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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Nonlinear Dispersion Relation and Out‐of‐Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long‐lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, second and third harmonic generation in MoSSe and WSSe Janus monolayers is studied. Polarization‐resolved spectroscopy is used to map the full second‐order susceptibility tensor of MoSSe, including its out‐of‐plane components. In addition, the effective third‐order susceptibility and the second‐order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe are measured at room and cryogenic temperatures. This work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next‐generation on‐chip multifaceted photonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ionic transport in electrostatic Janus Membranes. An explicit solvent molecular dynamic simulation.

Janus –or two-sided, charged membranes offer promise as ionic current rectifiers. In such systems, pores consisting of two regions of opposite charge can be used to generate a current from a gradient in salinity. The efficiency of nanoscale Janus pores increases dramatically as their diameter becomes smaller. However, little is known about the underlying transport processes, particularly under experimentally accessible conditions. In this work, we examine the molecular basis for rectification in Janus nanopores using an applied electric field. Molecular simulations with explicit water and ions are used to examine the structure and dynamics of all molecular species in aqueous electrolyte solutions. For several macroscopic observables, the results of such simulations are consistent with experimental observations on asymmetric membranes. Our analysis reveals a number of previously unknown features, including a pronounced local re-orientation of water molecules in the pores, and a segregation of ionic species that has not been anticipated by previously reported continuum analyses of Janus pores. Using these insights, a model is proposed for ionic current rectification in which electric leakage at pore entrance controls net transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Intrinsic ferromagnetism and restrictive thermodynamic stability in MA$_{2}$N$_{4}$ and Janus VSiGeN$_{4}$ monolayers

The seminal experimental discovery of the remarkably stable MoSi 2 N 4 monolayer has led to a handful of predicted magnetic two-dimensional (2D) materials in the MA 2 Z 4 family (M = transition metals, A = Si, Ge, and Z = N, P, As). These magnetic monolayers were predicted to be dynamically stable, but none of them has been synthesized to date. In this Research Letter, from first-principles thermodynamic stability analysis, we demonstrate that only the nitrides are thermodynamically stable and this occurs under N-rich conditions. Based on this finding, we propose two ferromagnetic, semiconducting Janus monolayers in the family: VSiGeN 4 and VSiSnN 4 . They are both dynamically and thermally stable, but only the former is thermodynamically stable. Intriguingly, Janus VSiGeN 4 and VSiSnN 4 monolayers show weak in-plane anisotropy compared with the VSi 2 N 4 monolayer. Furthermore, these two emerging Janus magnetic semiconductors offer opportunities for studying 2D magnetism and spin control for spintronics applications.

2-dimensional systems↗
NASA NTRS1993

Linear structures on the small inner satellites of Saturn

Shape modelling methods developed for non-spherical worlds were applied to four satellites of Saturn: Prometheus, Pandora, Janus, and Epimetheus. This results in the first detailed shaded relief maps of their surfaces. Ridges and valleys are described with their implications for satellite history and asteroid 951 Gaspra. They probably result from fracturing during break-up of parent bodies and/or later large impacts. Prometheus and perhaps Gaspra may be coated with debris from parent body fragmentation as well as more recent regolith. These four satellites are covered by relatively few useful images, so the shapes are imperfectly known and positions of features on maps may be wrong by up to a few tens of degrees in some areas (worst where a feature is seen only near a limb). Nevertheless, these shape models are more useful than the previous triaxial ellipsoid models.

Stooke, Philip J.↗
DOE OSTI2023

Real-Time Diagnostics of 2D Crystal Transformations by Pulsed Laser Deposition: Controlled Synthesis of Janus WSSe Monolayers and Alloys

