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DOE OSTI2023

Kinetics and mechanism of light-induced phase separation in a mixed-halide perovskite

Halide ion phase separation is a barrier to the application of mixed-halide perovskites, whereby the presence of large populations of photo-generated or injected carriers causes undesirable changes in the local band gap. Here, we investigate the mechanism of phase separation in CsPbI x Br 3-x perovskite single crystals driven by light. The phase separation process and its dynamics are visualized at the nanometer scale at cryogenic temperatures using in-situ scanning transmission electron microscopy and cathodoluminescence. Combined with phase field modeling that accounts for the coupling between electronic and chemical driving forces, our observations point to a spinodal decomposition mechanism in which both the amplitude of composition fluctuation and the characteristic length scale grow non-linearly with time. Our findings provide microscopic insights that can assist in further engineering mixed-halide perovskites either for stability or for intentional programming of the local halide ion composition, opening pathways to a wide range of applications.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Probing eddy size and its effective mixing length in stably stratified roughness sublayer flows

Stably stratified roughness sublayer flows are ubiquitous yet remain difficult to represent in models and to interpret using field experiments. Here, continuous high-frequency potential temperature profiles from the forest floor up to 6.5 times the canopy height observed with distributed temperature sensing (DTS) are used to link eddy topology to roughness sublayer stability correction functions and coupling between air layers within and above the canopy. The experiments are conducted at two forest stands classified as hydrodynamically sparse and dense. Near-continuous profiles of eddy sizes (length scales) and effective mixing lengths for heat are derived from the observed profiles using a novel conditional sampling approach. The approach utilizes potential temperature isoline fluctuations from a statically stable background state. The transport of potential temperature by an observed eddy is assumed to be conserved (adiabatic movement) and we assume that irreversible heat exchange between the eddy and the surrounding background occurs along the (vertical) periphery of the eddy. This assumption is analogous to Prandtl's mixing-length concept, where momentum is transported rapidly vertically and then equilibrated with the local mean velocity gradient. A distinct dependence of the derived length scales on background stratification, height above ground, and canopy characteristics emerges from the observed profiles. Implications of these findings for (1) the failure of Monin–Obukhov similarity in the roughness sublayer and (2) above-canopy flow coupling to the forest floor are examined. The findings have practical applications in terms of analysing similar DTS data sets with the proposed approach, modelling roughness sublayer flows, and interpreting nocturnal eddy covariance measurements above tall forested canopies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Models and Algorithms for Equilibrium Analysis of Mixed-Material Nucleic Acid Systems

Dynamic programming algorithms within the NUPACK software suite enable analysis of equilibrium base-pairing properties for complex and test tube ensembles containing arbitrary numbers of interacting nucleic acid strands. Currently, calculations are limited to single-material systems that are either all-RNA or all-DNA. Here, to enable analysis of mixed-material systems that are critical for modern applications in vitro, in situ, and in vivo, we develop physical models and dynamic programming algorithms that allow the material of the system to be specified at nucleotide resolution. Free energy parameter sets are constructed for both RNA/DNA and RNA/2'OMe-RNA mixed-material systems by combining available empirical mixed-material parameters with single-material parameter sets to enable treatment of the full complex and test tube ensembles. New dynamic programming recursions account for the material of each nucleotide throughout the recursive process. For a complex with N nucleotides, the mixed-material dynamic programming algorithms maintain the O(N 3 ) time complexity of the single-material algorithms, enabling efficient calculation of diverse physical quantities over complex and test tube ensembles (e.g., complex partition function, equilibrium complex concentrations, equilibrium base-pairing probabilities, minimum free energy secondary structure(s), and Boltzmann-sampled secondary structures) at a cost increase of roughly 2.0-3.5×. The results of existing single-material algorithms are exactly reproduced when applying the new mixed-material algorithms to single-material systems. Accuracy is significantly enhanced using mixed-material models and algorithms to predict RNA/DNA and RNA/2'OMe-RNA duplex melting temperatures from the experimental literature as well as RNA/DNA melt profiles from new experiments. In conclusion, mixed-material analyses can be performed online using the NUPACK web app (www.nupack.org) or locally using the NUPACK Python module.

