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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Thermodynamic Limit for Excitonic Light-Emitting Diodes

Here, we derive the thermodynamic limit for organic light-emitting diodes (OLEDs), and show that strong exciton binding in these devices requires a higher voltage to achieve the same luminance as a comparable inorganic LED. The OLED overpotential, which does not reduce the power conversion efficiency, is minimized by having a small exciton binding energy, a long exciton lifetime, and a large Langevin coefficient for electron-hole recombination. Based on these results, it seems likely that the best phosphorescent and thermally activated delayed fluorescence OLEDs reported to date approach their thermodynamic limit. The framework developed here is broadly applicable to other excitonic materials, and should therefore help guide the development of low voltage LEDs for display and solid-state lighting applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Vertical full-colour micro-LEDs via 2D materials-based layer transfer

Micro-LEDs (µLEDs) have been explored for augmented and virtual reality display applications that require extremely high pixels per inch and luminance. However, conventional manufacturing processes based on the lateral assembly of red, green and blue (RGB) µLEDs have limitations in enhancing pixel density. Recent demonstrations of vertical µLED displays have attempted to address this issue by stacking freestanding RGB LED membranes and fabricating top-down, but minimization of the lateral dimensions of stacked µLEDs has been difficult. Here we report full-colour, vertically stacked µLEDs that achieve, to our knowledge, the highest array density (5,100 pixels per inch) and the smallest size (4 µm) reported to date. This is enabled by a two-dimensional materials-based layer transfer technique that allows the growth of RGB LEDs of near-submicron thickness on two-dimensional material-coated substrates via remote or van der Waals epitaxy, mechanical release and stacking of LEDs, followed by top-down fabrication. The smallest-ever stack height of around 9 µm is the key enabler for record high µLED array density. We also demonstrate vertical integration of blue µLEDs with silicon membrane transistors for active matrix operation. Furthermore, these results establish routes to creating full-colour µLED displays for augmented and virtual reality, while also offering a generalizable platform for broader classes of three-dimensional integrated devices.

42 ENGINEERING↗
DOE OSTI2023

Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day

Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Interlaboratory Study: Testing Reproducibility of Solid Biofuels Component Identification Using Reflected Light Microscopy

Considering global market trends and concerns about climate change and sustainability, increased biomass use for energy is expected to continue. As more diverse materials are being utilized to manufacture solid biomass fuels, it is critical to implement quality assessment methods to analyze these fuels thoroughly. One such method is reflected light microscopy (RLM), which has the potential to complement and enhance current standard testing, leading to improving fuel quality assessment and, ultimately, preventing avoidable air pollution. An interlaboratory study (ILS) was conducted to test the reproducibility of biomass fuels component identification using a reflected light microscopy technique. The exercise was conducted on thirty photomicrographs showing biomass and various undesired components (like plastics or mineral matter), which were purposely added (by the ILS organizers) to contaminate wood pellets and charcoal-based grilling fuels. Forty-six participants had various levels of difficulty identifying the marked components, and as a result, the percentage of correct answers ranged from 52.2 to 94.4%. Among the most difficult components to distinguish were petroleum products and inorganic matter. Various reasons led to the misidentification, including insufficient morphological descriptions of the components provided to participants, ambiguities of the nomenclature, limitations of the analytical and exercise method, and insufficient experience of the participants. Overall, the results indicate that RLM has the potential to enhance the quality assessment of biomass fuels. However, they also demonstrate that the petrographic classification used in this exercise requires further refinement before it can be standardized. While a new simplified classification of solid biomass fuels components was created as an outcome of this study, future research is necessary to refine the nomenclature, develop a microscopic morphological description of the components, and verify the accuracy of component identification with a follow-up ILS.

biomass↗
NASA NTRS1990

Model of carbon fixation in microbial mats from 3,500 Myr ago to the present

Using modern microbial mats as analogs for ancient stromatolites, it is shown that the rate of carbon fixation is higher at the greater levels of atmospheric CO2 that were probably present in the past. It is suggested that carbon fixation in microbial mats was not carbon-limited during the early Precambrian, but became carbon-limited as the supply of inorganic carbon decreased. Carbon limitation led to a lower rate of carbon fixation, especially towards the end of the Precambrian.

