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At least 73 records · Page 4

Engineering the radiative dynamics of thermalized excitons with metal interfaces

As a platform for optoelectronic devices based on exciton dynamics, monolayer transition metal dichalcogenides (TMDCs) are often placed near metal interfaces or inside planar cavities. While the radiative properties of point dipoles at metal interfaces has been studied extensively, those of excitons, which are delocalized and exhibit a temperature-dependent momentum distribution, lack a thorough treatment. Here, we analyze the emission properties of excitons in TMDCs near planar metal interfaces and explore their dependence on exciton center-of-mass momentum, transition dipole orientation, and temperature. Defining a characteristic energy scale k B T c = ($\hbar k$) 2 /2m (k being the radiative wavevector and m the exciton mass), we find that at temperatures T $\gg$ T c and low densities where the momentum distribution can be characterized by Maxwell-Boltzmann statistics, the modified emission rates (normalized to free space) behave similarly to point dipoles. This similarity in behavior arises due to the broad nature of wavevector components making up the exciton and point dipole emission. On the other hand, the narrow momentum distribution of excitons for T < T c can result in significantly different emission behavior as compared to point dipoles. These differences can be further amplified by considering excitons with a Bose Einstein distribution at high phase space densities, such as in a condensate phase. We find suppression or enhancement of emission relative to the point dipole case by several orders of magnitude. These insights can help optimize the performance of optoelectronic devices that incorporate 2D semiconductors near metal electrodes and can inform future studies of exciton radiative dynamics at low temperatures. Additionally, these studies show that nanoscale optical cavities are a viable pathway to generating long-lifetime exciton states in TMDCs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Near-field radiative heat transfer between irregularly shaped dielectric particles modeled with the discrete system Green's function method

Near-field radiative heat transfer (NFRHT) between irregularly shaped dielectric particles made of SiO 2 and morphology characterized by Gaussian random spheres is studied. Particles are modeled using the discrete system Green's function (DSGF) approach, which is a volume integral numerical method based on fluctuational electrodynamics. This method is applicable to finite, three-dimensional objects, and all system interactions are defined independent of thermal excitation by a generalized system Green's function. The DSGF method is deemed suitable to model NFRHT between irregularly shaped particles after verification against the analytical solution for chains of two and three SiO 2 spheres. The NFRHT results reveal that geometric irregularity in particles leads to a reduction of the total conductance from that of comparable perfect spheres at vacuum separation distances smaller than the particle size, a regime in which NFRHT is a surface phenomenon. At vacuum separation distances larger than the particle size, NFRHT becomes a volumetric process, and the total conductance between irregularly shaped particles converges to that of comparable perfect spheres. Spectral analysis reveals, however, that particle irregularity leads to damping and broadening of resonances at all separation distances, thereby highlighting the importance of the DSGF method for spectral engineering in the near field. The reduced spectral coherence when particle size is larger than the vacuum separation distance is attributed to coupling of surface phonon-polaritons within the randomly generated, distorted particle features. For particle size smaller than the vacuum separation distance, resonance broadening and damping are linked with the multiple localized surface phonon modes supported by the composite spherical harmonic morphologies of the Gaussian random spheres. In conclusion, this paper has direct implications for thermal management of packed particle systems, with applications in radiative property control, electronics, energy conversion, and nanomanufacturing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The importance of Aitken mode aerosol particles for cloud sustenance in the summertime high Arctic – a simulation study supported by observational data

The potential importance of Aitken mode particles (diameters ~ 25–80 nm) for stratiform mixed-phase clouds in the summertime high Arctic (>80° N) has been investigated using two large-eddy simulation models. We find that, in both models, Aitken mode particles significantly affect the simulated microphysical and radiative properties of the cloud and can help sustain the cloud when accumulation mode concentrations are low (< 10–20 cm –3 ), even when the particles have low hygroscopicity (hygroscopicity parameter – κ=0.1). However, the influence of the Aitken mode decreases if the overall liquid water content of the cloud is low, either due to a higher ice fraction or due to low radiative cooling rates. An analysis of the simulated supersaturation (ss) statistics shows that the ss frequently reaches 0.5 % and sometimes even exceeds 1 %, which confirms that Aitken mode particles can be activated. The modelling results are in qualitative agreement with observations of the Hoppel minimum obtained from four different expeditions in the high Arctic. Our findings highlight the importance of better understanding Aitken mode particle formation, chemical properties and emissions, particularly in clean environments such as the high Arctic.

