properties.

42 ENGINEERING↗

Dependent scattering and fractal microstructure determine the transparency of aerogel monoliths

This study reveals how dependent scattering and microstructure significantly affect electromagnetic wave propagation through aerogel monoliths, contributing to their transparency. Light scattering by particle ensembles is considered “dependent” when the scattering properties rely not only on particle size and optical constants but also on their spatial distribution, typically occurring when the average interparticle distance is small in comparison with the wavelength of incident radiation. Addressing dependent scattering requires solving Maxwell’s equations for complex heterogeneous structures, which is computationally demanding and usually limited to sample thicknesses on the same scale as the wavelength. This study combines computer-generated ambigel microstructures of fractal aggregates of polydisperse nanoparticles and the radiative transfer with reciprocal transaction method to predict the transmittance of thick ambigel slabs. Transmittance measurements of ambiently dried aerogel monoliths (ambigels) with porosities from about 50% to 90% closely matched the predicted values for their digital twins. However, ignoring dependent scattering or particle aggregation led to inaccurate predictions. This study validated the computational framework, and its findings offer insights for designing photonic metamaterials and analyzing their interactions with electromagnetic waves.

Yalcin, Refet A. (ORCID:0000000339973494)↗

Role of shell composition and morphology in achieving single-emitter photostability for green-emitting “giant” quantum dots

The use of the varied chemical reactivity of precursors to drive the production of a desired nanocrystal architecture has become a common method to grow thick-shell graded alloy quantum dots (QDs) with robust optical properties. Conclusions on their behavior assume the ideal chemical gradation and uniform particle composition. In this work, advanced analytical electron microscopy (high-resolution scanning transmission electron microscopy coupled with energy dispersive spectroscopy) is used to confirm the nature and extent of compositional gradation and these data are compared with performance behavior obtained from single-nanocrystal spectroscopy to elucidate structure, chemical-composition, and optical-property correlations. In particular, the evolution of the chemical structure and single-nanocrystal luminescence was determined for a time-series of graded-alloy “CdZnSSe/ZnS” core/shell QDs prepared in a single-pot reaction. In a separate step, thick (~6 monolayers) to giant (>14 monolayers) shells of ZnS were added to the alloyed QDs via a successive ionic layer adsorption and reaction (SILAR) process, and the impact of this shell on the optical performance was also assessed. By determining the degree of alloying for each component element on a per-particle basis, we observe that the actual product from the single-pot reaction is less “graded” in Cd and more so in Se than anticipated, with Se extending throughout the structure. The latter suggests much slower Se reaction kinetics than expected or an ability of Se to diffuse away from the initially nucleated core. It was also found that the subsequent growth of thick phase-pure ZnS shells by the SILAR method was required to significantly reduce blinking and photobleaching. However, correlated single-nanocrystal optical characterization and electron microscopy further revealed that these beneficial properties are only achieved if the thick ZnS shell is complete and without large lattice discontinuities. Thus, we identify the necessary structural design features that are required for ideal light emission properties in these green-visible emitting QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

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↗