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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 127 records · Page 7

Highly Efficient Pure‐Blue Light‐Emitting Diodes Based on Rubidium and Chlorine Alloyed Metal Halide Perovskite

Abstract Perovskite light‐emitting diodes (PeLEDs) are promising candidates for display and solid‐state lighting, due to their tunable colors, high conversion efficiencies, and low cost. However, the performance of blue PeLEDs is far inferior to that of the near‐infrared, red, and green counterparts. Here, the fabrication of pure‐blue PeLEDs with an emission peak at 475 nm, a peak external quantum efficiency of 10.1%, and a maximum luminance of 14 000 cd m −2 is demonstrated by tailoring the compositions of perovskites. The pure‐blue electroluminescence is achieved by simultaneous addition of rubidium and chlorine ions into CsPbBr 3 and incorporation of phenylethylammonium chloride forms quasi‐2D hybrid perovskites. The combination of these composition engineering results in blueshifted emissions without reducing the quantum yield. The judicious alloying is shown to be critical to result in the better morphology with suppressed current leakage and enhanced light outcoupling.

Yang, Yang↗

Novel High Efficient Organic Photovoltaic Materials

Solar energy is a renewable, nonpolluting, and most abundant energy source for human exploration of a remote site or outer space. In order to generate appreciable electrical power in space or on the earth, it is necessary to collect sunlight from large areas and with high efficiency due to the low density of sunlight. Future organic or polymer (plastic) solar cells appear very attractive due to their unique features such as light weight, flexible shape, tunability of energy band-gaps via versatile molecular or supramolecular design, synthesis, processing and device fabrication schemes, and much lower cost on large scale industrial production. It has been predicted that supramolecular and nano-phase separated block copolymer systems containing electron rich donor blocks and electron deficient acceptor blocks may facilitate the charge carrier separation and migration due to improved electronic ultrastructure and morphology in comparison to polymer composite system. This presentation will describe our recent progress in the design, synthesis and characterization of a novel block copolymer system containing donor and acceptor blocks covalently attached. Specifically, the donor block contains an electron donating alkyloxy derivatized polyphenylenevinylene (RO-PPV), the acceptor block contains an electron withdrawing alkyl-sulfone derivatized polyphenylenevinylene (SF-PPV). The key synthetic strategy includes the synthesis of each individual block first, then couple the blocks together. While the donor block has a strong PL emission at around 560 nm, and acceptor block has a strong PL emission at around 520 nm, the PL emissions of final block copolymers are severely quenched. This verifies the expected electron transfer and charge separation due to interfaces of donor and acceptor nano phase separated blocks. The system therefore has potential for variety light harvesting applications, including high efficient photovoltaic applications.

Sun, Sam↗

Protection against Chemical Warfare Agents and Biological Threats Using Metal–Organic Frameworks as Active Layers