54 ENVIRONMENTAL SCIENCES↗

Marine Shallow Cloud Adjustments to the Presence of Shortwave-Absorbing Aerosols: Advancing Understanding Through a Combined Analysis of Lasic Datasets and Process Modeling (Final Report)

This is a final report for this award, whose purpose was to support the analysis of data emanating from the LASIC (Layered Atlantic Smoke Interaction with Clouds) campaign. (Layered Atlantic Smoke Interactions with Clouds) is a strategy to improve our understanding of aged carbonaceous aerosol, its seasonal evolution, and the mechanisms by which clouds adjust to the presence of the aerosol. The observational strategy centers on deploying the AMF1 cloud, aerosol, and atmospheric profiling instrumentation to Ascension Island, located within the trade-wind shallow cumulus regime (14.50W, 80S) 3000 km offshore of continental Africa. The location is within the latitude zone of the maximum outflow of aerosol, with the deepening boundary layer known to entrain free-tropospheric smoke. The primary activities for LASIC are: 1) to improve current knowledge on aged biomass burning aerosol and its radiative properties as a function of the seasonal cycle; 2) to use surface-based remote sensing to sensitively interrogate the atmosphere for the relative vertical location of aerosol and clouds; 3) to improve our understanding of the cloud adjustments to the presence of shortwave-absorbing aerosol within the vertical column, both through aerosol-radiation and through aerosol-cloud interactions; 4) to aid low cloud parameterization efforts for climate models. This award serves to further these activities and includes a sub-award to Dr. Pablo Saide at UCLA for activities 3) and 4).

54 ENVIRONMENTAL SCIENCES↗

Bifunctional Asymmetric Fabric with Tailored Thermal Conduction and Radiation for Personal Cooling and Warming

Personal thermal management is emerging as a promising strategy to provide thermal comfort for the human body while conserving energy. By improving control over the heat dissipating from the human body, personal thermal management can provide effective personal cooling and warming. Here, we propose a facile surface modification approach to tailor the thermal conduction and radiation properties based on commercially available fabrics, to realize better management of the whole heat transport pathway from the human body to the ambient. Additionally, a bifunctional asymmetric fabric (BAF) offering both a cooling and a warming effect is demonstrated. Due to the advantages of roughness asymmetry and surface modification, the BAF demonstrates an effective cooling effect through enhanced heat conduction and radiation in the cooling mode; in the warming mode, heat dissipation along both routes is reduced for personal warming. As a result, a 4.6 °C skin temperature difference is measured between the cooling and warming BAF modes, indicating that the thermal comfort zone of the human body can be enlarged with one piece of BAF clothing. We expect this work to present new insights for the design of personal thermal management textiles as well as a novel solution for the facile modification of available fabrics for both personal cooling and warming.

42 ENGINEERING↗

Nuclear Data Sheets for A=242

Here, detailed level schemes, decay schemes, band structure, and the experimental data on which they are based are presented for all nuclei with mass number A=242. The experimental data are evaluated and adopted values are given for level and radiation properties. For references on theory refer to the NSR file at the web site given below under Cutoff Date:. This evaluation replaces the A=242 publication by Y. A. Akovali in Nuclear Data Sheets 96, 177 (2002) (2002Ak06).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Using Machine Learning to Generate a GISS ModelE Calibrated Physics Ensemble (CPE)

A neural network (NN) surrogate of the NASA GISS ModelE atmosphere (version E3) is trained on a perturbed parameter ensemble (PPE) spanning 45 physics parameters and 36 outputs. The NN is leveraged in a Markov Chain Monte Carlo (MCMC) Bayesian parameter inference framework to generate a second posterior constrained ensemble coined a “calibrated physics ensemble,” or CPE. The CPE members are characterized by diverse parameter combinations and are, by definition, close to top-of-atmosphere radiative balance, and must broadly agree with numerous hydrologic, energy cycle and radiative forcing metrics simultaneously. Global observations of numerous cloud, environment, and radiation properties (provided by global satellite products) are crucial for CPE generation. The inference framework explicitly accounts for discrepancies (or biases) in satellite products during CPE generation. We demonstrate that product discrepancies strongly impact calibration of important model parameter settings (e.g., convective plume entrainment rates; fall speed for cloud ice). Structural improvements new to E3 are retained across CPE members (e.g., stratocumulus simulation). Notably, the framework improved the simulation of shallow cumulus and Amazon rainfall while not degrading radiation fields, an upgrade that neither default parameters nor Latin Hypercube parameter searching achieved. Analyses of the initial PPE suggested several parameters were unimportant for output variation. However, many “unimportant” parameters were needed for CPE generation, a result that brings to the forefront how parameter importance should be determined in PPEs. From the CPE, two diverse 45-dimensional parameter configurations are retained to generate radiatively-balanced, auto-tuned atmospheres that were used in two E3 submissions to CMIP6.

