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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 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Nonclassical light from finite-range interactions in a two-dimensional quantum mirror

Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. We investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly nonclassical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditions of electromagnetically induced transparency and thereby provides an efficient mechanism for single-photon switching between high transmission and reflectance of the monolayer, with a tunable dynamical timescale of the emerging photon-photon interactions. Remarkably, it turns out that the resulting high degree of photon correlations remains virtually unaffected by Rydberg-state decoherence, in excess of nonradiative decoherence observed for ground-state excitons in two-dimensional semiconductors. This robustness to imperfections suggests a promising approach to quantum photonics at the level of individual photons.

36 MATERIALS SCIENCE↗
NASA NTRS1995

Stress Tuning of Laser Crystals

The topic of stress tunable laser crystals is addressed in this study with the purpose of determining the piezo-optic coefficients of a new laser material. This data was collected using a quadruple pass birefringence technique because of its high degree of sensitivity relative to the other methods examined including fringe shift analysis using a Mach-Zender interferometer. A green He-Ne laser was passed through a light chopper and Glan-Thompson prism before entering a crystal of Erbium doped Yttrium Aluminum Garnet (Er:YAG) (used in order to validate the experimental technique). The Er:YAG crystal is mounted in a press mechanism and the laser is quadruple passed through test specimen before being returned through the prism and the orthogonally polarized portion of the beam measured with a optical sensor. At a later stage, the Er:YAG crystal was replaced with a new crystal in order to determine the piezo-optic coefficients of this uncharacterized material. The applied load was monitored with the use of a 50 lb. load cell placed in line with the press. Light transmission readings were taken using a lock-in amplifier while load cell measurements were taken with a voltmeter from a 5 volt, 0.5 amp power supply. Despite the fact that an effective crystal press damping system was developed, size limitations precluded the use of the complete system. For this reason, data points were taken only once per full turn so as to minimize the effect of non uniform load application on the collected data. Good correlation was found in the transmission data between the experimentally determined Er:YAG and the previously known peizo-optic constants of non-doped crystal with which it was compared. The variation which was found between the two could be accounted for by the aforementioned presence of Erbium in the experimental sample (for which exact empirical data was not known). The same test procedure was then carried out on a Yttrium Gallium Aluminum garnet (YGAG) for the purpose of establishing values of its unknown piezo-optic constant tensor using experimentally collected transmission data. Significant variation between the piezo-optic constants of YAG and YGAG crystals was found however, the excellent data correlation of separate experimental runs carried out on the YGAG sample demonstrates the validity of these results. The data collected during the stressing of the YGAG was of high quality, however the amount of data collected was somewhat limited by a fracture of YGAG specimen which undoubted altered the crystalline lattice structure and hence precluded any further testing.

Carty, Atherton A.↗
DOE OSTI2016

Encapsulation of Perovskite Nanocrystals into Macroscale Polymer Matrices: Enhanced Stability and Polarization

Lead halide perovskites hold promise for photonic devices, due to their superior optoelectronic properties. However, their use is limited by poor stability and toxicity. We demonstrate enhanced water and light stability of high-surface-area colloidal perovskite nanocrystals by encapsulation of colloidal CsPbBr 3 quantum dots into matched hydrophobic macroscale polymeric matrices. This is achieved by mixing the quantum dots with presynthesized high-molecular-weight polymers. In this work, we monitor the photoluminescence quantum yield of the perovskite-polymer nanocomposite films under water-soaking for the first time, finding no change even after >4 months of continuous immersion in water. Furthermore, photostability is greatly enhanced in the macroscale polymer-encapsulated nanocrystal perovskites, which sustain >10 10 absorption events per quantum dot prior to photodegradation, a significant threshold for potential device use. Control of the quantum dot shape in these thin-film polymer composite enables color tunability via strong quantum-confinement in nanoplates and significant room temperature polarized emission from perovskite nanowires. Not only does the high-molecular-weight polymer protect the perovskites from the environment but also no escaped lead was detected in water that was in contact with the encapsulated perovskites for months. In conclusion, our ligand-passivated perovskite-macroscale polymer composites provide a robust platform for diverse photonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi 2 Se 3 and MoS 2 atomic layers

