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At least 145 records · Page 8

Interactions Between the Amazonian Rainforest and Cumuli Clouds: A Large‐Eddy Simulation, High‐Resolution ECMWF, and Observational Intercomparison Study

Abstract The explicit coupling at meter and second scales of vegetation's responses to the atmospheric‐boundary layer dynamics drives a dynamic heterogeneity that influences canopy‐top fluxes and cloud formation. Focusing on a representative day during the Amazonian dry season, we investigate the diurnal cycle of energy, moisture and carbon dioxide at the canopy top, and the transition from clear to cloudy conditions. To this end, we compare results from a large‐eddy simulation technique, a high‐resolution global weather model, and a complete observational data set collected during the GoAmazon14/15 campaign. The overall model‐observation comparisons of radiation and canopy‐top fluxes, turbulence, and cloud dynamics are very satisfactory, with all the modeled variables lying within the standard deviation of the monthly aggregated observations. Our analysis indicates that the timing of the change in the daylight carbon exchange, from a sink to a source, remains uncertain and is probably related to the stomata closure caused by the increase in vapor pressure deficit during the afternoon. We demonstrate quantitatively that heat and moisture transport from the subcloud layer into the cloud layer are misrepresented by the global model, yielding low values of specific humidity and thermal instability above the cloud base. Finally, the numerical simulations and observational data are adequate settings for benchmarking more comprehensive studies of plant responses, microphysics, and radiation.

Vilà‐Guerau de Arellano, J.↗

Vertical Structure of Clouds and Precipitation During Arctic Cold–Air Outbreaks and Warm–Air Intrusions: Observations From COMBLE

The Arctic is marked by deep intrusions of warm, moist air, alternating with outbreaks of cold air down to lower latitudes. The typical vertical structure of clouds and precipitation during these two synoptic weather extremes is examined at a coastal site at 69°N in Norway. The Norwegian Sea is a corridor for warm-air intrusions (WAIs) and frequently witnesses cold-air outbreaks (CAOs). This study uses data from profiling radar, lidar, and microwave radiometer, radiosondes and other probes that were collected during the CAOs in the Marine Boundary Layer Experiment (COMBLE) between 1 December 2019 and 31 May 2020. Marine CAOs are defined in terms of thermal instability relative to the sea surface temperature, and WAIs in terms of equivalent potential temperature stratification between the surface and 850 hPa. Cloud structures in CAOs are convective, driven by strong surface heat fluxes over a long fetch of open water, with cloud tops rarely exceeding 6 km above sea level. The mostly open-cellular convection produces intermittent moderately-heavy precipitation at the observational site, notwithstanding the low precipitable water vapor (PWV). In contrast, WAIs are marked by high values of PWV and integrated vapor transport. Here, WAI clouds are synoptically driven, stratiform, with cloud tops often exceeding 5 km, sometimes layered, and generally producing persistent precipitation that can be heavier than in CAOs.

54 ENVIRONMENTAL SCIENCES↗

Enabling stable and high-rate cycling of a Ni-rich layered oxide cathode for lithium-ion batteries by modification with an artificial Li⁺-conducting cathode-electrolyte interphase

Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathodes are investigated to realize high energy density Li ion batteries for long life electric vehicle applications. However, capacity decay and thermal instability due to cathode-electrolyte interfacial degradation remain challenges that require sophisticated surface stabilization methods to address. Here, we propose a strategy, for the first time, to form an artificial Li + -conducting cathode-electrolyte interphase (ALCEI) on the NCM811 cathode surface using a nucleophilic reaction between polysulfides and vinylene carbonate (VC). Furthemore, the as-formed ALCEI layer simultaneously protects the NCM particles from electrolyte corrosion and facilitates Li + ion transport, thus enabling stable and high rate cycling of NCM811. As a result, the ALCEI-modified NCM811 cathode exhibits a high capacity (211.6 mA h g -1 at 0.1C), notable rate capability (134 mA h g -1 at 10C), and superior cycle stability (94.2% over 200 cycles at 1C). These results underscore the use of interfacial engineering in high voltage cathode material development and provide a feasible strategy for stabilizing Ni-rich cathode interfaces in practical Li ion battery applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stabilization of reactive rare earth alkyl complexes through mechanistic studies