54 ENVIRONMENTAL SCIENCES↗

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

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

54 ENVIRONMENTAL SCIENCES↗

Particle Size Distribution and Its Impacts on Ash Deposition and Radiative Transfer during Oxy-Combustion of Rice Husk–Natural Gas

Rice husk (RH) co-combustion with natural gas in highly oxygen-enriched concentrations presents a net carbon-negative energy production opportunity while minimizing flue gas recycling. However, recent experiments have shown enhanced ash deposition rates in oxygen-enriched conditions, with deposition/shedding also being dependent on the particle size distribution (PSD) of the parent RH fuel. To uncover the causative mechanisms behind these observations, add-on models for ash deposition/shedding and radiative properties were employed in computational fluid dynamics simulations. The combustion scenarios investigated encompassed two types of RH (US RH, Chinese RH) with widely varying ash contents (by % mass) and inlet fuel PSD with air and O2/CO2 (70/30 vol %, OXY70) as oxidizers. Utilizing the measured fly-ash PSDs near the deposit surface and modeling the particle viscosity accurately, particle kinetic-energy (PKE)-based capture and shedding criteria were identified as the keys to accurate deposition/shedding rate predictions. The OXY70 scenarios showed higher ash-capturing propensities due to their lower PKE. Conversely, higher erosion rates were predicted in the AIR firing scenarios. In addition, the radiative characteristics across all the scenarios were dominated by the gases and were not sensitive to the fly-ash PSD. Therefore, the higher particle concentrations in the OXY70 conditions did not negatively impact the heat extraction.

Krishnamoorthy, Gautham (ORCID:0000000255205092)↗

Radiative Reconnection-powered TeV Flares from the Black Hole Magnetosphere in M87

Abstract Active galactic nuclei in general, and the supermassive black hole in M87 in particular, show bright and rapid gamma-ray flares up to energies of 100 GeV and above. For M87, the flares show multiwavelength components, and the variability timescale is comparable to the dynamical time of the event horizon, suggesting that the emission may come from a compact region near the nucleus. However, the emission mechanism for these flares is not well understood. Recent high-resolution general-relativistic magnetohydrodynamic simulations show the occurrence of episodic magnetic reconnection events that can power flares near the black hole event horizon. In this work, we analyze the radiative properties of the reconnecting current layer under the extreme plasma conditions applicable to the black hole in M87 from first principles. We show that abundant pair production is expected in the vicinity of the reconnection layer, to the extent that the produced secondary pair plasma dominates the reconnection dynamics. Using analytic estimates backed by two-dimensional particle-in-cell simulations, we demonstrate that in the presence of strong synchrotron cooling, reconnection can produce a hard power-law distribution of pair plasma imprinted in the outgoing synchrotron (up to a few tens of MeV) and the inverse-Compton signal (up to TeV). We produce synthetic radiation spectra from our simulations, which can be directly compared with the results of future multiwavelength observations of M87* flares.

79 ASTRONOMY AND ASTROPHYSICS↗

Cloud Top Radiative Cooling Rate Drives Non-Precipitating Stratiform Cloud Responses to Aerosol Concentration

Increases in aerosol concentration are well known to influence the microphysical processes and radiative properties of clouds. By reducing droplet size, an increase in aerosol can lessen collision efficiency and increase liquid water path (LWP) in precipitating clouds or enhance evaporation rate and decrease LWP in non-precipitating clouds. We utilize large eddy simulations to further investigate these aerosol indirect effects in Arctic mixed-phase clouds and find, in agreement with previous studies, precipitating clouds to experience an increase in LWP and non-precipitating clouds a decrease in LWP. Most importantly however, our results reveal a different explanation for why such an LWP decrease occurs in decoupled, non-precipitating clouds. We find enhanced evaporation near cloud top to be driven primarily by a strengthening of maximum radiative cooling rate with aerosol concentration which drives stronger entrainment, an effect that holds true even in clouds that are optically thick.