Vertical stacking is widely viewed as a promising approach for designing advanced functionalities using two-dimensional (2D) materials. Combining crystallographically commensurate materials in these 2D stacks has been shown to result in rich new electronic structure, magnetotransport, and optical properties. In this context, vertical stacks of crystallographically incommensurate 2D materials with well-defined crystallographic order are a counterintuitive concept and, hence, fundamentally intriguing. We show that crystallographically dissimilar and incommensurate atomically thin MoS 2 and Bi 2 Se 3 layers can form rotationally aligned stacks with long-range crystallographic order. Our first-principles theoretical modeling predicts heterocrystal electronic band structures, which are quite distinct from those of the parent crystals, characterized with an indirect bandgap. Experiments reveal striking optical changes when Bi 2 Se 3 is stacked layer by layer on monolayer MoS 2 , including 100% photoluminescence (PL) suppression, tunable transmittance edge (1.1→0.75 eV), suppressed Raman, and wide-band evolution of spectral transmittance. Disrupting the interface using a focused laser results in a marked the reversal of PL, Raman, and transmittance, demonstrating for the first time that in situ manipulation of interfaces can enable “reconfigurable” 2D materials. We demonstrate submicrometer resolution, “laser-drawing” and “bit-writing,” and novel laser-induced broadband light emission in these heterocrystal sheets.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Giant Electrostriction via Nanodomain Engineering in Relaxor Ferroelectric Polymers

Relaxor ferroelectric (RFE) polymers hold great promise for artificial muscles due to their high actuation strain, high loading stress, and fast response. However, the structural origin underlying their large electrostrictive deformation remains elusive. In this study, we investigate poly(vinylidene fluoride-co-trifluoroethylene) [P(VDF-TrFE)]-based RFE terpolymers, incorporating 1,1-chlorofluoroethylene (CFE) or chlorotrifluoroethylene (CTFE) (the terpolymers are denoted as terP-CFE and terP-CTFE, respectively) as termonomers. Although both terpolymers show similar semicrystalline morphology, drastically different electrostrictive properties are observed. Specifically, the terP-CFE annealed at 100 °C achieves a record-high transverse strain of ∼10.6%, whereas 100 °C-annealed terP-CTFE only shows a much lower actuation strain of ∼4.2% at the same poling field of 190 MV/m. To elucidate the origin of this difference, time-resolved wide-angle X-ray diffraction, small-angle X-ray scattering, and Fourier transform infrared experiments are performed during in situ electric poling. An RFE-to-ferroelectric (FE) crystal phase transition is observed for terP-CFE but is absent for terP-CTFE. Beyond the contribution of the crystalline phase, the oriented amorphous fraction and crystalline defects (e.g., taut-tie molecules) also play significant roles in enhancing electrostriction. In conclusion, this mechanistic insight provides a valuable foundation for the rational design of next-generation RFE polymers with tunable properties through defect engineering of their semicrystalline structures.

36 MATERIALS SCIENCE↗
NASA NTRSDate not supplied

A Vacuum-Compatible, Spectrally Tunable, Flat Panel Uniform Source for Testing Large Aperture Earth Observation Systems

Labsphere, Inc. in conjunction with NASA GSFC and Genesis Engineering Solutions Inc., has developed an innovative, vacuum compatible, calibration spectro-radiometric illumination source with a highly uniform large-area rectangular flat panel active area. This device features a uniquely shaped diffuse integration geometry to achieve high uniformity over a large active output area while maintaining a smaller and more robust overall form-factor when compared to previous designs or integrating spheres. A new liquid-cooled hybrid quartz-tungsten (QT) and light emitting diode (LED) source module has been engineered to provide direct-in-vacuum reference illumination over the full dynamic range and spectrum of the VIIRS instrument’s optical bands during pre-launch testing. The first unit has been demonstrated to meet its requirements using ambient technology and a fully-vacuum-compatible second unit is planned to allow testing in thermal vacuum (TVAC) campaigns. This technology is flexible and capable of meeting the needs of many other instruments/missions requiring this type of test/calibration capability.

Jeffrey Holt↗
DOE OSTI2018

Hybrid 0D–2D black phosphorus quantum dots–graphitic carbon nitride nanosheets for efficient hydrogen evolution

As an emerging post-graphene two-dimensional (2D) nanomaterial, black phosphorus (BP) is attracting a great deal of current attention for the direct conversion of solar energy into solar fuels on account of its unique tunable direct-bandgap and high charge-carrier mobility. Herein, for the first time, we immobilize BP quantum dots (BPQDs) onto graphitic carbon nitride (g-C 3 N 4 ) nanosheets to create a 0D-2D inorganic-organic hybrid via a conventional and cost–effective sonication approach. The as-prepared BPQDs/g-C 3 N 4 hybrids display BPQD content-dependent performance in visible-light-driven hydrogen generation. 5 wt% BPQDs/g-C 3 N 4 with cyclability exhibits the greatest hydrogen evolution rate of 271 μmol h-1 g-1 that is 5.6 and 4.2 times greater than that of pristine g-C 3 N 4 and BPQDs, respectively. We demonstrate that the type-II band alignment, the formation of phosphorus–carbon bonds and the efficient interfacial charge separation between well-dispersed BPQDs and g-C 3 N 4 synergetically enhance the photoactivity and photostability. In conclusion, this study opens possibilities to create viable BP-based heterostructures for energy conversion and storage.

