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DOE OSTI2023

Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes

Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm 2 , respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.

14 SOLAR ENERGY↗

DOE OSTI2019

Tetragonal C 24 : a topological nodal-surface semimetal with potential as an anode material for sodium ion batteries

Na-ion batteries, as an alternative to Li-ion batteries, have gained increasing attention due to the abundance of sodium and its low cost. In the present work, we prepare a 3D porous carbon material by inserting hexagonal carbon rings into sp 3 C–C bonds in a previously established 3D-(4,4) lattice, termed tC 24 . Ab initio calculations uncover that not only is tC 24 thermally, dynamically and mechanically stable, but it also exhibits a unique electronic band structure with two topological nodal surfaces traversing through the whole Brillouin zone. More importantly, tC 24 is the first all carbon topological nodal-surface semimetal for Na-ion batteries, exhibiting a high theoretical capacity of 232.65 mA h g -1 , a low diffusion energy barrier for Na ions, an appropriate average voltage of 0.54 V and a negligible volume change (~0.94%) during charging/discharging operation. These properties provide tC 24 with a potentially long cycling life when used as an anode material for Na-ion batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

The genetic architecture of leaf stable carbon isotope composition in Zea mays and the effect of transpiration efficiency on leaf elemental accumulation

With increased demand on freshwater resources for agriculture, it is imperative that more water-use efficient crops are developed. Leaf stable carbon isotope composition, δ 13 C, is a proxy for transpiration efficiency and a possible tool for breeders, but the underlying mechanisms effecting δ 13 C in C 4 plants are not known. It has been suggested that differences in specific leaf area (SLA), which potentially reflects variation in internal CO 2 diffusion, can impact leaf δ 13 C. Furthermore, although it is known that water movement is important for elemental uptake, it is not clear how manipulation of transpiration for increased water-use efficiency may impact nutrient accumulation. Here, we characterize the genetic architecture of leaf δ 13 C and test its relationship to SLA and the ionome in five populations of maize. Five significant QTL for leaf δ 13 C were identified, including novel QTL as well as some that were identified previously in maize kernels. One of the QTL regions contains an Erecta-like gene, the ortholog of which has been shown to regulate transpiration efficiency and leaf δ 13 C in Arabidopsis. QTL for δ 13 C were located in the same general chromosome region, but slightly shifted, when comparing data from two different years. Our data does not support a relationship between δ 13 C and SLA, and of the 19 elements analyzed, only a weak correlation between molybdenum and δ 13 C was detected. Together these data add to the genetic understanding of leaf δ 13 C in maize and suggest that improvements to plant water use may be possible without significantly influencing elemental homeostasis.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1974

Development of an improved membrane for a vapor diffusion water recovery process

Recovery of potable water from urine on manned space missions of extended duration was the objective of work aimed at the improvement of membrane performance for the vapor diffusion process (VDR). Kynar, Teflon, PVC, and polysulfone candidate membranes were evaluated from chemical, thermal, mechanical, and fabricating standpoints to determine their suitability for operation in the VDR pervaporation module. Pervaporation rates and other performance characteristics were determined in a breadboard pervaporator test rig. Kynar and Teflon membranes were demonstrated to be chemically stable at pervaporation temperatures in urine pretreated with chromic acid bactericide. The separation of the pervaporator and condenser modules, the use of a recirculating sweep gas to conduct pervaporate to the condenser, and the selection of a hollow fiber membrane configuration for pervaporator module design is recommended as a result of the investigation.

Rich, T. R.↗

NASA NTRS1978

Induced junction solar cell and method of fabrication

An induced junction solar cell is fabricated on a p-type silicon substrate by first diffusing a grid of criss-crossed current collecting n+ stripes and thermally growing a thin SiO2 film, and then, using silicon-rich chemical vapor deposition (CVD), producing a layer of SiO2 having inherent defects, such as silicon interstices, which function as deep traps for spontaneous positive charges. Ion implantation increases the stable positive charge distribution for a greater inversion layer in the p-type silicon near the surface. After etching through the oxide to parallel collecting stripes, a pattern of metal is produced consisting of a set of contact stripes over the exposed collecting stripes and a diamond shaped pattern which functions as a current collection bus. Then the reverse side is metallized.