The SARS-CoV-2 pandemic outbreak and the unfortunate misuse of toxic chemical warfare agents (CWAs) highlight the importance of developing functional materials to protect against these chemical and pathogen threats. Metal–organic frameworks (MOFs), which comprise a tunable class of crystalline porous materials built from inorganic nodes and organic linkers, have emerged as a class of heterogeneous catalysts capable of rapid detoxification of multiple classes of these harmful chemical or biological hazards. In particular, zirconium-based MOFs (Zr-MOFs) feature Lewis acidic nodes that serve as active sites for a wide range of catalytic reactions, including the hydrolysis of organophosphorus nerve agents within seconds in basic aqueous solutions. In addition, postsynthetic modification of Zr-MOFs enables the release of active species capable of reacting with and deactivating harmful pathogens. Despite this impressive performance, utilizing Zr- MOFs in powder form is not practical for application in masks or protective uniforms. To address this challenge, our team sought to develop MOF/fiber composite systems that could be adapted for use under realistic operating conditions to protect civilians, military personnel, and first responders from harmful pathogens and chemical warfare agents. Over the last several years, our group has designed and fabricated reactive and biocidal MOF/fiber composites that effectively capture and deactivate these toxic species. In this Account, we describe the evolution of these porous and reactive MOF/fiber composites and focus on key design challenges and considerations. First, we devised a scalable method for the integration of Zr-MOFs onto textile substrates using aqueous precursor solutions and without using pretreated textiles, highlighting the potential scalability of this method. Moving beyond standard textiles, we also developed a microbial synthesis strategy to prepare hierarchically porous MOF/bacterial cellulose nanofiber composite sponges that can both capture and detoxify nerve agents when exposed to contaminated gas flows. The mass loading of the MOF in the nanofibrous composite sponge is up to 90%, affording higher work capacities compared to those of textile-fiber-based composites with relatively lower MOF loadings. Next, we demonstrated that heterogeneous polymeric bases are suitable replacements for volatile liquid bases typically used in solution-phase reactions, and we showed that these composite systems are capable of effectively hydrolyzing nerve agents in the solid state by using only water that is present as humidity. Moreover, incorporating a reactive dye precursor into the composite affords a dual function sensing and detoxifying material that changes color from white to orange upon reaction with the byproduct following nerve agent hydrolysis, demonstrating the versatility of this platform for use in decontamination applications. We then created chlorine-loaded MOF/fiber composites that act as biocidal and reactive textiles that are capable of not only detoxifying sulfur-mustard-based chemical warfare agents and simulants but also deactivating both bacteria and the SARS-CoV-2 virus within minutes of exposure. Lastly, we synthesized a mixed-metal Ti/Zr-MOF coating on cotton fibers to afford a photoactive biocidal cloth that shows fast and broad-spectrum biocidal performance against viruses and Gram-positive and Gram-negative bacteria under visible light irradiation. Given the tunable, multifunctional nature of these MOF/fiber composites, we believe that this Account will offer new insights for the rational design and preparation of functional MOF/fiber composites and pave the way toward the development of next-generation reactive and protective textiles.

36 MATERIALS SCIENCE↗

Control of Excitonic Energy Transfer in RGB Quantum Dot:Polymer Composites for Tunable White Emission

Tint-controlled white light is crucial for both illumination systems and display applications. Here, in this study, we demonstrate solution-processed quantum-dot light-emitting diodes (QD-LEDs) featuring a red–green–blue (RGB) QD–poly(methyl methacrylate) (PMMA) composite emissive layer (EML) for tunable white electroluminescence (EL). In this composite EML, PMMA functions as a dispersion matrix that modulates the interdot spacing (d), thereby controlling Förster resonance energy transfer (FRET) between QDs. By adjustment of the PMMA content, the balance of R, G, and B emissions is controlled, enabling systematic and continuous tuning of the EL color from greenish to reddish white at a fixed RGB ratio and constant driving bias. Time-resolved photoluminescence measurements confirm that the variation in the exciton lifetime with the PMMA fraction is the primary factor for tuning the EL color. Notably, nearly pure white EL with CIE coordinates close to (0.33, 0.33) is achieved using a diluted PMMA matrix without significant degradation of the electrical properties. Our results demonstrate d as an independent design parameter for decoupling color tuning from RGB composition and electrical operation, providing a versatile design framework for high-quality white- or tint-controlled QD-LEDs toward advanced solid-state lighting and display technologies.

36 MATERIALS SCIENCE↗

Probing and Tuning Strain‐Localized Exciton Emission in 2D Material Bubbles at Room Temperature

In monolayer transition metal dichalcogenides bubbles-nanoscale deformations typically exhibiting a dome-like shape-Excitons are confined by the strain effect, which exhibits extraordinary emission properties, such as single photon generation, enhanced light emission, and spectrally tunable excitonic states. While the strain profiles of these bubbles are extensively studied, this work provides an approach 1) to directly visualize the associated exciton properties in bubbles formed in WSe2 monolayer, revealing an intrinsic emission wavelength shift of ≈40 nm, and 2) actively modify local strain, enabling further exciton emission tuning over a range of 50 nm. These are achieved by emission mapping and nanoindentation using a dielectric near-field probe, which enables the detection of local emission spectra and emission lifetimes within individual bubbles. Statistical analysis of 67 bubbles uncovers an emission wavelength distribution centered around 780 nm. Furthermore, saturation behavior in the power-dependent studies and the associated lifetime change reveal the localized nature of the strain-induced states. These findings provide direct insights into the strain-localized emission dynamics in bubbles and establish a robust framework for non-destructive, reversible, and predictable nanoscale emission control, presenting a potential avenue for developing next-generation tunable quantum optical sources.