2′OMe-RNA↗

NASA NTRS2010

Possible Influences of Air Pollution, Dust and Sandstorms on the Indian Monsoon

In Asian monsoon countries, such as China and India, human health and safety problems caused by air pollution are becoming increasingly serious, due to the increased loading of atmospheric pollutants from waste gas emissions and from rising energy demand associated with the rapid pace of industrialization and modernization. Meanwhile, uneven distribution of monsoon rain associated with flash floods or prolonged drought, has caused major loss of human life and damage to crops and.property with devastating societal impacts. Historically, air-pollution and monsoons research are treated as separate problems. However recent studies have suggested that the two problems may be intrinsically linked and need to be studied jointly. Fundamentally, aerosols can affect precipitation through radiative effects cif suspended particles in the atmosphere (direct effect) and/or by interfering and changing: the cloud and precipitation formation processes (indirect effect). Based on their optical properties, aerosols can be classified into two types.: those that absorb solar radiation, and those that do not. Both types of aerosols scatter sunlight and reduce the amount of solar radiation from reaching the Earth's surface, causing it to cool. The surface cooling increases atmospheric stability and reduces convection potential, Absorbing aerosols, however, in addition to cooling the surface, can heat the atmosphere. The heating of the atmosphere may reduce the amount of low clouds by increased evaporation in cloud drops. The heating, however, may induce rising motion, enhance low-level moisture, convergence and, hence, increases rainfall, The latent heating from enhanced rainfall may excite feedback processes in the large-scale circulation, further amplify.the initial response to aerosol heating and producing more rain. Additionally, aerosols can increase the concentration of cloud condensation nuclei (CCN), increase cloud amount and decrease coalescence and collision rates, leading to reduced precipitation. However, in the presence of increasing moist and warm air, the reduced coalescence/collision may lead to supercooled drops at higher altitudes where ice precipitation falls and melts. The latent heat release from freezing aloft and melting below implies greater upward heat transport in polluted clouds and invigorate deep convection. In this way, aerosols may lead to increased local convection. Hence, depending on the ambient large-scale conditions and dynamical feedback processes, aerosols' effect on precipitation can be positive, negative or mixed. In the Asian monsoon and adjacent regions, the aerosol forcing and responses of the water cycle are even more complex, Both direct and indirect effects may take place locally and simultaneously, interacting with each other. in addition to local effects, monsoon rainfall may be affected by aerosols transported from other regions and intensified through large-scale circulation and moisture feedback. Thus, dust transported by the large-scale circulation from the adjacent deserts to northern India may affect rainfall over the Bay of Bengal; sulphate and black carbon front industrial pollution in central, southern China and northern India may affect the rainfall regime over the Korean peninsula and Japan; organic and black carbon front biomass burning from Indo-China may modulate the pre-monsoon rainfall regime over southern China and coastal regions, contributing to variability in differential heating and cooling of the atmosphere and to the land-sea thermal contrast. During the pre-monsoon season and monsoon breaks, it has been suggested that radiative forcing by absorbing aerosols have nearly the same order of magnitude as the forcing due to latent heating from convection and surface fluxes. The magnitude of the total aerosol radiative cooling due to sulphates and soot is of the order of 20-40 W/m2 over the Asian monsoon land region in the pre-monsoon season, compared to about 1-2 W/m2 for global warng. However, the combined forcing at the surface and in the atmosphere, including all species. if aerosols, and details of aerosol mixing, and impacts on the energy and water cycles in the monsoon land regions, are not well known.

Lau, William K. M.↗

DOE OSTI2021

Compositional patterning in irradiated alloys: Effective potentials and effective interfacial energy

Compositional patterning (CP) in binary alloys during energetic particle irradiation is studied using a kinetic model that considers two competing kinetic processes, a thermally activated one promoting macroscopic phase separation (MPS) of the concentration field c(r,t) and a forced one resulting in finite-range random atomic mixing. The forced mixing is modeled by a Gaussian relocation distribution with a characteristic distance R. A series of approximate kinetic models are introduced by expanding the mixing function into a series of n terms, thus replacing the non-local evaluations of the concentration field c(r'-r,t) by local derivatives of c(r,t). This approach makes it possible to obtain exact effective potentials and build steady-state diagrams for each order-n model. Phase field (PF) simulations using these order-n models reveal that near the onset of patterning, phase evolution is accurately described using an order-3 model, which changes smoothly from an extended Cahn-Hilliard free energy in the MPS regime to a one-mode Swift-Hohenberg functional in the CP regime. Deeper into the patterning regime, higher-order models are required to achieve convergence, yielding square-like concentration profiles characteristic of a strong segregation regime. These higher-order effective free energies are analogous to multimodal Swift-Hohenberg functionals. Here, a new definition for the effective interfacial energy is proposed in the CP regime, since the interfacial area is no longer an excess quantity in that regime, precluding the use of the standard thermodynamic definition of interfacial energy.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Excitation spectrum and low-temperature magnetism in the disordered defect-fluorite Ho2⁢Zr2⁢O7