36 MATERIALS SCIENCE↗
DOE OSTI2011

An Artificial neural network based $b$ jet identification algorithm at the CDF Experiment

We present the development and validation of a new multivariate $b$ jet identification algorithm ('$b$ tagger') used at the CDF experiment at the Fermilab Tevatron. At collider experiments, $b$ taggers allow one to distinguish particle jets containing $B$ hadrons from other jets. Employing feed-forward neural network architectures, this tagger is unique in its emphasis on using information from individual tracks. This tagger not only contains the usual advantages of a multivariate technique such as maximal use of information in a jet and tunable purity/efficiency operating points, but is also capable of evaluating jets with only a single track. To demonstrate the effectiveness of the tagger, we employ a novel method wherein we calculate the false tag rate and tag efficiency as a function of the placement of a lower threshold on a jet's neural network output value in $Z+1$ jet and $t\bar{t}$ candidate samples, rich in light flavor and $b$ jets, respectively.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Constructing Highly Porous Thermoelectric Monoliths with High-Performance and Improved Portability from Solution-Synthesized Shape-Controlled Nanocrystals

Thermoelectricity offers a viable and reliable solution to convert waste heat into electricity. To enhance the performance and portability of thermoelectric materials, the crystal grain and pore structure should be simultaneously manipulated to achieve high electrical conductivity (σ), low thermal conductivity (κ), high figure of merit (zT), and low relative density. However, they cannot be synchronously realized using nanocrystals with uncontrolled domain size and shape as building blocks. Here, we employ solution-synthesized PbS nanocrystals with large grain size, controllable shape and tunable spatial packing to realize the aforementioned structural tuning. In this work, the as-sintered highly porous and well crystalline monolith exhibits high σ, low κ, high zT (1.06 at 838 K) and low relative density (82%). The phonon transport is studied by density functional theory highlighting the crucial role of phonon–pore scattering in reducing κ to enhance zT. Our strategy may benefit thermoelectrics and shed light on other technical fields such as catalysis, gas sensing, photovoltaics, and so forth.

nanocrystal↗
DOE OSTI2018

Two-dimensional transition metal carbides as supports for tuning the chemistry of catalytic nanoparticles

Supported nanoparticles are broadly employed in industrial catalytic processes, where the active sites can be tuned by metal-support interactions (MSIs). Although it is well accepted that supports can modify the chemistry of metal nanoparticles, systematic utilization of MSIs for achieving desired catalytic performance is still challenging. The developments of supports with appropriate chemical properties and identification of the resulting active sites are the main barriers. Here, we develop two-dimensional transition metal carbides (MXenes) supported platinum as efficient catalysts for light alkane dehydrogenations. Ordered Pt 3 Ti and surface Pt 3 Nb intermetallic compound nanoparticles are formed via reactive metal-support interactions on Pt/Ti 3 C 2 T x and Pt/Nb 2 CT x catalysts, respectively. MXene supports modulate the nature of the active sites, making them highly selective toward C–H activation. Such exploitation of the MSIs makes MXenes promising platforms with versatile chemical reactivity and tunability for facile design of supported intermetallic nanoparticles over a wide range of compositions and structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Tip- and Plasmon-Enhanced Infrared Nanoscopy for Ultrasensitive Molecular Characterizations

Herein, we propose a method for ultrasensitive infrared (IR) vibrational spectroscopy of molecules with nanoscale footprints by combining the tip enhancement of a scattering-type scanning near-field optical microscope (s-SNOM) and the plasmon enhancement of breathing-mode (BM) plasmon resonances of graphene nanodisks (GNDs). To demonstrate this, we develop a quantitative model that is capable of computing accurately the s-SNOM signals of nanoscale samples. With our modeling, we show that the s-SNOM tip can effectively excite gate-tunable BM plasmonic resonances in GNDs with strong field enhancement and sensitive dependence on the size of GND. Moreover, we demonstrate that the intense electric field of tip-excited plasmonic BMs can strongly enhance the IR vibrational modes of molecules. As a result, IR vibrational signatures of individual molecular particles with sizes down to 1–2 nm are readily observable by s-SNOM. Our study sheds light on future ultrasensitive IR biosensing that takes advantage of both the tip and plasmon enhancement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Understanding and Tuning Magnetism in Layered Ising‐Type Antiferromagnet FePSe 3 for Potential 2D Magnet

