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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

Green syntheses of stable and efficient organic dyes for organic hybrid light-emitting diodes

Organic hybrid light-emitting diodes (hybrid-LEDs) employ organic dyes as light converters on top of commercial blue inorganic LEDs, replacing incumbent inorganic phosphor light converters synthesized from rare-earth and/or toxic metallic elements to optimize device environmental sustainability. Here, we present two naturally derived organic dyes for hybrid-LEDs, highlighting stability and efficiency enhancement based on a novel “acceptor–acceptor” molecular design. This “acceptor–acceptor” skeleton comprises theobromine and thiadiazole, two electron-withdrawing groups that lower energy levels and suppress photooxidation. This differentiates these dyes from the widely adopted “donor–acceptor” skeleton, where photooxidation is facilitated by the presence of electron-donating units. Simultaneously, sidechains on organic dyes used to enhance solution processability, crucial for film transparency, introduce an additional photooxidation pathway. With this “acceptor–acceptor” skeleton, the destabilization from sidechains was offset by the stability enhancement from the electronic effects in the backbone. Additionally, when blended within an industrial polymer, poly(styrene-butadiene-styrene) (SBS), their enhanced solubility enables the formation of highly transparent films, crucial for reducing scattering loss in LEDs. Furthermore, resultant dye-SBS films achieved photoluminescence quantum yields (PLQYs) of around 90% under ambient conditions. Taking advantage of their transparency and solution processability, we fabricated a waveguide with this theobromine-dye-SBS composite, which was subsequentially assembled into an edge-lit LED device of no glare and enhanced aesthetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

Efficient and bright white light-emitting diodes based on single-layer heterophase halide perovskites

At present, electric lighting accounts for ~15% of global power consumption and thus the adoption of efficient, low-cost lighting technologies is important. Here, halide perovskites have been shown to be good emitters of pure red, green and blue light, but an efficient source of broadband white electroluminescence suitable for lighting applications is desirable. Here, we report a white light-emitting diode (LED) strategy based on solution-processed heterophase halide perovskites that, unlike GaN white LEDs, feature only one broadband emissive layer and no phosphor. Our LEDs operate with a peak luminance of 12,200 cd m –2 at a bias of 6.6 V and a maximum external quantum efficiency of 6.5% at a current density of 8.3 mA cm –2 . Systematic in situ and ex situ characterizations reveal that the mechanism of efficient electroluminescence is charge injection into the α phase of CsPbI 3 , α to δ charge transfer and α–δ balanced radiative recombination. Future advances in fabrication technology and mechanistic understanding should lead to further improvements in device efficiency and luminance.

36 MATERIALS SCIENCE↗

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↗

Unidirectional luminescence from InGaN/GaN quantum-well metasurfaces

III–nitride light-emitting diodes (LEDs) are the backbone of ubiquitous lighting and display applications. Imparting directional emission is an essential requirement for many LED implementations. Although optical packaging, nanopatterning and surface roughening4 techniques can enhance LED extraction, directing the emitted light requires bulky optical components. Optical metasurfaces provide precise control over transmitted and reflected waveforms, suggesting a new route for directing light emission. However, it is difficult to adapt metasurface concepts for incoherent light emission, due to the lack of a phase-locking incident wave. Here, we demonstrate a metasurface-based design of InGaN/GaN quantum-well structures that generate narrow, unidirectional transmission and emission lobes at arbitrary engineered angles. We further demonstrate 7-fold and 100-fold enhancements of total and air-coupled external quantum efficiencies, respectively. The results present a new strategy for exploiting metasurface functionality in light-emitting devices.

inorganic LEDs↗

Light sources with bias tunable spectrum based on van der Waals interface transistors

Light-emitting electronic devices are ubiquitous in key areas of current technology, such as data communications, solid-state lighting, displays, and optical interconnects. Controlling the spectrum of the emitted light electrically, by simply acting on the device bias conditions, is an important goal with potential technological repercussions. However, identifying a material platform enabling broad electrical tuning of the spectrum of electroluminescent devices remains challenging. Here, we propose light-emitting field-effect transistors based on van der Waals interfaces of atomically thin semiconductors as a promising class of devices to achieve this goal. We demonstrate that large spectral changes in room-temperature electroluminescence can be controlled both at the device assembly stage –by suitably selecting the material forming the interfaces– and on-chip, by changing the bias to modify the device operation point. Even though the precise relation between device bias and kinetics of the radiative transitions remains to be understood, our experiments show that the physical mechanism responsible for light emission is robust, making these devices compatible with simple large areas device production methods.