Maserjian, J.↗

NASA NTRS1992

Growth and decay of disturbances in stratified shear flow in a rotating frame

The stability of stratified plane Couette flow in a rotating frame is investigated for a case in which the gravitational force is parallel to the rotation vector. Partial differential equations describing the behavior of disturbances in the linear regime are derived. Unstratified flow is stable as long as the angular momentum gradient is positive. If the gradient is negative, nonaxisymmetric disturbances grow as a power law in time, if the gradient is sufficiently steep. In flow which is unstable to convection, all perturbations asymptotically grow at the rate given by the Brunt-Vaisala frequency. If heat diffusion is included, all nonaxisymmetric perturbations now eventually decay as t exp -2, even if the flow is unstable to convection. If heat diffusion and viscosity are weak, nonaxisymmetric disturbances in convectively unstable flow will undergo a large transient growth before their eventual decay.

Korycansky, D. G.↗

NASA NTRS1995

A turbulence module for the NPARC code

A turbulence module is developed for the 2D version of the NPARC code which is currently restricted to planar or axisymmetric flows without swirling. Four turbulence models have been built into the module: Baldwin-Lomax, Chien, Shih-Lumley and CMOTT models. The first is a mixing-length eddy-viscosity model which is mainly used for initialization of computational fields and the last three are the low Reynolds number two-equation models. Unlike chien's model, both the Shih-Lumley and CMOTT models do not involve the dimensionless wall distance y(sup +), an advantage for separated flow calculations. Contrary to the NPARC and most other compressible codes, the non-delta form of transport equations is used which leads to a simpler linearization and is more effective than using the delta form in ensuring the positiveness of the turbulent kinetic energy and its dissipation rate. To reduce numerical diffusion while maintaining necessary stability, a second-order accurate and bounded scheme is used for the convective terms of the turbulent transport equations. This scheme is implemented in a deferred correction manner so that the main coefficients of the resulting difference equations are always positive, thus making the numerical solutions process unconditionally stable. The system of equations is solved via a decoupled method and by the alternating direction TDMA of Thomas. The module can be easily linked to the NPARC code for turbulent flow calculations.

Zhu, J.↗

DOE OSTI2022

Faster ablative Kelvin–Helmholtz instability growth in a magnetic field

Shear flows along a plasma interface will quickly grow unstable due to the Kelvin–Helmholtz instability. If there is a concurrent temperature gradient across the interface, higher modes are stabilized by the thermal diffusion. These ablative effects must be considered in, for example, jet features in inertial confinement fusion hot-spots, or plasma plumes in young supernovae. We show that magnetization of the plasma can greatly affect the instability, even if magnetic pressure is small. This is because electrons are localized by their gyromotion, reducing the heat flux and material ablation. We use a two-dimensional numerical extended-magnetohydrodynamics approach to assess this effect for dense fusion conditions. In comparison with the unmagnetized case, self-generated Biermann fields make only a minor difference to growth rates. However, simulations with a large 50 kT external field found that the growth rate of the least stable mode increased by 40%. In conclusion, this has implications for mix processes in Z-pinches and magnetized inertial confinement fusion concepts.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Characterization of UV optical components for photon detector calibration in liquid argon TPCs

Large liquid argon time projection chambers (LArTPCs)require stable and well-characterized delivery of ultraviolet (UV)light for in situ calibration of photosensors at cryogenictemperatures. This article reports bench-top and cryogenicmeasurements of the optical components used in a UV lightcalibration system, including multi-mode fused-silica fibers,SMA-to-SMA connectors, optical fiber feedthroughs, andlight-diffuser assemblies. Light loss in several fiber types and SMAconnectors was measured across wavelengths from275–970 mm. In addition,light-loss measurements of the tested fibers after severalliquid-nitrogen thermal cycles showed no statistically significantdegradation relative to baseline measurements, and high-rate pulsedexposure (30–90 million pulses from a275 nm LED) likewise showed nomeasurable aging in jacketed fibers. A compact, palm-sized,3D-printed PEEK diffuser housing with stacked UV-grade fused-silicadiffusers yields Lambertian emission and the most uniform angulardistribution. Optical components exhibiting improved UV transmissionwere deployed successfully in multiple DUNE small- and large-scaleprototypes, demonstrating reliable operation of UV light calibrationsystem. These findings inform component selection and calibrationprocedures for achieving reliable, uniform UV light delivery inlarge-scale cryogenic detectors such as DUNE.