Rothschild, Lynn J.↗
NASA NTRS2016

Two-Step Resonance-Enhanced Desorption Laser Mass Spectrometry for In Situ Analysis of Organic-Rich Environments

A wide diversity of planetary surfaces in the solar system represent high priority targets for in situ compositional and contextual analysis as part of future missions. The planned mission portfolio will inform our knowledge of the chemistry at play on Mars, icy moons, comets, and primitive asteroids, which can lead to advances in our understanding of the interplay between inorganic and organic building blocks that led to the evolution of habitable environments on Earth and beyond. In many of these environments, the presence of water or aqueously altered mineralogy is an important indicator of habitable environments that are present or may have been present in the past. As a result, the search for complex organic chemistry that may imply the presence of a feedstock, if not an inventory of biosignatures, is naturally aligned with targeted analyses of water-rich surface materials. Here we describe the two-step laser mass spectrometry (L2MS) analytical technique that has seen broad application in the study of organics in meteoritic samples, now demonstrated to be compatible with an in situ investigation with technique improvements to target high priority planetary environments as part of a future scientific payload. An ultraviolet (UV) pulsed laser is used in previous and current embodiments of laser desorption/ionization mass spectrometry (LDMS) to produce ionized species traceable to the mineral and organic composition of a planetary surface sample. L2MS, an advanced technique in laser mass spectrometry, is selective to the aromatic organic fraction of a complex sample, which can provide additional sensitivity and confidence in the detection of specific compound structures. Use of a compact two-step laser mass spectrometer prototype has been previously reported to provide specificity to key aromatic species, such as PAHs, nucleobases, and certain amino acids. Recent improvements in this technique have focused on the interaction between the mineral matrix and the organic analyte. The majority of planetary targets of astrobiological interest are characterized by the presence of water or hydrated mineral phases. Water signatures can indicate a history of available liquid water that may have played an important role in the chemical environment of these planetary surfaces and subsurfaces. The studies we report here investigate the influence of water content on the detectability of organics by L2MS in planetary analog samples.

primitive asteroids↗
DOE OSTI2024

Integrating Tide‐Driven Wetland Soil Redox and Biogeochemical Interactions Into a Land Surface Model

Abstract Redox processes, aqueous and solid‐phase chemistry, and pH dynamics are key drivers of subsurface biogeochemical cycling and methanogenesis in terrestrial and wetland ecosystems but are typically not included in terrestrial carbon cycle models. These omissions may introduce errors when simulating systems where redox interactions and pH fluctuations are important, such as wetlands where saturation of soils can produce anoxic conditions and coastal systems where sulfate inputs from seawater can influence biogeochemistry. Integrating cycling of redox‐sensitive elements could therefore allow models to better represent key elements of carbon cycling and greenhouse gas production. We describe a model framework that couples the Energy Exascale Earth System Model (E3SM) Land Model (ELM) with PFLOTRAN biogeochemistry, allowing geochemical processes and redox interactions to be integrated with land surface model simulations. We implemented a reaction network including aerobic decomposition, fermentation, sulfate reduction, sulfide oxidation, methanogenesis, and methanotrophy as well as pH dynamics along with iron oxide and iron sulfide mineral precipitation and dissolution. We simulated biogeochemical cycling in tidal wetlands subject to either saltwater or freshwater inputs driven by tidal hydrological dynamics. In simulations with saltwater tidal inputs, sulfate reduction led to accumulation of sulfide, higher dissolved inorganic carbon concentrations, lower dissolved organic carbon concentrations, and lower methane emissions than simulations with freshwater tidal inputs. Model simulations compared well with measured porewater concentrations and surface gas emissions from coastal wetlands in the Northeastern United States. These results demonstrate how simulating geochemical reaction networks can improve land surface model simulations of subsurface biogeochemistry and carbon cycling.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Unraveling the Luminescence Quenching Mechanism in Strong and Weak Quantum-Confined CsPbBr 3 Triggered by Triarylamine-Based Hole Transport Layers