58 GEOSCIENCES↗

EPCAPE Mt. Soledad In Situ Ozone Field Campaign Report

The focus of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) is to characterize the extent, radiative properties, aerosol interactions, and precipitation characteristics of stratocumulus clouds in the Eastern Pacific Ocean across all four seasons at a coastal location, the Scripps Pier and the Scripps Institution of Oceanography Mt. Soledad sites in La Jolla, California. An important enhancement in support of this study was the measurement of ozone at the Scripps Mt. Soledad site to help in distinguishing in situ sampling of air parcels originating from regional polluted and clean marine sources.

54 ENVIRONMENTAL SCIENCES↗

Polar Cloud Microphysics and Surface Energy Budget from AWARE (Final Technical Report)

This was a collaborative project between the Scripps Institution of Oceanography at the University of California San Diego (SIO), Byrd Polar and Climate Research Center at The Ohio State University (BPCRC), The Department of Meteorology and Atmospheric Science at The Pennsylvania State University (Penn State), and Brookhaven National Laboratory (BNL). The project’s over-arching objectives involved maximizing the scientific potential of the ARM West Antarctic Radiation Experiment (AWARE) data set, in two respects: (1) application of polar-optimized climate models to test the most current and comprehensive cloud microphysical parameterizations; and (2) analysis of the most advanced ARM Mobile Facility sensors (e.g., cloud radar, spectroradiometer, and aerosol observing system data) to advance understanding of Antarctic cloud microphysical and radiative properties, particularly on a climatological basis with emphasis on contrasts with the high Arctic. The team’s efforts have resulted in 16 peer-review publications, in addition to an overview of the AWARE campaign in the Bulletin of the American Meteorological Society. Our emphasis throughout this program was to go beyond the traditional “case study” approach to model evaluation, in which a “classical” or otherwise well-characterized surface-atmosphere-cloud system of short duration is simulated by several climate models. Instead, we attempted analysis of longer time series in the AWARE data, both climatologically and with models. We have numerous successful results from both AWARE locations: The main AMF-2 deployment at McMurdo Station on Ross Island (13 months duration), and the extended facility at the West Antarctic Ice Sheet (WAIS) Divide Ice Camp (40 days during austral summer 2015-16).

54 ENVIRONMENTAL SCIENCES↗

Toward constraint of ionization-potential depression models in a convergent geometry

We demonstrate the value of inner-shell x-ray absorption spectroscopy for dense-plasma atomic physics and explore the coupling between constraint of the thermodynamic state and constraint of ionization-potential depression models. Synthetic K-shell absorption spectra are generated along a radius from a point-like core and analyzed using different ionization-potential depression models. Within this synthetic analysis framework, we identify plasma conditions (T e = 400 eV, ρ = 40g/cm 3 ) accessible by spherical implosions where K-shell absorption spectra discriminate between models if the material temperature is measured to a precision of 20%. The analysis is extensible to a finite-sized core and can be used to guide future studies of ionization-potential depression, informing material and radiative properties of matter in fusion plasmas and stellar interiors.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Radioactive waste immobilization of Hanford sludge in magnesium potassium phosphate ceramic forms

Here, this paper evaluates immobilization of Hanford K-Basin tank sludge in magnesium potassium phosphate ceramic forms. The waste forms were produced using two simulated non-radioactive sludge streams, each with distinct characteristics and composition. Ceramicrete with wollastonite as filler was used as the matrix for this purpose. The resulting waste forms were tested for their mechanical properties, radiation stability, and leaching resistance. In another series of tests, the samples were vitrified in borosilicate glass and glass waste forms were produced. The Product Consistency Test, the American Nuclear Society's ANS 16.1 test, and the Toxicity Characteristic Leaching Procedure, which are used to develop waste acceptance criteria in the United States for permanent storage of treated waste, were used for evaluation of the leaching resistance of all waste forms.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Blowing Snow at McMurdo Station, Antarctica During the AWARE Field Campaign: Surface and Ceilometer Observations