In this work, we report on the thermomagnetic characterization and crystalline-electric field (CEF) energy scheme of the disordered defect-fluorite Ho2⁢Zr2⁢O7. This structural phase is distinguished by the coexistence of magnetic frustration and extensive disorder, with Ho3+ and Zr4+ sharing randomly the same 4⁢𝑎 site with even 50% occupancy, and an average 1/8 oxygen vacancy per unit cell. AC magnetic susceptibility measurements performed on powder samples down to 0.5 K revealed signs of slowing spin dynamics without glassy behavior, including a frequency dependent peak at ∼1K. Yet, no evidence for long-range magnetic order is found down to 200 mK in the specific heat. Inelastic neutron scattering measurements show a weak, low-lying CEF excitation around 2 meV, accompanied by a broad level centered at 60 meV. To fit our observations, we propose an approach to account for structural disorder in the crystal-field splitting of the non-Kramers Ho3+. Our model provides an explanation to the broadening of the high-energy, single-ion excitations and suggests that the zirconate ground-state wavefunction has zero magnetic moment. Through the breaking of local symmetry, structural disorder enables the magnetic response observed in Ho2⁢Zr2⁢O7, allowing the mixing of low-lying states at finite temperatures. Finally, we show that this scenario is in good agreement with the bulk properties reported in this work.

Gardner, Jason [ORNL] (ORCID:0000000278234072)↗

DOE OSTI2024

Coherent homodyne detection for amplified cross-beam electric-field induced second harmonic

The electric-field induced second harmonic (E-FISH) signal sensing is commonly used as a nonlinear optical technique to probe electric fields inside a plasma region. Cross-beam E-FISH is being investigated to improve spatial resolution by defining the interaction volume via a controlled geometry of two overlapping noncolinear optical beams. This drastic reduction in interaction length of the electric field and laser region results in a significant signal reduction. Here, to overcome this signal reduction, we introduce coherent amplification of the cross-beam E-FISH signal by mixing the low E-FISH signal with a phase-locked bright local oscillator. We demonstrate enhancement of the signal. By introducing a local oscillator we can now derive the polarity of the measured electric field through the phase of the homodyne signal. To illustrate the technique, we, for the first time, to the best of our knowledge, measure the magnitude and the direction of the electric field in a cold atmospheric pressure plasma jet, which dynamically follows the profile of the applied bias current.

42 ENGINEERING↗

NASA NTRS1972

Interaction between an upstream facing wall jet and a supersonic stream

The flow field resulting from the interaction of an upstream facing wall jet with a supersonic counterflowing stream has been investigated. A flow field model and the main parameters governing the phenomena were determined from quantitative and qualitative experimental observations. Experimental results for different ranges of the main parameters are presented. A theoretical analysis was performed to describe the flow field in the mixing region between the two counterflowing streams. The results obtained by applying a locally similar solution compare favorably with the experimentally measured values. Large values of jet penetration were obtained with a high subsonic or low supersonic jet; large interaction forces are characteristics of higher supersonic injections. For the case of large penetration the cooling effectiveness presented as a function of the main parameters indicates the possibility of interacting cooling applications.

Piva, R.↗

NASA NTRS1974

Impact-induced fractionation in the lunar highlands

A synthesis of the relevant data concerning lunar highland polymict breccias from the fields of petrography, chemistry, photogeology, and impact studies compels the prediction that the breccias should have homogeneous matrices from rock to rock within regions of the highlands of limited size where impact mixing has been efficient and extensive. But the matrices of returned breccias, even from one landing site, display a wide range in composition. This incompatibility between prediction and observation is a paradox that may be resolved by a process that acts after impact mixing to cause a differentiation of the breccia compositions. Partial melting of the local surficial material, and separation of melt and residue in ejecta and/or fall-back blankets, is compatible with the reviewed data and may resolve the paradox.