Rare earth tris(alkyl) complexes such as M(CH 2 SiMe 3 ) 3 (sol) n are widely used as precursors for many compounds and as homogeneous catalysts for alkene polymerization and alkane functionalization. However, the thermal instability of those most conveniently made from the commercially available lithium salt of the neosilyl anion, LiCH 2 SiMe 3 , Li(r), restricts their utility. We present a new range of synthetically useful, more kinetically stable rare earth neosilyl solvates, derived from a full kinetic study of the various possible decomposition mechanisms of 7 known and 12 new solvated rare earth neosilyl complexes M(CH 2 SiMe 3 ) 3 (sol) n M = Sc(III), Y(III), Lu(III), Sm(III), and sol = THF; TMEDA; DMPE; diglyme ((CH 3 ) 2 (OCH 2 CH 2 ) 2 O, G 2 ), triglyme ((CH 3 ) 2 (OCH 2 CH 2 ) 3 O, G 3 ). Surprisingly, simply using higher-denticity donors to sterically disfavor neosilyl γ-H elimination is not effective. While Sc(r) 3 ((CH 3 ) 2 (OCH 2 CH 2 ) 2 O) has a half-life, t 1/2 , of 258.1 h, six times longer than for Sc(r) 3 (C 4 H 8 O) 2 (t 1/2 = 43 h), Lu(r) 3 ((CH 3 ) 2 (OCH 2 CH 2 ) 2 O) and Y(r) 3 ((CH 3 ) 2 (OCH 2 CH 2 ) 2 O) do not show the expected, analogous increased t 1/2 . This is because new decomposition pathways appear for poorly fitting donors. Finally, kinetic studies demonstrate the impact of small, and increasing amounts of LiCl on the kinetics of the reactivity of the smaller alkyls Y(r) 3 (THF) 2 and Lu(r) 3 (THF) 2 ; molecules used in hydrocarbon chemistry and catalysis for fifty years. A new route to pure Y(r) 3 (THF) 2 , which avoids the traditional use of Li(r), is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Advanced spectrometric methods for characterizing bio-oils to enable refineries to reduce fuel carbon intensity during co-processing

A promising approach for supplementing petroleum-derived fuels to support reductions in green-house gas emissions is to convert abundant biomass feedstocks into renewable carbon-rich oils using pyrolysis. However, the resultant bio-oils contain various oxygenated compounds that can impart acidity, chemical and thermal instability, and immiscibility with petroleum derived fuels, necessitating further upgrading to derive fuel blendstocks. Co-processing bio-oils and petroleum-derived liquids in existing refineries is a potentially near-term, cost-effective approach for upgrading bio-oils while reducing refinery carbon intensities. However, one cause for hesitation in co-processing bio-oils is limited comprehensive characterization and speciation of the bio-oil components. Advanced analytical techniques are currently under investigation to enable identification of elusive species in bio-oils, enabling researchers to develop strategies to mitigate catalyst deactivation agents and contaminants. This review provides a brief overview of several analytical methods commonly used to analyze bio-oils and their limitations. In addition, advanced techniques currently under development are discussed to further elucidate bio-oil components that may limit its end use. This will help inform the technical and economic feasibility of co-processing bio-oils with petroleum-derived liquids, therefore, improving the overall downstream processes for biofuels blendstock production.

09 BIOMASS FUELS↗

Evolution and feedback of AGN jets of different cosmic ray composition

Jet feedback from active galactic nuclei (AGN) is one of the most promising mechanisms for suppressing cooling flows in cool-core clusters. However, the composition of AGN jets and bubbles remains uncertain; they could be thermally dominated, or dominated by cosmic ray proton (CRp), cosmic ray electron (CRe), or magnetic energy. In this work, we investigate the evolution and feedback effects of CRp and CRe dominated jets by conducting 3D magnetohydrodynamic simulations of AGN jet-inflated bubbles in the intracluster medium using the FLASH code. We present the evolution of their energies, dynamics, and heating, and model their expected cavity-power versus radio-luminosity relation (P cav –L R ). We find that bubbles inflated by CRe dominated jets follow a very similar dynamical evolution to CRp dominated bubbles even though CRe within bubbles suffer significantly stronger synchrotron and inverse-Compton cooling. This is because, as CRe lose their energy, the jet-inflated bubbles quickly become thermally dominated within ∼30 Myr. Their total energy stops decreasing with CR energy and evolves similarly to CRp dominated bubbles. The ability of CRe and CRp dominated bubbles to heat the intracluster medium is also comparable; the cold gas formed via local thermal instabilities is well suppressed in both cases. The CRp and CRe bubbles follow different evolutionary trajectories on the P cav –L R plane, but the values are broadly consistent with observed ranges for FR-I sources. We also discuss observational techniques that have potential for constraining the composition of AGN jets and bubbles.