Blowing snow (BLSN) is an impactful process in cold climates, affecting regional thermodynamics, radiation properties, and the surface mass balance of snow. Though it has significant climatic impacts, the process is still poorly understood and not widely included in weather and climate models. In 2016, the AWARE Field Campaign saw the deployment of a large suite of in situ and remote sensing instruments to McMurdo Station, Antarctica allowing for investigation of BLSN. A ceilometer–based BLSN detection algorithm used elsewhere in Antarctica is applied to data from AWARE, yielding a BLSN frequency of 14.1% compared to 8.2% as detected by human observers. To increase confidence in detections, the algorithm is updated to have shorter temporal averaging and to include a variety of meteorological thresholds to limit false detections due to fog. Efforts to incorporate a laser disdrometer into the algorithm were unsuccessful. An unphysical dependence of particle size distributions on wind speed is found suggesting observations are problematic at wind speeds greater than 10 m s –1 . The revised algorithm detected a BLSN frequency of 7.4%, increasing agreement with human observations and confidence that the process is actively occurring at the observation site. Furthermore, these observations are put into context of a climatology of human observations of BLSN at McMurdo station from 2002–2018. An annual average of 8.0%–14.0% is estimated, with a total annual range of 3.4%–21.3%. Regardless of whether BLSN is observed by humans or instrument, the majority of cases at this location are associated with ongoing precipitation.

54 ENVIRONMENTAL SCIENCES↗

Ice‐Nucleating Particles That Impact Clouds and Climate: Observational and Modeling Research Needs

Abstract Atmospheric ice‐nucleating particles (INPs) play a critical role in cloud freezing processes, with important implications for precipitation formation and cloud radiative properties, and thus for weather and climate. Additionally, INP emissions respond to changes in the Earth System and climate, for example, desertification, agricultural practices, and fires, and therefore may introduce climate feedbacks that are still poorly understood. As knowledge of the nature and origins of INPs has advanced, regional and global weather, climate, and Earth system models have increasingly begun to link cloud ice processes to model‐simulated aerosol abundance and types. While these recent advances are exciting, coupling cloud processes to simulated aerosol also makes cloud physics simulations increasingly susceptible to uncertainties in simulation of INPs, which are still poorly constrained by observations. Advancing the predictability of INP abundance with reasonable spatiotemporal resolution will require an increased focus on research that bridges the measurement and modeling communities. This review summarizes the current state of knowledge and identifies critical knowledge gaps from both observational and modeling perspectives. In particular, we emphasize needs in two key areas: (a) observational closure between aerosol and INP quantities and (b) skillful simulation of INPs within existing weather and climate models. We discuss the state of knowledge on various INP particle types and briefly discuss the challenges faced in understanding the cloud impacts of INPs with present‐day models. Finally, we identify priority research directions for both observations and models to improve understanding of INPs and their interactions with the Earth System.

54 ENVIRONMENTAL SCIENCES↗

Maximum Supersaturation in the Marine Boundary Layer Clouds Over the North Atlantic

Abstract The maximum supersaturation ( S x ) in clouds is a key parameter affecting the cloud's microphysical and radiative properties. We investigate the S x of the marine boundary layer clouds by combining airborne and surface observations in the Eastern North Atlantic. The cloud droplet number concentration ( N c ) in the least diluted cloud cores agrees well with the number concentration of particles larger than the Hoppel Minimum (HM) ( N >HM ) below clouds, indicating that the HM represents the average size threshold above which particles are activated to form cloud droplets. The S x values derived from surface observations vary from 0.10% to 0.50% from June 2017 to June 2018, with a clear seasonal variation exhibiting higher values during winter. Most of the S x variance (∼60%) can be explained by the cloud condensation nuclei (CCN) concentration and updraft velocity ( w ), with the CCN concentration playing a more important role than w in explaining the variation of S x . The influence of CCN concentration on S x leads to a buffered response of N c to aerosol perturbations. The response of N c to low aerosol concentration during winter is further buffered by the high w . The global Community Earth System Model (CESM) simulated S x values in the Azores have a positive bias compared to measured S x , likely due to overestimated w and underestimated CCN concentration. The CESM simulated S x exhibits higher values further north over the North Atlantic Ocean, which is attributed to stronger w . The suppression of S x by aerosol is also evident in regions with high CCN concentrations.

54 ENVIRONMENTAL SCIENCES↗