2D materials bubbles↗

Impact of Halogen Groups on the Properties of PEA–Based 2D Pb–Sn Halide Perovskites

Tuning broad emission in 2D Pb–Sn halide perovskites (HPs) is essential for advancing optoelectronic applications, particularly for color-tunable and white-light-emitting devices. This broad emission is linked to structural factors, such as defects and phase segregation of the Pb component within the Pb–Sn system, which are strongly influenced by the molecular structure and chemical properties of spacer cations. Atomic tuning of the spacers via halogenation opens up a new way to fine-tune the molecular properties, enabling further augmentations of HP functionalities. Nevertheless, the distinct broad emission's sensitivity to spacer chemistry remains underexplored. Here, halogenation's influence is systematically investigated on 2D HP emission characteristics using a high-throughput workflow. These findings reveal that the F-containing phenethylammonium (4F-PEA) spacer narrows the broadband PL, whereas Cl broadens it. Through a correlative study, it is found that 4F-PEA reduces not only the local phase segregation but also the defect levels and microstrains in 2D HPs. This is likely attributed to the manifestation of less lattice distortion via stronger surface coordination of the dipole-augmented 4F-PEA. Furthermore, these results highlight halogenation as a key factor in modulating phase segregation and defect density in 2D Pb–Sn HPs, offering a promising pathway to tune the emission for enhanced optoelectronic performance.

2D Pb-Sn halide perovskites↗

Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C 4 N 2 H 14 PbBr 4 by Pressure-Suppressed Nonradiative Loss

Low-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure–property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide C 4 N 2 H 14 PbBr 4 , and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations. Under a gigapascal pressure scale, the PL quantum yields (PLQYs) were quantitatively determined to show a dramatic increase from the initial value of 20% at ambient conditions to over 90% at 2.8 GPa. With in situ characterization of photophysical properties and theoretical analysis, we found that the PLQY enhancement was mainly attributed to the greatly suppressed nonradiative decay. Pressure can effectively tune the energy level of self-trapped states and increase the exciton binding energy, which leads to a larger Stokes shift. The resulting highly localized excitons with stronger binding reduce the probability for carrier scattering, to result in the significantly suppressed nonradiative decay. Overall, our findings clearly show that the characteristics of STEs in low-dimensional metal halides can be well-tuned by external pressure, and enhanced optical properties can be achieved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strain-engineered high-responsivity MoTe 2 photodetector for silicon photonic integrated circuits

In integrated photonics, specific wavelengths are preferred such as 1550 nm due to low-loss transmission and the availability of optical gain in this spectral region. For chip-based photodetectors, layered two-dimensional (2D) materials bear scientific and technologically relevant properties such as electrostatic tunability and strong light-matter interactions. However, no efficient photodetector in the telecommunication C-band has been realized with 2D transition metal dichalcogenide materials due to their large optical bandgap. Furthermore, we demonstrate a MoTe 2 -based photodetector featuring strong photoresponse (responsivity = 0.5 A/W -1 ) operating at 1550 nm in silicon photonics enabled by strain engineering the 2D material. Non-planarized waveguide structures show a locally-induced bandgap change of 0.2 eV inside MoTe 2 , resulting in large photo-response, in an otherwise photo-inactive medium when unstrained. Unlike Graphene-based photodetectors relying on a gapless band structure, this photodetector shows a ~100X improved dark current, enabling an efficient noise equivalent power of 90 pW/Hz -0.5 . Such strain-engineered integrated photodetector provides new opportunities for integrated optoelectronic systems.