Warner, J. L.↗

NASA NTRS1977

Lunar highland rock types: Their implications for impact-induced fractionation

Lunar rocks may be classified into three major groups: (1) coarse-grained igneous rocks, (2) fine-grained igneous rocks, and (3) breccias. Group 1 is interpreted as primitive lunar crustal rocks that display various degrees of crushing and/or annealing. Group 2 is interpreted as volcanic rocks. Group 3 is interpreted as resulting from impacts on the lunar surface and is subdivided on the basis of matrix textures into fragmental breccias, crystalline breccias that have been annealed, and crystalline breccias with igneous matrices. A synthesis of the data concerning lunar highlands polymict breccias compels the prediction that the breccias should have homogeneous matrices from rock to rock within regions of the highlands of limited size where impact mixing has been efficient and extensive. But the returned breccias, even from one landing site, display a wide range in composition. This incompatibility between prediction and observation is a paradox that may be resolved by a process that acts after impact mixing to cause a differentiation of the breccia compositions. Partial melting of the local average crustal composition (as modeled by the average soil composition for each site) and separation of melt and residue in ejecta and/or fall-back blankets are compatible with the reviewed data and may resolve the paradox.

Phinney, W. C.↗

NASA NTRS1977

Stress intensities for cracks emanating from pin-loaded holes

A series of stress freezing photoelastic experiments were conducted on large plates containing central holes with cracks emanating from the edge formed by the intersection of the hole with the plate surface. Loads were applied through rigid pins with neat fits in the holes. Stress-intensity factors (SIF) were estimated by a computer assisted least squares analysis of the photoelastic data taken from slices near the points of intersection of the flaw border with the hole boundary and the plate surface. Results indicate that the local mode of loading changes from Mode 1 near the hole boundary to mixed mode near the plate surface. The analysis is extended to include mixed mode loading, and results are compared with an existing approximate theory.

Smith, C. W.↗

NASA NTRS1992

Physical properties of Meridiani Sinus-type units in the central equatorial region of Mars

Classification and mapping of surficial units in the central equatorial region of Mars (30 degrees N to 20 degrees S, 57 degrees E to 75 degrees W) using enhanced color images and Mars Consortium data identified four major color/albedo units in the dark, reddish-gray regions that form the classical dark albedo markings of Mars, including Meridiani Sinus. The darkest, least red (relatively 'blue') materials form splotches (some with dune forms) in craters, inter-crater depressions, and part of Valles Marineris. These form the 'Dark Blue' Meridiani unit. Abundant materials that have higher albedos and are somewhat redder than the 'Dark Blue' unit have uniquely high green/(violet + red) color ratios in Viking Orbiter images. These materials, named 'Green-blue' Meridiani surround and mix with 'Dark Blue' Meridiani patches and are abundant on crater rims and local elevations. Discontinuous, patchy deposits with still higher albedos and much redder colors have morphologies classified of the Type Ib bright depositional dust streaks and sheets that were classified by Thomas et al. These dust deposits, which appear to be optically thin and patchy and are darker and not as red as other Type Ib dust deposits on Mars, and their Meridiani substrates, were designated the 'Red' Meridiani unit. Distinctive deposits that form highly eroded mesas and escarpments in northern Meridiani Sinus were named 'Light Blue' Meridiani, since they are not as red as other materials with moderately high albedos. Large areas dominated by these units form Meridiani Province in the central equatorial region of Mars.

Strickland, Edwin L., III↗

NASA NTRS1994

Characteristics of a trapped-vortex (TV) combustor

The characteristics of a Trapped-Vortex (TV) combustor are presented. A vortex is trapped in the cavity established between two disks mounted in tandem. Fuel and air are injected directly into the cavity in such a way as to increase the vortex strength. Some air from the annular flow is also entrained into the recirculation zone of the vortex. Lean blow-out limits of the combustor are determined for a wide range of annular air flow rates. These data indicate that the lean blow-out limits are considerably lower for the TV combustor than for flames stabilized using swirl or bluff-bodies. The pressure loss through the annular duct is also low, being less than 2% for the flow conditions in this study. The instantaneous shape of the recirculation zone of the trapped vortex is measured using a two-color PIV technique. Temperature profiles obtained with CARS indicate a well mixed recirculation zone and demonstrate the impact of primary air injection on the local equivalence ratio.