79 ASTRONOMY AND ASTROPHYSICS↗

Utilizing the deuterium-tritium fusion resonance to diagnose thermal runaway in igniting plasmas

For high-efficiency inertial confinement fusion implosions, it is predicted that a burning hot spot will successfully encompass all surrounding fuel and then transition into a thermal runaway where the internal energy increase from fusion occurs on a timescale faster than the expansion of the fuel is able to quench the fusion chain reaction after ignition occurs. Observation of this dynamic phase transition would indicate distinct burn properties and indicate an implosion's robustness. A technique for diagnosing the presence of thermal runaway from measurements of nuclear reaction history is presented. The technique is based on taking the logarithmic derivative of the nuclear reaction history, called the 𝛼 curve, and allowing a mathematical decoupling of the mass, volume, and thermal reactivity in the fusion reaction rate equation. During thermal runaway, where the thermal temperature dominates the burn dynamics, a maximum in the 𝛼 curve is found where there is a maximum in the first derivative of the thermal fusion reactivity, an effect to the deuterium-tritium (DT) fusion cross-section resonance. This provides a distinct signature related to the fundamental nature of the DT fusion nuclear resonance and signifies the transition into the fusion thermal instability. Impacts of charged particle transport on the effect are also assessed and the analytical formulas are compared and found to be in agreement with radiation hydrodynamic codes.

high-energy-density plasmas↗

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↗

Enhanced Light Outcoupling from OLEDs Fabricated on Novel Low-Cost Patterned Plastic Substrates of Varying Periodicity

OLEDs continue to make strides in display applications, but their commercial utilization in solid-state lighting (SSL) is lagging. An ongoing challenge, in particular for manufacturing, is the need for enhanced efficiency and hence the necessity to increase in an inexpensive approach the extraction of the light generated inside the OLED into the forward (viewing) hemisphere. In conventional OLEDs fabricated on a transparent flat anode coated on glass, the external quantum efficiency (EQE) is only ~20%. About 50% of the light is lost to internal waveguiding in the high refractive index (RI) organic + ITO anode layers and to surface plasmon polaritons (SPPs) at the organic/metal cathode interface. Another ~30% of the light is externally waveguided in the substrate to its edges. While extraction of the externally waveguided light is commonly addressed by adding a microlens array (MLA) or a scattering layer at the substrate’s air-side, light outcoupling increases by only ~1.6-1.7x (vs up to 2.5x in improving from ~20% to ~50%). The use of a hemispherical lens or an index matching fluid (IMF) at the substrate/photodetector (PD) interface increases the outcoupling by at least 2x; these approaches however, are not viable industrially, and even a MLA is sometimes undesirable due to its non-planar, scattering structure. In multi-stack tandem OLEDs, where the metal cathode is far from the emitting zone(s), the impact of photons loss to SPPs decreases. Our project addressed the ~50% loss to the internally waveguided light and SPPs. We evaluated OLEDs fabricated on patterned or planarized plastic substrates manufactured in a cost-effective approach compatible with a roll-to-roll (R2R) process. The OLEDs were either (i) patterned to various degrees depending on the pitch a and height or depth h of the pattern features or (ii) planar, with a pattern buried under a flat high RI planarization layer. We demonstrated that the outcoupling from green patterned OLEDs reaches ~50% by mitigating plasmon–related loss and internal waveguiding, even without the addition of a MLA, a hemispherical lens, or IMF. Simulations conducted in parallel with the experimental effort demonstrated how diffraction by conformally corrugated OLEDs increases the outcoupling to >60%. Structures with varying pitch values were also simulated indicating that combining domains of varying pitch could increase outcoupling to 55-60%. Experimentally, we additionally assessed the role a and h in determining not only the OLED efficiencies, but also their structural properties, i.e., the uniformity and conformality throughout the OLED stack. As planar OLEDs are preferred over corrugated devices, we studied different patterns in plastic substrates that were planarized by a high RI formulation. Planar green OLEDs on such structures showed enhanced efficiencies with EQEs larger than 60% with the addition of an IMF (to extract the substrate mode) at the substrate/Si PD interface. White OLEDs showed EQEs of 45.5%. Plastic substrates are currently less attractive than glass substrates due to drawbacks such as permeability to water vapor and oxygen, and in some cases thermal instability. Plastic substrates however, are flexible and easy to handle unlike thin flexible glass, and once transparent thin barrier films are available, they will become more attractive; they are already of interest in medical applications. Importantly, as it is easy to generate various patterns in different plastic materials, they provide excellent means for assessing and optimizing enhancing extracting structures. Such structures can also be transferred to glass substrates with some process modifications. The technical effectiveness and economic feasibility of the project lie in the patterning of the extracting plastic substrates in an approach that is scalable to R2R manufacturing. R2R processes are of drastically lower-cost than batch or single-unit fabrication. The patterned plastic can be a part of an integrated substrate either plastic or glass, which includes also a MLA or a planar layer with embedded scattering particles, as well as a conductive metal mesh/electrode design. SSL is environmentally-friendly and as OLED SSL becomes more efficient it will reduce electricity consumption, and hence lighting cost, as well as produce less expensive attractive lighting fixtures. Our university-industry collaboration is hence of major benefit to the public as it demonstrates the feasibility of manufacturing optimized extracting substrates for highly efficient OLEDs for SSL in a future R2R process, which would drastically reduce the manufacturing cost and increase production in the USA. Moreover, newly developed methods by our team allow low-cost roll manufactured substrates to be transferred to flexible or rigid glass substrates, which solves the plastic substrate barrier issues, and when combined with device encapsulation will increase the OLEDs’ environmental stability.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Understanding the Mechanisms of Self-Organization in Atmospheric Pressure DC Glows