47 OTHER INSTRUMENTATION↗

Elucidating the differences in oxidation of high-performance α- and β- diisobutylene biofuels via Synchrotron photoionization mass spectrometry

Abstract Biofuels are a promising ecologically viable and renewable alternative to petroleum fuels, with the potential to reduce net greenhouse gas emissions. However, biomass sourced fuels are often produced as blends of hydrocarbons and their oxygenates. Such blending complicates the implementation of these fuels in combustion applications. Variations in a biofuel’s composition will dictate combustion properties such as auto ignition temperature, reaction delay time, and reaction pathways. A handful of novel drop-in replacement biofuels for conventional transportation fuels have recently been down selected from a list of over 10,000 potential candidates as part of the U.S. Department of Energy’s (DOE) Co-Optimization of Fuels and Engines (Co-Optima) initiative. Diisobutylene (DIB) is one such high-performing hydrocarbon which can readily be produced from the dehydration and dimerization of isobutanol, produced from the fermentation of biomass-derived sugars. The two most common isomers realized, from this process, are 2,4,4-trimethyl-1-pentene (α-DIB) and 2,4,4-trimethyl-2-pentene (β-DIB). Due to a difference in olefinic bond location, the α- and β- isomer exhibit dramatically different ignition temperatures at constant pressure and equivalence ratio. This may be attributed to different fragmentation pathways enabled by allylic versus vinylic carbons. For optimal implementation of these biofuel candidates, explicit identification of the intermediates formed during the combustion of each of the isomers is needed. To investigate the combustion pathways of these molecules, tunable vacuum ultraviolet (VUV) light (in the range 8.1–11.0 eV) available at the Lawrence Berkeley National Laboratory’s Advanced Light Source (ALS) has been used in conjunction with a jet stirred reactor (JSR) and time-of-flight mass spectrometry to probe intermediates formed. Relative intensity curves for intermediate mass fragments produced during this process were obtained. Several important unique intermediates were identified at the lowest observable combustion temperature with static pressure of 93,325 Pa and for 1.5 s residence time. As this relatively short residence time is just after ignition, this study is targeted at the fuels’ ignition events. Ignition characteristics for both isomers were found to be strongly dependent on the kinetics of C 4 and C 7 fragment production and decomposition, with the tert-butyl radical as a key intermediate species. However, the ignition of α-DIB exhibited larger concentrations of C 4 compounds over C 7 , while the reverse was true for β-DIB. These identified species will allow for enhanced engineering modeling of fuel blending and engine design.

09 BIOMASS FUELS↗

Separation of alkane and alkene mixtures by metal–organic frameworks

The separation of alkane/alkene gas mixtures represents an important yet challenging process in the petrochemical industry to produce valuable chemical feedstocks with sufficiently high purity. These molecules have similar physical properties, making their separation difficult and capital-intensive. The current separation and purification technology relies largely on heat-driven distillations with a huge unit composed of hundreds of trays. Adsorptive separation using porous solids is capable of accomplishing the purification under ambient conditions, offering potential energy and environmental benefits. In particular, metal–organic frameworks (MOFs) hold enormous promise for this separation process in light of their highly tunable pore shape, pore size, and pore surface functionality. In this review article, we provide a comprehensive account of metal–organic frameworks that have been investigated for the separation of alkanes and alkenes with a focus on C 2 –C 3 hydrocarbons. Here, the material design rationale, separation mechanisms, and structure–property relations are highlighted. Finally, the existing challenges and possible design strategies for desirable materials are also discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A unified reaction network on the formation of five-membered ringed polycyclic aromatic hydrocarbons (PAHs) and their role in ring expansion processes through radical–radical reactions