Energetic processing methods such as hyperthermal implantation hold special promise to achieve the precision synthesis of metastable two-dimensional (2D) materials such as Janus monolayers; however, they require precise control. Here, we report a feedback approach to reveal and control the transformation pathways in materials synthesis by pulsed laser deposition (PLD) and apply it to investigate the transformation kinetics of monolayer WS 2 crystals into Janus WSSe and WSe 2 by implantation of Se clusters with different maximum kinetic energies (<42 eV/Se-atom) generated by laser ablation of a Se target. Real-time Raman spectroscopy and photoluminescence are used to assess the structure, composition, and optoelectronic quality of the monolayer crystal as it is implanted with well-controlled fluxes of selenium for different kinetic energies that are regulated with in situ ICCD imaging, ion probe, and spectroscopy diagnostics. First-principles calculations, XPS, and atomic-resolution HAADF STEM imaging are used to understand the intermediate alloy compositions and their vibrational modes to identify transformation pathways. The real-time kinetics measurements reveal highly selective top-layer conversion as WS 2 transforms through WS 2(1–x) Se 2x alloys to WSe 2 and provide the means to adjust processing conditions to achieve fractional and complete Janus WSSe monolayers as metastable transition states. The general approach demonstrates a real-time feedback method to achieve Janus layers or other metastable alloys of the desired composition, and a general means to adjust the structure and quality of materials grown by PLD, addressing priority research directions for precision synthesis with real-time adaptive control.

2D materials↗
DOE OSTI2021

Designing artificial two-dimensional landscapes via atomic-layer substitution

Significance Manipulating materials with atomic-scale precision is essential for the development of a next-generation material design toolbox. Tremendous efforts have been made to advance the compositional, structural, and spatial accuracy of material deposition and patterning. Here, we presented a new reaction pathway to implement the conversions of two-dimensional materials within the atomic-layer thickness at room temperature for electrical dipole manipulation. Not only could various Janus monolayer transition metal dichalcogenides with vertical dipole be realized, but also some heterostructures, including the dipole-nondipole heterostructures (MoS 2 -MoSSe) and multiheterostructures (MoS 2 -MoSSe-MoSeS-MoSe 2 ) within the same monolayer host structure are developed, in which the dipoles can be selectively patterned to be zero (MoS 2 , MoSe 2 ), positive (MoSSe), and negative (MoSeS).

Guo, Yunfan↗
DOE OSTI2023

Microdynamics of active particles in defect-rich colloidal crystals

Hypothesis. Because they are self-propulsive, active colloidal particles can interact with their environment in ways that differ from passive, Brownian particles. Here, we explore how interactions in different microstructural regions may contribute to colloidal crystal annealing. Experiments. We investigate active particles propagating in a quasi-2D colloidal crystal monolayer produced by alternating current electric fields (active-to-passive particle ratio ~ 1:720). The active particle is a platinum Janus sphere propelled by asymmetric decomposition of hydrogen peroxide. Crystals are characterized for changes in void properties. The mean-squared-displacement of Janus particles are measured to determine how active microdynamics depend on the local microstructure, which is comprised of void regions, void-adjacent regions (defined as within three particle diameters of a void), and interstitial regions. Findings. At active particle energy E A = 2.55 k B T, the average void size increases as much as three times and the average void anisotropy increases about 40% relative to the passive case. Further, the average microdynamical enhancement, <δ(t)>, of Janus particles in the crystal relative to an equivalent passive Janus particle is reduced compared to that of a free, active particle (<δ(t) > is 1.88 ± 0.04 and 2.66 ± 0.08, respectively). The concentration of active particles is enriched in void and void-adjacent regions. Active particles exhibit the greatest change in dynamics relative to the passive control in void-adjacent regions (<δ(t)> = 2.58 ± 0.06). The results support the conjecture that active particle microdynamical enhancement in crystal lattices is affected by local defect structure.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Janus Nanocages of Platinum-Group Metals and Their Use as Effective Dual-Electrocatalysts

Janus nanocages with distinctive platinum-group metals on the outer and inner surfaces can naturally catalyze at least two different reactions. In this work, we report a general method based on successive deposition and then selective etching for the facile synthesis of such nanocages. Herein, we have fabricated 11 different types of Janus nanocages characterized by a uniform size and well-defined {100} facets, together with porous, ultrathin, asymmetric walls up to 1.6 nm thick. When tested as dual-electrocatalysts toward oxygen reduction and evolution reactions, the Janus nanocages based on Pt and Ir exhibited superior activities depending on the thickness and relative position of the metal layer. Density functional theory studies suggest that the alloy composition and surface structure of the nanocages both play important roles in enhancing the electrocatalytic activities by modulating the stability of key reaction intermediates.