One of the most challenging areas in atmospheric pressure plasmas is controlling uniformity and contact area. Indeed it is this problem which is closely related to scale up that has impeded the widespread applications of these plasmas. The atmospheric pressure plasma glow is a type of atmospheric pressure discharge akin to a traditional low pressure glow particularly when compared with discharge morphology. But this is where the similarities end. Unlike low pressure glows, atmospheric pressure glows do not rely on electrode processes such as secondary electron emission to make the discharge self-sustaining, rather the discharge is sustained by typically processes such as the presence of a resistive layer or through favorable atomic collisional processes such as that which prevail in helium that stabilizes the discharge so that the thermal instability is mitigated. These discharges can feature either solid metal electrodes or geometries where at least one electrode is a liquid water electrolyte. Regardless of the implementation, DC 1 Atm glows are fascinating in that the plasma attachment under certain conditions can self-organize. The attachment surface area therefore changes as a result. Therefore, self-organization could be the key to optimizing plasma contact area and thereby open the door to applications in the real world. The plasma physical processes prevailing at the surface where the self-organization takes place remain largely unexplored. There is very little published research on the conditions that prevail at the surface and virtually no scholarship on measured plasma parameters of the self-organized attachments themselves or the surface electric field. This effort breaks new ground by elucidating these largely unexplored physical processes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Determination of Phenolic Groups in Bio-Oils Using Revised Folin-Ciocalteu Methods: Single Cuvette and Plate Reader. Laboratory Analytical Procedure (LAP), Issue Date: May 12, 2022

Phenol components are ubiquitous in wood-derived bio-oils and biocrudes. Their reaction with other functional groups (e.g., aldehydes) may contribute to the formation of carbonaceous species and the expected thermal instability of pyrolysis oils. During hydrotreating, phenols can be recalcitrant species, requiring higher reaction temperatures than other oxygen-containing functional groups. Phenols are also present in upgraded products and have been shown to lead to catalyst deactivation during hydrotreating. They also are the first oxygenated functional group to re-appear in the upgraded product, signaling catalyst deactivation. This procedure covers the determination of phenolic compounds in fast pyrolysis oils. This Laboratory Analytical Procedure (LAP) includes two methods, the first allowing for shorter analysis time at increased reaction temperature, while the second employs a longer analysis time but at room temperature. Additionally, the use of both a single cuvette and of a plate reader are also presented.