Luminescence quenching by hole transport layers (HTLs) is one of the major issues in developing efficient perovskite light-emitting diodes (PeLEDs), particularly prominent in blue-emitting devices. While a variety of material systems have been used as interfacial layers, the origin of such quenching and the type of interactions between perovskites and HTLs are still ambiguous. Here, we present a systematic investigation of the luminescence quenching of CsPbBr 3 by a commonly employed hole transport polymer, Poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB) in LEDs. Strong and weakly quantum-confined CsPbBr 3 (nanoplatelets (NPLs)/nanocrystals (NCs)) are rationally selected to study the quenching mechanism by considering the differences in their morphology, energy level alignments, and quantum confinement. The steady-state and time-resolved Stern-Volmer plots unravel the dominance of dynamic and static quenching at lower and higher concentrations of TFB, respectively, with maximum quenching efficiency of 98%. The quenching rate in NCs is faster than in NPLs owing to their longer PL lifetimes and weak quantum confinement. The ultrafast transient absorption results support these dynamics and rule out the involvement of Forster or Dexter energy transfer. Finally, the 1D 1 H and 2D NOESY NMR study confirms the exchange of native ligands at the NCs surface with TFB, leading to dark CsPbBr 3 -TFB ensemble formation accountable for luminescence quenching. This highlights the critical role of the triarylamine functional group on TFB (also the backbone of many HTLs) in the quenching process. These results shed light on the underlying reasons for the luminescence quenching in PeLEDs and will help to choose the interfacial layers rationally for developing efficient LEDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Process for Making Single-Domain Magnetite Crystals

A process for making chemically pure, single-domain magnetite crystals substantially free of structural defects has been invented as a byproduct of research into the origin of globules in a meteorite found in Antarctica and believed to have originated on Mars. The globules in the meteorite comprise layers of mixed (Mg, Fe, and Ca) carbonates, magnetite, and iron sulfides. Since the discovery of the meteorite was announced in August 1996, scientists have debated whether the globules are of biological origin or were formed from inorganic materials by processes that could have taken place on Mars. While the research that led to the present invention has not provided a definitive conclusion concerning the origin of the globules, it has shown that globules of a different but related chemically layered structure can be grown from inorganic ingredients in a multistep precipitation process. As described in more detail below, the present invention comprises the multistep precipitation process plus a subsequent heat treatment. The multistep precipitation process was demonstrated in a laboratory experiment on the growth of submicron ankerite crystals, overgrown by submicron siderite and pyrite crystals, overgrown by submicron magnesite crystals, overgrown by submicron siderite and pyrite. In each step, chloride salts of appropriate cations (Ca, Fe, and Mg) were dissolved in deoxygenated, CO2- saturated water. NaHCO3 was added as a pH buffer while CO2 was passed continuously through the solution. A 15-mL aliquot of the resulting solution was transferred into each of several 20 mL, poly(tetrafluoroethylene)-lined hydrothermal pressure vessels. The vessels were closed in a CO2 atmosphere, then transferred into an oven at a temperature of 150 C. After a predetermined time, the hydrothermal vessels were removed from the oven and quenched in a freezer. Supernatant solutions were decanted, and carbonate precipitates were washed free of soluble salts by repeated decantations with deionized water.

Golden, D. C.↗
DOE OSTI2024

A database of thermally activated delayed fluorescent molecules auto-generated from scientific literature with ChemDataExtractor

A database of thermally activated delayed fluorescent (TADF) molecules was automatically generated from the scientific literature. It consists of 25,482 data records with an overall precision of 82%. Among these, 5,349 records have chemical names in the form of SMILES strings which are represented with 91% accuracy; these are grouped in a subsidiary database. Each data record contains one of the following four properties: maximum emission wavelength (λ EM ), photoluminescence quantum yield (PLQY), singlet-triplet energy splitting (ΔE ST ), and delayed lifetime (τ D ). The databases were created through text mining using ChemDataExtractor, a chemistry-aware natural-language-processing toolkit, which has been adapted for TADF research. The text-mined corpus consisted of 2,733 papers from the Royal Society of Chemistry and Elsevier. To the best of our knowledge, these databases are the first databases that have been auto-generated for TADF molecules from existing publications. The databases have been publicly released for experimental and computational applications in the TADF research field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Electroluminescence and Plasmon-Assisted Directional Photoluminescence from 2D HgTe Nanoplatelets

In the visible range, 2D nanoplatelets (NPLs) have brought significant benefits compared to their 0D counterpart with an inherently anisotropic emission, a narrower photoluminescence (PL) signal, and new degrees of freedom to design heterostructures. Compared to the properties of cadmium chalcogenide NPLs in the visible, similar research is still mostly lacking in the infrared, in spite of existing synthetic paths to obtain narrow band gap semiconductors in 2D colloidal form. Here, in this paper, we focus on 2D HgTe NPLs and show how their PL can be stabilized through the proper choice of surface chemistry. We then demonstrate two important steps toward bright infrared light emitting diodes (LEDs) which are (i) the coupling to a plasmonic grating to control the magnitude and spatial direction of the PL signal and (ii) the observation of electroluminescence at 1300 nm, which is near telecom wavelength.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1973