Exploiting a chemical microreactor in combination with an isomer-selective product identification through fragment-free photoionization utilizing tunable vacuum ultraviolet (VUV) light in tandem with the detection of the ionized molecules by a high resolution reflection time-of-flight mass spectrometer (Re-TOF-MS), the present investigation reveals molecular mass growth processes to four distinct polycyclic aromatic hydrocarbons carrying two six- and one five-membered ring (C 13 H 10 ): 3H-cyclopenta[a]naphthalene, 1H-cyclopenta[b]naphthalene, 1H-cyclopenta[a]naphthalene, and fluorene in the gas phase. Temperatures of 973 and 1023 K simulating conditions in combustion settings along with circumstellar envelopes of carbon-rich stars and planetary nebulae. These reactions highlight the importance of methyl-substituted aromatic reactants (biphenyl, naphthalene) which can be converted to the methylene (–CH 2 ˙) motive by hydrogen abstraction or photolysis. Upon reaction with acetylene, methylene-substituted aromatics carrying a hydrogen atom at the ortho position of the ring can be then converted to cyclopentadiene-annulated aromatics thus providing a versatile pathway to five-membered ring aromatics at elevated temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photonic integration of Er 3+ :Y 2 SiO 5 with thin-film lithium niobate by flip chip bonding

Rare earth ions are known as promising candidates for building quantum light-matter interface. However, tunable photonic cavity access to rare earth ions in their desired host crystal remains challenging. Here, we demonstrate the integration of erbium doped yttrium orthosilicate (Er 3+ :Y 2 SiO 5 ) with thin-film lithium niobate photonic circuit by plasma-activated direct flip chip bonding. Resonant coupling to erbium ions is realized by on-chip electro-optically tuned high Q lithium niobate micro-ring resonators. Fluorescence and absorption of erbium ions at 1536.48 nm are measured in the waveguides, while the collective ion-cavity cooperativity with micro-ring resonators is assessed to be 0.36. This work presents a versatile scheme for future rare earth ion integrated quantum devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ultralow-threshold thin-film lithium niobate optical parametric oscillator

Materials with strong second-order ( χ <#comment/> ( 2 ) ) optical nonlinearity, especially lithium niobate, play a critical role in building optical parametric oscillators (OPOs). However, chip-scale integration of low-loss χ <#comment/> ( 2 ) materials remains challenging and limits the threshold power of on-chip χ <#comment/> ( 2 ) OPO. Here we report an on-chip lithium niobate optical parametric oscillator at the telecom wavelengths using a quasi-phase-matched, high-quality microring resonator, whose threshold power ( ∼ <#comment/> 30 µ <#comment/> W ) is 400 times lower than that in previous χ <#comment/> ( 2 ) integrated photonics platforms. An on-chip power conversion efficiency of 11% is obtained from pump to signal and idler fields at a pump power of 93 µW. The OPO wavelength tuning is achieved by varying the pump frequency and chip temperature. With the lowest power threshold among all on-chip OPOs demonstrated so far, as well as advantages including high conversion efficiency, flexibility in quasi-phase-matching, and device scalability, the thin-film lithium niobate OPO opens new opportunities for chip-based tunable classical and quantum light sources and provides a potential platform for realizing photonic neural networks.

Lu, Juanjuan (ORCID:0000000319389119)↗

Fabrication of Low-Cost Large-Volume Ceramic A 2 HfX 6 (A= Cs or Tl, X = Cl, Br, or I) Scintillators for Gamma Ray Detection (SBIR Phase I Final Technical Report)

Scintillator crystals play an important role in the radiation detection field. Widespread use of scintillators as gamma-ray detectors is largely generated by their extensive availability and tunable properties, such high light output, high stopping power (Z eff ), fast decay time, and good proportionality. Additionally, the cost for manufacturing a scintillation detector like NaI:Tl is usually considerably lower than the cost for manufacturing a semiconductor detector like CdZnTe. Because there is no such thing as an ideal scintillation material, an application requiring certain detection characteristics may incorporate a scintillator tailored to its specific properties. The vast variety of applications and requirements necessitates more research into new scintillation materials and/or better methods of producing existing materials.The goal of this project was to grow low cost and environmentally stable inorganic transparent ceramic scintillators with excellent gamma ray resolution, excellent energy proportionality, excellent detection efficiency due to high density (>5 g/cm 3 ) and very high Z eff (55-80), and good light yields (>40,000 ph/MeV). In Phase I Xtallized Intelligence, Inc. (XI, Inc) developed a novel ceramic fabrication technique to produce low cost and environmentally stable highly efficient inorganic transparent ceramic scintillators of various dimensions. XI, Inc., collaborating with Fisk University (Fisk), investigated the scintillation properties of these new ceramic scintillators and compared them to in their single crystal counterparts. The results of this Phase I project show that successful production of high-quality inorganic halide ceramic scintillators Cs 2 HfCl 6 (CHC) and Tl 2 HfCl 6 (THC). Both ceramic CHC and THC scintillators have achieved good performance close to the performance of their single crystal counterparts. Fabricating these inorganic ceramic scintillators mitigate many issues encountered during conventional bulk crystal growth by melt methods. Additional benefits of the ceramic fabrication technique include high production yield, low production cost, fast production time, and no material waste Inorganic transparent ceramic scintillators produced in this project will enhance cost effectiveness at the instrument level based on low projected cost of the proposed compounds, as much smaller crystal sizes would be required to achieve similar efficiency as current radioisotope identification devices (RIID’s) used in homeland security applications as well as spectrometers in high energy physics applications.