36 MATERIALS SCIENCE↗

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↗

From lab to lamp: Understanding downconverter degradation in LED packages

Downconverters, primarily inorganic phosphors, are critical components in white solid-state LED-based lighting and liquid crystal display backlights. Research efforts have led to a fundamental understanding of a downconverter's absorption, photoluminescence, and efficiency as a function of composition, structure, and processing conditions. However, considerably less work has focused on the reliability of phosphors once they are incorporated into LED packages. Solving these issues is often the final step before the commercialization of new materials, but the significant resources and time required to evaluate and mitigate materials failure are rarely discussed in the literature. In this Perspective, we discuss the need for conducting downconverter reliability testing and the potential of accelerating, screening, and understanding downconverter failure modes. Our focus highlights the mechanisms of failure and discusses how this influences materials selection and the design of different LED packages. We also stress the potential for accelerated reliability testing protocols and note the potential role first-principles calculations and data-driven models could play in establishing the compositional-processing trends for different aspects of downconverter reliability. In conclusion, we close with possible research directions that could improve downconverter reliability and emphasize the importance of assessing a material's (chemical) stability where multiple manufacturing and processing steps can dictate system performance.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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↗

Cesium Lead Halide Perovskite Nanocrystals Assembled in Metal–Organic Frameworks for Stable Blue Light Emitting Diodes

All inorganic cesium lead trihalide nanocrystals are promising light emitters for bright light emitting diodes (LEDs). Here we demonstrate CsPb(BrCl) 1.5 nanocrystals in metal-organic frameworks (MOF) thin films to achieve bright and stable blue LEDs. The lead metal nodes in the MOF thin film react with Cs-halide salts, resulting in 10~20 nm nanocrystals. This is revealed by X-ray scattering and transmission electron microscopy. Employing the CsPbX 3 - MOF thin films as emission layers, bright deep blue and sky-blue LEDs are demonstrated that emit at 452 nm and 476 nm respectively. The maximum external quantum efficiencies of these devices are 0.72% for deep blue LEDs and 5.6% for sky blue LEDs. More importantly, the device can maintain 50% of its original electroluminescence (T 50 ) for 2.23 hours when driving at 4.2V. Detailed optical spectroscopy and time-of-flight secondary ion mass spectroscopy suggest that the ion migration can be suppressed that maintains the emission brightness and spectra. Our study provides a new route for fabricating stable blue light emitting diodes with all-inorganic perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

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.↗

Microwave-Assisted Preparation of Luminescent Inorganic Materials: A Fast Route to Light Conversion and Storage Phosphors

Luminescent inorganic materials are used in several technological applications such as light-emitting displays, white LEDs for illumination, bioimaging, and photodynamic therapy. Usually, inorganic phosphors (e.g., complex oxides, silicates) need high temperatures and, in some cases, specific atmospheres to be formed or to obtain a homogeneous composition. Low ionic diffusion and high melting points of the precursors lead to long processing times in these solid-state syntheses with a cost in energy consumption when conventional heating methods are applied. Microwave-assisted synthesis relies on selective, volumetric heating attributed to the electromagnetic radiation interaction with the matter. The microwave heating allows for rapid heating rates and small temperature gradients yielding homogeneous, well-formed materials swiftly. Luminescent inorganic materials can benefit significantly from the microwave-assisted synthesis for high homogeneity, diverse morphology, and rapid screening of different compositions. The rapid screening allows for fast material investigation, whereas the benefits of enhanced homogeneity include improvement in the optical properties such as quantum yields and storage capacity.

59 BASIC BIOLOGICAL SCIENCES↗

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↗

Lead-Free Organic–Perovskite Hybrid Quantum Wells for Highly Stable Light-Emitting Diodes

Two-dimensional perovskites that could be regarded as natural organic-inorganic hybrid quantum wells (HQWs) are promising for light-emitting diode (LED) applications. High photoluminescence quantum efficiencies (approaching 80%) and extremely narrow emission bandwidth (less than 20 nm) have been demonstrated in their single crystals; however, a reliable electrically driven LED device has not been realized owing to inefficient charge injection and extremely poor stability. Furthermore, the use of toxic lead raises concerns. Here, we report Sn(II)-based organic-perovskite HQWs employing molecularly tailored organic semiconducting barrier layers for efficient and stable LEDs. Utilizing femtosecond transient absorption spectroscopy, we demonstrate the energy transfer from organic barrier to inorganic perovskite emitter occurs faster than the intramolecular charge transfer in the organic layer. Consequently, this process allows efficient conversion of lower-energy emission associated with the organic layer into higher-energy emission from the perovskite layer. Thus, this greatly broadened the candidate pool for the organic layer. Incorporating a bulky small bandgap organic barrier in the HQW, charge transport is enhanced and ion migration is greatly suppressed. We demonstrate a HQW-LED device with pure red emission, a maximum luminance of 3466 cd m -2 , a peak external quantum efficiency up to 3.33%, and an operational stability of over 150 h, which are significantly better than previously reported lead-free perovskite LEDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

Chiral-induced spin selectivity enables a room-temperature spin light-emitting diode

In traditional optoelectronic approaches, control over spin, charge, and light requires the use of both electrical and magnetic fields. In a spin-polarized light-emitting diode (spin-LED), charges are injected, and circularly polarized light is emitted from spin-polarized carrier pairs. Typically, the injection of carriers occurs with the application of an electric field, whereas spin polarization can be achieved using an applied magnetic field or polarized ferromagnetic contacts. We used chiral-induced spin selectivity (CISS) to produce spin-polarized carriers and demonstrate a spin-LED that operates at room temperature without magnetic fields or ferromagnetic contacts. The CISS layer consists of oriented, self-assembled small chiral molecules within a layered organic-inorganic metal-halide hybrid semiconductor framework. The spin-LED achieves ±2.6% circularly polarized electroluminescence at room temperature.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

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↗