Abstract Recent developments in 2D magnetic materials have motivated the search for new van der Waals magnetic materials, especially Ising‐type magnets with strong magnetic anisotropy. Fe‐based M P X 3 ( M = transition metal, X = chalcogen) compounds such as FePS 3 and FePSe 3 both exhibit an Ising‐type magnetic order, but FePSe 3 receives much less attention compared to FePS 3 . This work focuses on establishing the strategy to engineer magnetic anisotropy and exchange interactions in this less‐explored compound. Through chalcogen and metal substitutions, the magnetic anisotropy is found to be immune against S substitution for Se whereas tunable only with heavy Mn substitution for Fe. In particular, Mn substitution leads to a continuous rotation of magnetic moments from the out‐of‐plane direction toward the in‐plane. Furthermore, the magnetic ordering temperature displays non‐monotonic doping dependence for both chalcogen and metal substitutions but due to different mechanisms. These findings provide deeper insight into the Ising‐type magnetism in this important van der Waals material, shedding light on the study of other Ising‐type magnetic systems as well as discovering novel 2D magnets for potential applications in spintronics.

2D magnet↗
DOE OSTI2016

Bandgap- and local field-dependent photoactivity of Ag/black phosphorus nanohybrids

Black phosphorus (BP) is the most exciting post-graphene layered nanomaterial that serendipitously bridges the 2D materials gap between semimetallic graphene and large bandgap transition-metal dichalcogenides in terms of high charge-carrier mobility and tunable direct bandgap, yet research into BP-based solar to chemical energy conversion is still in its infancy. Herein, a novel hybrid photocatalyst with Ag nanoparticles supported on BP nanosheets is prepared using a chemical reduction approach. Spin-polarized density functional theory (DFT) calculations show that Ag nanoparticles are stabilized on BP by covalent bonds at the Ag/BP interface and Ag–Ag interactions. In the visible-light photocatalysis of rhodamine B by Ag/BP plasmonic nanohybrids, a significant rise in photoactivity compared with pristine BP nanosheets is observed either by decreasing BP layer thickness or increasing Ag particle size, with the greatest enhancement being up to ~20-fold. By virtue of finite-difference time domain (FDTD) simulations and photocurrent measurements, we give insights into the enhanced photocatalytic performance of Ag/BP nanohybrids, including the effects of BP layer thickness and Ag particle size. In comparison with BP, Ag/BP nanohybrids present intense local field amplification at the perimeter of Ag NPs, which is increased by either decreasing the BP layer thickness from multiple to few layers or increasing the Ag particle size from 20 to 40 nm. Additionally, when the BP layer thickness is decreased from multiple to few layers, the bandgap becomes favorable to generate more strongly oxidative holes in the proximity of the Ag/BP interface to enhance photoactivity. Our findings illustrate a synergy between locally enhanced electric fields and BP bandgap, in which BP layer thickness and Ag particle size can be independently tuned to enhance photoactivity. Lastly, this study may open a new avenue for further exploiting BP-based plasmonic nanostructures in photocatalysis, photodetectors, and photovoltaics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Cellulose-Based Reflective Liquid Crystal Films as Optical Filters and Solar Gain Regulators

Many promising approaches for designing interactions of synthetic materials with light involve solid optical monocrystals and nanofabricated photonic crystal structures with spatially periodic variations of refractive index. Although their high costs limit current technological applications, remarkably, such photonic and optically anisotropic materials have also evolved throughout nature and enable narrow or broad-band spectral reflection of light. Here we use self-assembly of biomaterial cellulose nanocrystals to obtain three-layer films with helicoidal and nematic-like organization of the cellulose nanoparticles, which mimics naturally occurring polarization-insensitive reflectors found in the wings of Plusiotis resplendens beetles. These films were characterized with polarized optical microscopy and circular dichroism spectrometry, as well as scanning and transmission electron microscopies. These films exhibit high reflectivity tunable within the visible and near-infrared regions of the optical spectrum and may find applications ranging from color filters to smart cloth designs and in solar-gain-regulating building technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Structural features of xylan dictate reactivity and functionalization potential for bio-based materials