Behera, B. [South Dakota Sch. Mines Tech.] (ORCID:↗

DOE OSTI2020

Extended families of critical and stationary droplets for nonequilibrium phase transitions in spatially discrete bistable systems

Bistable nonequilibrium systems are realized in catalytic reaction-diffusion processes, biological transport and regulation, spatial epidemics, etc. Behavior in spatially continuous formulations, described at the mean-field level by reaction-diffusion type equations (RDEs), often mimics that of classic equilibrium van der Waals type systems. When accounting for noise, similarities include a discontinuous phase transition at some value, p eq , of a control parameter, p , with metastability and hysteresis around p eq . For each p , there is a unique critical droplet of the more stable phase embedded in the less stable or metastable phase which is stationary (neither shrinking nor growing), and with size diverging as p → p eq . Spatially discrete analogs of these mean-field formulations, described by lattice differential equations (LDEs), are more appropriate for some applications, but have received less attention. It is recognized that LDEs can exhibit richer behavior than RDEs, specifically propagation failure for planar interphases separating distinct phases. Herein, we show that this feature, together with an orientation dependence of planar interface propagation also deriving from spatial discreteness, results in the occurrence of entire families of stationary droplets. The extent of these families increases approaching the transition and can be infinite if propagation failure is realized. In addition, there can exist a regime of generic two-phase coexistence where arbitrarily large droplets of either phase always shrink. Such rich behavior is qualitatively distinct from that for classic nucleation in equilibrium and spatially continuous nonequilibrium systems.

97 MATHEMATICS AND COMPUTING↗

NASA NTRS1971

Observations of low-energy /0.3- to 1.8-MeV/ differential spectrums of trapped protons.

Measurements of differential energy spectrums of trapped protons obtained from several passes during the period January to November 1969 using the polar orbiting, low-altitude Injun 5 satellite equipped with a special solid-state detector proton-electron telescope are presented. Results reveal the existence of a quasi-persistent peak in the differential energy spectrum in the McIlwain shell parameter (L) range 2 to 2.6 and in the energy range of approximately 0.32 to 0.72 MeV. The fact that the shape of the spectrum is stable for several days or can change with time scales as small as 4 hours suggests an impulsive acceleration mechanism deep in the radiation belts. Other features of the spectrum show that if the spectrum is represented by an exponential form in energy, the dependence of the spectral parameter is in general agreement with diffusion theory over the L range of approximately 2 to 4.

Venkatesan, D.↗

NASA NTRS1974

The atmospheres of Titan and the Galilean satellites

The stability of various atmospheres on Titan and the Galilean satellites is examined relative to escape. One method consists of the comparison of exospheric temperature and a blow-off temperature defined for the various constituents. Another method consists of the evaluation of outflow based on a polytropic model. Hydrogen, methane, nitrogen, and neon atmospheres are examined. It is found that the Jovian satellites require heavier gases if they are to have any but very tenuous atmospheres, since all constituents examined are unstable. Nitrogen is stable on Titan, but methane and neon are marginally stable. Hydrogen is extremely unstable as a major constituent. As a minor constituent it is rapidly lost from Titan's thermosphere and must be replenished by outgassing or dissociation of a hydrogen compound, if the presently observed hydrogen content on Titan is not a transient occurrence. The rate of loss may be limited by diffusion, but could be augmented by vertical convection.

Gross, S. H.↗

NASA NTRS1993

An extended Lagrangian method

A unique formulation of describing fluid motion is presented. The method, referred to as 'extended Lagrangian method', is interesting from both theoretical and numerical points of view. The formulation offers accuracy in numerical solution by avoiding numerical diffusion resulting from mixing of fluxes in the Eulerian description. Meanwhile, it also avoids the inaccuracy incurred due to geometry and variable interpolations used by the previous Lagrangian methods. The present method is general and capable of treating subsonic flows as well as supersonic flows. The method proposed in this paper is robust and stable. It automatically adapts to flow features without resorting to clustering, thereby maintaining rather uniform grid spacing throughout and large time step. Moreover, the method is shown to resolve multidimensional discontinuities with a high level of accuracy, similar to that found in 1D problems.