Inorganic separator technology program

Testing and failure analyses of silver zinc cells with largely inorganic separators were performed. The results showed that the wet stand and cycle life objective of the silver-zinc cell development program were essentially accomplished and led to recommendations for cell composition, design, and operation that should yield further improvement in wet and cycle life. A series of advanced inorganic materials was successfully developed and formulated into rigid and semiflexible separator samples. Suitable screening tests for evaluation of largely inorganic separators were selected and modified for application to the separator materials. The results showed that many of these formulations are potentially superior to previously used materials and permitted selection of three promising materials for further evaluation in silver-zinc cells.

Smatko, J. S.↗
DOE OSTI2024

Long-Term Stability in Perovskite Solar Cells Through Atomic Layer Deposition of Tin Oxide

Robust contact schemes that boost stability and simplify the production process are needed for perovskite solar cells (PSCs). We codeposited perovskite and hole-selective contact while protecting the perovskite to enable deposition of SnOx/Ag without the use of a fullerene. The SnOx, prepared through atomic layer deposition, serves as a durable inorganic electron transport layer. Tailoring the oxygen vacancy defects in the SnOx layer led to power conversion efficiencies (PCEs) of >25%. Our devices exhibit superior stability over conventional p-i-n PSCs, successfully meeting several benchmark stability tests. They retained >95% PCE after 2000 hours of continuous operation at their maximum power point under simulated AM1.5 illumination at 65degrees C. Additionally, they boast a certified T97 lifetime exceeding 1000 hours.

c60↗
DOE OSTI2025

How do substituted phenyl-based cations affect the structure-property-stability relationship of low-dimensional perovskites?

Incorporating organic bulky cations in the precursor or post-treatment to achieve two-dimensional/three-dimensional (2D/3D) heterojunction is an effective strategy for enhancing the stability of perovskite materials. However, the issue of insufficient charge transport in 2D perovskites limits their development, and the fundamental mechanism of out-of-plane carrier transport remains unclear. This study designed and synthesized seven organic phenyl-core cations, differentiated at the 1- and 1,4-positions, and identified the impacts on the corresponding properties of the 2D crystalline perovskite. Shorter cations facilitated a more compact arrangement of adjacent inorganic layers, aligning to favor charge transport along the vertical direction. In addition, introducing high electronegativity led to increased intermolecular interactions, resulting in enhanced structural stability and improved phenyl ring π-orbital overlap and interlayer electron coupling, yielding efficient charge transport. Resilience to thermal stressing of the perovskite was strongly correlated with the carbon chain length of the spacer cations. Here, the increase in cation length and the reduction in the rigidity of the amino-terminal both aided in the dispersion of thermal stress in the inorganic framework. Additional hydrogen bonding also contributed to mitigating structural disorder.

14 SOLAR ENERGY↗
NASA NTRS2012

Applications of MODIS Fluorescent Line Height Measurements to Monitor Water Quality Trends and Algal Bloom Activity