09 BIOMASS FUELS↗

JWST Noise Floor. II. Systematic Error Sources in JWST NIRCam Time Series

The James Webb Space Telescope (JWST) holds great promise for characterizing atmospheres of transiting exoplanets, potentially providing insights into Earth-sized planets within the habitable zones of M-dwarf host stars if photon-limited performance can be achieved. Here, we discuss the systematic error sources that are expected to be present in grism time-series observations with the NIRCam instrument. We find that pointing jitter and high-gain antenna moves in addition to the detectors’ subpixel crosshatch patterns will produce relatively small variations (less than 6 parts per million, ppm). The time-dependent aperture losses due to thermal instabilities in the optics can also be kept to below 2 ppm. To achieve these low noise values, it is important to employ a sufficiently large (more than 11) extraction aperture. Persistence due to charge-trapping will have a minor (less than 3 ppm) effect on the time series 20 minutes into an exposure and is expected to play a much smaller role than it does for the Hubble Space Telescope WFC3 detectors. We expect detector temperature fluctuations to contribute less than 3 ppm. In total, our estimated noise floor from known systematic error sources is only 9 ppm per visit. We urge caution, however, because unknown systematic error sources could be present in flight and will only be measurable on astrophysical sources such as quiescent stars. We find that reciprocity failure may introduce a perennial instrument offset at the 40 ppm level, so corrections may be needed when a multi-instrument multi-observatory spectrum is stitched together over wide wavelength ranges.

47 OTHER INSTRUMENTATION↗

Formation of solar prominences.

Thermal instability mechanism for quiescent solar prominence formation by condensation from solar corona, noting condensation inhibition by free electrons heat conduction

Raju, P. K.↗

Thickening of axisymmetric accretion disks and flows

A study is made to determine whether or not hot plasma flowing from the inner edge of an accretion disk around a black hole can thicken out of the disk plane with the onset of a Pringle-Rees thermal instability. The instability is caused by the density thinning caused by the sharp increase in radial infall velocity near the radius of the marginally stable circular orbit, or by abrupt variations in viscosity or Lightman-Eardly secular instabilities. An estimate of the thickening timescale is given. Various physically realistic situations involving radial steady-state flow and where significant disk thickening can occur in the region of the radius of the marginally stable circular orbit are identified. It is noted that its evolution into a large spherical cloud would require large velocities of the viscosity parameter and the amount of energy dissipated in the unstable region.

Stoeger, W. R.↗

On the formation and confinement of dense clouds in QSOs and active galactic nuclei

A model for the formation and confinement of dense (at least about 1 billion per cu cm) clouds in QSOs and active galactic nuclei is presented wherein thermal instabilities behind radiative shocks cause the collapse of regions where the preshock density is enhanced over that of the surrounding medium. Such shocks (of total energy around 10 to the 51st ergs) are likely to occur if the frequent optical outbursts observed in many of these objects are accompanied by mass ejections of comparable energy. It is found that clouds quite similar to those thought to exist in QSOs etc. can be created in this manner at radii of the order of 10 to the 17th cm. The clouds can be subsequently accelerated to observed bulk velocities by either radiation pressure or a collision with a much stronger (total energy around 10 to the 53 ergs) shock. Alternatively, their high observed velocities could be caused by gravitational infall or rotation. The mass production required at inner radii by the outflow models can be supplied through a mechanism previously discussed by Shields (1977).

Marscher, A. P.↗

Radio-frequency heating of emission-line gas near compact extragalactic radio sources

High-brightness-temperature radio sources significantly heat by free-free absorption any nearby gas that has properties similar to those inferred for QSO emission-line gas. As a result, the outer layers of the gas clouds expand, and their visible line emission decreases. Moderate heating enhances the collisionally excited ultraviolet line of O VI at 1034 A. Stronger heating penetrates the entire cloud and extinguishes all lines. Strong enough radio fluxes cause a thermal instability by stimulated Compton heating that is only saturated by Compton cooling at very high temperatures. It is speculated that BL Lac objects differ from quasars by having higher radio turnover frequencies, lower gas pressures, or more violent variability, all of which make radio heating more effective.

Krolik, J. H.↗

Thermonuclear runaways on neutron stars

Thermonuclear runaways which develop when neutron stars of 0.476 solar masses accrete hydrogen-rich material at 10 to the -10th and 2 x 10 to the -9th solar masses/year have been followed using a numerical model. It is found that a thermal instability occurs at densities in excess of 10 to the 5th g/cu cm and that the maximum accumulated mass required to initiate the runaway is 0.7 x 10 to the -12th and 2.1 x 10 to the -12th solar masses for the mass accretion rates of 10 to the -10th and 2 x 10 to the -9th solar masses/year, respectively. Heating the of the neutron star envelope by hydrogen burning leads to the ignition of helium. The nonequilibrium burning of helium by a combination of (alpha, p), (p, gamma), and (alpha, gamma) reactions involving O-14, O-15, and other heavy nuclei provides the energy for an X-ray burst. The gross properties of these models bear suggestive resemblance to those observed for some X-ray burst sources.

Taam, R. E.↗