Plant-based materials have the potential to replace some petroleum-based products, offering compostability and biodegradability as critical advantages. Xylan-rich biomass sources are gaining recognition due to their abundance and underutilization in current industrial applications. Research of potential xylan applications has been complicated by the complex and heterogeneous structure that varies for different xylan feedstocks. Acylation is a broadly used reaction in functionalization of polysaccharides at an industrial scale. However, the efficiency of this reaction varies with the xylan source. To optimize xylan valorization, a systematic understanding of structure–reactivity relationships is essential. This study explores, characterizes, and compares various xylan feedstocks in the acylation process. Xylan feedstocks were analyzed for their chemical composition, degree of polymerization, branching, solubility, and presence of impurities. These features were correlated with xylan glycotypes’ reactivity toward functionalization with succinic anhydride in an optimized DMSO/KOH condition, achieving carboxyl contents of up to 1.46. We used principal component analysis and hierarchical clustering to identify key structural features of xylan that promote its reactivity. Our findings reveal that xylans with higher xylose content and lower degrees of branching exhibit enhanced reactivity, achieving higher carboxyl content and yields. Structural analyses confirmed successful modification, and light scattering analyses showed dramatic changes in the solution properties. Succinylation improves the solubility and film-forming properties of native xylans. This study shows key structure–reactivity relationships in xylan succinylation, establishing that low branching, high xylose content, and reduced lignin impurity enhance chemical functionalization. The results offer a framework for selecting optimal biomass feedstocks and support future efforts in genetic and synthetic biology to design plants with tunable xylan architectures. These findings advance the hemicellulose valorization for applications in coatings and packaging.

Acylation↗
DOE OSTI2015

Novel hetero-bilayered materials for photovoltaics

The recently synthesized GaS and MoSe 2 nanosheets have been used as appropriate substrates for other layered materials, e.g. silicene/GaS heterosheets akin to graphene/BN systems. Here, we have performed a comprehensive first-principles study of the electronic and optical properties of two-dimensional (2D) GaS/MoSe 2 hetero-bilayers based on density functional theory (DFT). Here we found almost all proposed GaS/MoSe2 hetero-bilayers in the current study have an indirect band gap from the Γ point to the K point, except for one with a direct band gap at the K point. Tunable band gaps GaS/MoSe 2 hetero-bilayers can be controlled by strain modulation. State-of-the-art GW-Bethe–Salpeter method, accounting for electron-electron and electron-hole interactions, has been employed to compute accurate absorbance spectra for layered materials. Compared with its composing GaS and MoSe 2 monolayers, GaS/MoSe 2 hetero-bilayers show superior behavior on optical absorbance, indicating a stronger visible-light absorption and applications in solar energy harvesting. We foresee that the novel GaS/MoSe 2 hetero-bilayers would stimulate the fabrication of materials with unprecedented optical and physico-chemical properties that may apply in nanodevices and photovoltaic cells.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Polymer Hole Transport Material Functional Group Tuning for Improved Perovskite Solar Cell Performance

As lead halide perovskites (LHPs) continue to achieve success as a light-harvesting material in perovskite solar cells (PSCs), exploring and understanding other materials in the device stack become increasingly important. Particularly, selection of suitable hole transport materials (HTMs) that demonstrate high performance and stability is imperative in the design of P-I-N PSCs. Presented here are a family of 12 structurally related polymers based on either fluorene or carbazole main chains with select aromatic side groups that introduce tunable properties for use in PSCs. How properties such as the highest occupied molecular orbital energy level, conductivity, glass-transition temperature, and wettability of the HTM affect the PSC performance is explored. Devices that incorporate the polymer HTMs perform well relative to PTAA in benchmark P-I-N PSC architectures while exhibiting similar or superior stability under accelerated aging studies. The relative synthetic simplicity and resultant performance of the HTMs in PSCs coupled with the ability to customize properties with different functional groups demonstrates the potential of this family of HTMs for a variety of LHP materials.

14 SOLAR ENERGY↗
DOE OSTI2018

Generation and characterization of ultrathin free-flowing liquid sheets

The physics and chemistry of liquid solutions play a central role in science, and our understanding of life on Earth. Unfortunately, key tools for interrogating aqueous systems, such as infrared and soft X-ray spectroscopy, cannot readily be applied because of strong absorption in water. Here we use gas-dynamic forces to generate free-flowing, sub-micron, liquid sheets which are two orders of magnitude thinner than anything previously reported. Optical, infrared, and X-ray spectroscopies are used to characterize the sheets, which are found to be tunable in thickness from over 1 μm down to less than 20 nm, which corresponds to fewer than 100 water molecules thick. At this thickness, aqueous sheets can readily transmit photons across the spectrum, leading to potentially transformative applications in infrared, X-ray, electron spectroscopies and beyond. Lastly, the ultrathin sheets are stable for days in vacuum, and we demonstrate their use at free-electron laser and synchrotron light sources.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