Recent advances in satellite and airborne remote sensing, such as improvements in sensor and algorithm calibrations, processing techniques and atmospheric correction procedures have provided for increased coverage of remote-sensing, ocean-color products for coastal regions. In particular, for the Moderate Resolution Imaging Spectrometer (MODIS) sensor calibration updates, improved aerosol retrievals and new aerosol models has led to improved atmospheric correction algorithms for turbid waters and have improved the retrieval of ocean color in coastal waters. This has opened the way for studying ocean phenomena and processes at finer spatial scales, such as the interactions at the land-sea interface, trends in coastal water quality and algal blooms. Human population growth and changes in coastal management practices have brought about significant changes in the concentrations of organic and inorganic, particulate and dissolved substances entering the coastal ocean. There is increasing concern that these inputs have led to declines in water quality and have increase local concentrations of phytoplankton, which cause harmful algal blooms. In two case studies we present MODIS observations of fluorescence line height (FLH) to 1) assess trends in water quality for Tampa Bay, Florida and 2) illustrate seasonal and annual variability of algal bloom activity in Monterey Bay, California as well as document estuarine/riverine plume induced red tide events. In a comprehensive analysis of long term (2003-2011) in situ monitoring data and satellite imagery from Tampa Bay we assess the validity of the MODIS FLH product against chlorophyll-a and a suite of water quality parameters taken in a variety of conditions throughout a large optically complex estuarine system. A systematic analysis of sampling sites throughout the bay is undertaken to understand how the relationship between FLH and in situ chlorophyll-a responds to varying conditions and to develop a near decadal trend in water quality changes. In situ monitoring locations that correlated well with satellite imagery were in depths greater than seven meters and were located over five kilometers from shore. Water quality parameter of total nitrogen, phosphorous, turbidity and biological oxygen demand had high correlations with these sites, as well. Satellite FLH estimates show improving water quality from 2003-2007 with a slight decline up through 2011. Dinoflagellate blooms in Monterey Bay, California (USA) have recently increased in frequency and intensity. Nine years of MODIS FLH observations are used to describe the annual and seasonal variability of bloom activity within the Bay. Three classes of MODIS algorithms were correlated against in situ chlorophyll measurements. The FLH algorithm provided the most robust estimate of bloom activity. Elevated concentrations of phytoplankton were evident during the months of August-November, a period during which increased occurrences of dinoflagellate blooms have been observed in situ. Seasonal patterns of FLH show the on- and offshore movement of areas of high phytoplankton biomass between oceanographic seasons. Higher concentrations of phytoplankton are also evident in the vicinity of the land-based nutrient sources and outflows, and the cyclonic bay-wide circulation can transport these nutrients to the northern Bay bloom incubation region. Both of these case studies illustrate the utility MODIS FLH observations in supporting management decisions in coastal and estuarine waters.

Fischer, Andrew↗
DOE OSTI2024

Photocatalytic Hydrogen Evolution Using Mesoporous Honeycomb Iron Titanate

Mesoporous honeycomb iron titanate using a sol-gel, evaporation-induced self-assembly method is synthesized. A triblock copolymer, F127, serves as a structure-directing agents, with iron chloride and titanium (IV) isopropoxide as inorganic precursors. The strong intermolecular force of attraction among urea, metal precursors, and polymer led to the formation of the mesoporous honeycomb structure. The study of physicochemical properties using different techniques reveals the formation of microstructures with a remarkable degree of porosity. The amorphous iron titanate outperforms the photochemical generation of H 2 due to its disorderly structural arrangement and incomplete crystal formation. The randomness on the structure provides more area for catalytic reaction by providing more contact with the reactant and superior light absorption capability. The high amount of hydrogen gas, 40.66 mmolg -1 h -1 , is observed in the investigation over 3 h of activity for the iron titanate honeycomb sample. This yield is a more significant amount compared to the obtained for the commercially available TiO 2 (23.78 mmolg -1 h -1 ). The iron titanate materials synthesized with low-cost materials and methods are very effective and have the potential for hydrogen generation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Two-dimensional-lattice-confined single-molecule-like aggregates

Intermolecular distance largely determines the optoelectronic properties of organic matter. Conventional organic luminescent molecules are commonly used either as aggregates or as single molecules that are diluted in a foreigner matrix. They have garnered great research interest in recent decades for a variety of applications, including light-emitting diodes, lasers and quantum technologies, among others. However, there is still a knowledge gap on how these molecules behave between the aggregation and dilution states. Here we report an unprecedented phase of molecular aggregate that forms in a two-dimensional hybrid perovskite superlattice with a near-equilibrium distance, which we refer to as a single-molecule-like aggregate (SMA). By implementing two-dimensional superlattices, the organic emitters are held in proximity, but, surprisingly, remain electronically isolated, thereby resulting in a near-unity photoluminescence quantum yield, akin to that of single molecules. Moreover, the emitters within the perovskite superlattices demonstrate strong alignment and dense packing resembling aggregates, allowing for the observation of robust directional emission, substantially enhanced radiative recombination and efficient lasing. Molecular dynamics simulations together with single-crystal structure analysis emphasize the critical role of the internal rotational and vibrational degrees of freedom of the molecules in the two-dimensional lattice for creating the exclusive SMA phase. Furthermore, this two-dimensional superlattice unifies the paradoxical properties of single molecules and aggregates, thus offering exciting possibilities for advanced spectroscopic and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