Hsu, K.-Y.↗

NASA NTRS1995

Observations of the CO bulge on Venus and implications for mesospheric winds

Observations of CO at 2.6 mm (115.27 GHz) were made with the Owens Valley Radio Observatory (OVRO) millimeter interferometer in 1986 and 1988, yielding high-quality disk-resolved spectra which were inverted to determine the CO mixing ratio profile from distinct regions on the disk, allowing us to map the distribution of CO in the upper mesosphere of Venus both horizontally and vertically. The 1986 observations were of the morning terminator and were particularly useful in searching for a suspected CO maximum ('bulge') on the nightside. The resulting CO mixing ratio profiles were mapped for various altitudes as functions of latitude and local time, and we report that we have resolved the previously inferred CO bulge. The bulge increases in magnitude from a small day-night variation at 90 km to an extensive nightside peak at 100 km, the upper limit of our observations. The peak bulge-to-dayside ratio approached 20-30 at 100 km in 1986 and may have been as large as 50-100, assuming late-afternoon CO abundances found in 1988 were similar to those in 1986. Three-dimensional mapping shows that in the upper mesosphere the bulge was displaced from local midnight toward the morning equator, centered at 3:30 AM local time. Using the qualitative model of mesospheric circulation on Venus proposed by Clancy and Muhleman (1985, 1991), we explain this shift in terms of strong retrograde zonal winds throughout the mesosphere, matching the directly detected mesospheric circulation (Shah, K., D. O. Muhleman, and G. L. Berge 1991) observed with the same dataset in 1988.

Gurwell, Mark A.↗

NASA NTRS1996

On modeling pressure diffusion in non-homogeneous shear flows

New models are proposed for the 'slow and 'rapid' parts of the pressure diffusive transport based on the examination of DNS databases for plane mixing layers and wakes. The model for the 'slow' part is non-local, but requires the distribution of the triple-velocity correlation as a local source. The latter can be computed accurately for the normal component from standard gradient diffusion models, but such models are inadequate for the cross component. More work is required to remedy this situation.

Demuren, A. O.↗

NASA NTRS2005

Skin-Stiffener Debond Prediction Based on Computational Fracture Analysis

Interlaminar fracture mechanics has proven useful for characterizing the onset of delaminations in composites and has been used with limited success primarily to investigate onset in fracture toughness specimens and laboratory size coupon type specimens. Future acceptance of the methodology by industry and certification authorities however, requires the successful demonstration of the methodology on structural level. For this purpose a panel was selected that is reinforced with stringers. Shear loading causes the panel to buckle and the resulting out-of-plane deformations initiate skin/stringer separation at the location of an embedded defect. For finite element analysis, the panel and surrounding load fixture were modeled with shell elements. A small section of the stringer foot and the panel in the vicinity of the embedded defect were modeled with a local 3D solid model. Across the width of the stringer foot the mixed-mode strain energy release rates were calculated using the virtual crack closure technique. A failure index was calculated by correlating the results with the mixed-mode failure criterion of the graphite/epoxy material. For small applied loads the failure index is well below one across the entire width. With increasing load the failure index approaches one first near the edge of the stringer foot from which delamination is expected to grow. With increasing delamination lengths the buckling pattern of the panel changes and the failure index increases which suggests that rapid delamination growth from the initial defect is to be expected.

Krueger, Ronald↗

NASA NTRS2006

Analysis of Composite Panel-Stiffener Debonding Using a Shell/3D Modeling Technique

Krueger, Ronald↗

NASA NTRS2006

Fuel-air mixing apparatus for reducing gas turbine combustor exhaust emissions

A fuel-air mixer for use in a combustion chamber of a gas turbine engine is provided. The fuel air mixing apparatus comprises an annular fuel injector having a plurality of discrete plain jet orifices, a first swirler wherein the first swirler is located upstream from the fuel injector and a second swirler wherein the second swirler is located downstream from the fuel injector. The plurality of discrete plain jet orifices are situated between the highly swirling airstreams generated by the two radial swirlers. The distributed injection of the fuel between two highly swirling airstreams results in rapid and effective mixing to the desired fuel-air ratio and prevents the formation of local hot spots in the combustor primary zone. A combustor and a gas turbine engine comprising the fuel-air mixer of the present invention are also provided as well as a method using the fuel-air mixer of the present invention.

Zupanc, Frank J.↗