Liou, Meng-Sing↗

NASA NTRS2007

Wind Tunnel Investigation of the Effects of Surface Porosity and Vertical Tail Placement on Slender Wing Vortex Flow Aerodynamics at Supersonic Speeds

A wind tunnel experiment was conducted in the NASA Langley Research Center (LaRC) Unitary Plan Wind Tunnel (UPWT) to determine the effects of passive surface porosity and vertical tail placement on vortex flow development and interactions about a general research fighter configuration at supersonic speeds. Optical flow measurement and flow visualization techniques were used that featured pressure sensitive paint (PSP), laser vapor screen (LVS), and schlieren, These techniques were combined with conventional electronically-scanned pressure (ESP) and six-component force and moment measurements to quantify and to visualize the effects of flow-through porosity applied to a wing leading edge extension (LEX) and the placement of centerline and twin vertical tails on the vortex-dominated flow field of a 65 cropped delta wing model. Test results were obtained at free-stream Mach numbers of 1.6, 1.8, and 2.1 and a Reynolds number per foot of 2.0 million. LEX porosity promoted a wing vortex-dominated flow field as a result of a diffusion and weakening of the LEX vortex. The redistribution of the vortex-induced suction pressures contributed to large nose-down pitching moment increments but did not significantly affect the vortex-induced lift. The trends associated with LEX porosity were unaffected by vertical tail placement. The centerline tail configuration generally provided more stable rolling moments and yawing moments compared to the twin wing-mounted vertical tails. The strength of a complex system of shock waves between the twin tails was reduced by LEX porosity.

Erickson, Gary E.↗

DOE OSTI2019

Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO 2 via introducing strong electronic metal-support interaction for efficient CO 2 photoreduction

This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO 2 -V O (V O : oxygen vacancy) for gas-phase CO 2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO 2 -V O in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO 2 -V O resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO 2 -V O . The optimized Pt/TiO 2 -V O demonstrated a high quantum yield of 1.49% with high CH 4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO 2 -V O and Pt/TiO 2 . More importantly, the EMSI also played a critical role in preserving the surface metallic Pt 0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO 2 -V O , whereas rapid catalytic deactivation are observed for both TiO 2 -V O and Pt/TiO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries

The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni 2 P electrocatalyst supported on N, P co-doped graphene (Ni 2 P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni 2 P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li 2 S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni 2 P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm –2 , the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Nanoengineered Shape-Memory Hemostat

Uncontrolled hemorrhage is the predominant cause of preventable combat deaths. Various biomaterials serve as hemostatic agents due to their procoagulant or absorptive activity. However, these biomaterials often lack expansion capabilities, which severely limits use in noncompressible wounds. This study combines a hemostatic nanocomposite with a shape-memory polymer foam to design a composite material with both hemostatic and physical expansion properties. This composite is fabricated in two formulations: a foam externally coated in a highly concentrated nanocomposite (“coated composite”) and a foam containing a diluted nanocomposite infused throughout its pores (“infused composite”). Both formulations retain the shape-memory foam's expansion property. Further, the coated composite shows improved fluid uptake (>2-fold) versus infused composites or foam. The nanocomposite component dissociates from the foam under degradative conditions, with the foam remaining stable for 30 days. Hemostatic studies illustrate that the coated composite reduces the clotting time by ≈20%. Alternatively, the infused composite improves clotting over a larger distance (up to ≈2× distance from the composite). These results signify a modular hemostatic ability: the coated composite reduces clotting and improves fluid uptake, while the infused composite achieves diffuse clotting and maintains mechanical properties. Thus, these materials pose a strong potential for use in noncompressible wounds.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2024

Study of Void Formation at the Lithium|Solid Electrolyte Interface

There is growing recognition of the critical role of void formation in lithium metal anodes in solid-state batteries and its impact on electrochemical performance. While experimental studies have demonstrated the challenges ensuing from void formation at the lithium metal interface with the solid electrolyte, there is a need to understand and quantify the role of intrinsic transport properties in lithium metal and the impact of external stimuli, such as temperature, pressure, and current density. Here, we develop this understanding by constructing a phase field-based model that captures the evolution of void domains at the lithium-solid electrolyte interface. Growth of the pores is driven by the fast removal of lithium from the interface during stripping at high current densities. Relative magnitudes of the bulk and surface lithium diffusivities, along with the applied current density, dictate the final pore morphology. Increasing the temperature results in faster diffusion, while external applied pressure causes creep flow of lithium, both of which help to mitigate the evolution of voids by quickly transporting metal from the bulk to the interface. Finally, a phase map as a function of temperature and pressure is developed as a guide to determine the regions that can lead to the stable cycling of lithium metal.

25 ENERGY STORAGE↗