36 MATERIALS SCIENCE↗

Open-path tunable diode laser absorption for eddy correlation flux measurements of atmospheric trace gases

Biogenic emissions from and dry deposition to terrestrial surfaces are important processes determining the trace gas composition of the atmosphere. An instrument has been developed for flux measurements of gases such as CH4, N2O, and O3 based on the eddy correlation technique which combines trace gas fluctuation measurements with simultaneous windfield measurements. The instrument combines a tunable diode laser infrared light source with an open-path multipass absorption cell in order to provide the fast time response and short base pathlength required for the eddy correlation method. Initial field tests using the instrument to measure methane emissions from a local wetland demonstrate the capability for high precision eddy correlation flux measurements.

Anderson, Stuart M.↗

THUNDER Piezoelectric Actuators as a Method of Stretch-Tuning an Optical Fiber Grating

A method of stretching optical fiber holds interest for measuring strain in smart structures where the physical displacement may be used to tune optical fiber lasers. A small, light weight, low power tunable fiber laser is ideal for demodulating strain in optical fiber Bragg gratings attached to smart structures such as the re-usable launch vehicle that is being developed by NASA. A method is presented for stretching optical fibers using the THUNDER piezoelectric actuators invented at NASA Langley Research Center. THUNDER actuators use a piezoelectric layer bonded to a metal backing to enable the actuators to produce displacements larger than the unbonded piezoelectric material. The shift in reflected optical wavelength resulting from stretching the fiber Bragg grating is presented. Means of adapting THUNDER actuators for stretching optical fibers is discussed, including ferrules, ferrule clamp blocks, and plastic hinges made with stereo lithography.

Allison, Sidney G.↗

Optical Parametric Technology for Methane Measurements

Atmospheric methane (CH4) is the second most important anthropogenic greenhouse gas, with approximately 25 times the radiative forcing of carbon dioxide (CO2) per molecule. Yet, lack of understanding of the processes that control CH4 sources and sinks and its potential release from stored carbon reservoirs contributes significant uncertainty to our knowledge of the interaction between carbon cycle and climate change. At Goddard Space Flight Center (GSFC) we have been developing the technology needed to remotely measure CH4 from orbit. Our concept for a CH4 lidar is a nadir viewing instrument that uses the strong laser echoes from the Earth's surface to measure CH4. The instrument uses a tunable, narrow-frequency light source and photon-sensitive detector to make continuous measurements from orbit, in sunlight and darkness, at all latitudes and can be relatively immune to errors introduced by scattering from clouds and aerosols. Our measurement technique uses Integrated Path Differential Absorption (IPDA), which measures the absorption of laser pulses by a trace gas when tuned to a wavelength coincident with an absorption line. We have already demonstrated ground-based and airborne CH4 detection using Optical Parametric Amplifiers (OPA) at 1651 nm using a laser with approximately 10 microJ/pulse at 5kHz with a narrow linewidth. Next, we will upgrade our OPO system to add several more wavelengths in preparation for our September 2015 airborne campaign, and expect that these upgrades will enable CH4 measurements with 1% precision (10-20 ppb).

oscillator↗