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

Unique Orientation of the Solid–Solid Interface at the Janus Particle Boundary Induced by Ionic Liquids

This study reveals the unique role on Janus particles of the solid–solid interface at the boundary in determining particle interactions and assembly. In an aqueous ionic liquid (IL) solution, Janus spheres adopt intriguing orientations with their boundaries pinned on the glass substrate. In addition, it was further discovered that the orientation was affected by the particle amphiphilicity as well as the chemical structure and concentration of the IL. Further characterization suggests that the adsorption on the hydrophilic side is due to both an electrostatic interaction and hydrogen bonding, while adsorption on the hydrophobic side is due to hydrophobic attraction. Through the concerted interplay of all these interactions, the amphiphilic boundary may attract an excessive amount of IL cations, which guide the unique orientations of the Janus spheres. The results highlight the importance of the Janus boundary that has not been recognized previously. Adsorption at the solid–solid interfaces may inspire new applications in areas such as separation and catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

The determination of the mass and mean density of Enceladus from its observed shape

Application of limb-fitting methods to the 11 best Voyager 2 images of Enceladus has shown that the shape of this satellite is closely represented by a triaxial ellipsoid. The observed ratio of the differences of the principal axes F = (b - c)/(a - c) is 0.23 (sup +0.04 sub - 0.01), consisting with the value F = 0.23 expected for a synchronously rotating satellite in hydrostatic equilibrium. We also deduce from the Voyager observations, after allowing for limb topography, that the mean radius of the satellite is 249.4 +/- 0.2 km. For satellites of known mass, measurement of the size and shape leads to a determination of the satellite's mean density and moment of inertial. We have used this method to determine the moments of inertia of Mimas (1988) and Tethys (1991). Enceladus appears to be hydrostatically relaxed, making it an ideal candidate for this type of analysis. However, none of the Pioneer or Voyager spacecraft had a close encounter with this satellite and thus its mass is effectively unknown. Enceladus is trapped in a 2:1 orbit-orbit resonance with Dione, but the amplitudes of libration are too small to allow a useful mass determination. Using the observed shape alone, without any other assumptions other than that the satellite is in hydrostatic equilibrium at its present orbital radius, we place an upper bound on the mean density of 1.12 +/- 0.05 g/cu cm. Thus, the mean density of Enceladus is probably little more than that of water-ice and we conclude that this satellite is markedly deficient in rock. If the mass of a satellite is unknown, but the satellite is differentiated and has a deep mantle of known composition, then we show that measurement of the shape alone can lead to a determination of the satellite's mass, mean density, and moment of inertia. Application of this method to Enceladus, assuming that the satellite has a deep mantle of water-ice of density 0.93 g/cu cm, gives the result that the mean density of the satellite is 1.00 +/- 0.03 g/cu cm. This result fills the one remaining gap in our knowledge of the structure of the Saturnian satellite system. We now know the mean densities of all the primary Saturnian satellites in the sequence from the coorbital satellites, Janus and Epimetheus, through to the outer satellite Iapetus (the densities of the small, secondary satellites in Trojan-type orbits are still unknown). The Saturnian system possesses two striking features. (1) Because of significant porosity, the mean material densities of the satellites Janus, Epimetheus, and Mimas could be substantially greater than the apparent mean densities of these satellies. (2) The densities of the satellites are not correlated with their distances from the planet; in particular, the satellites Enceladus and Tethys have lower mean densities than their interior and exterior neighbors, Mimas and Dione. This may be the result of gross postformation redistribution of rock and ice, possibly due to satellite disruptions are suggested by Smith et al. (1982).

Dermott, Stanley F.↗
DOE OSTI2023

Luminescent Bimetallic Two-Coordinate Gold(I) Complexes Utilizing Janus Carbenes

A series of bimetallic carbene-metal-amide (cMa) complexes have been prepared with bridging biscarbene ligands to serve as a model for the design of luminescent materials with large oscillator strengths and small energy differences between the singlet and triplet states (ΔE ST ). The complexes have a general structure (R 2 N)Au(:carbene—carbene:)Au(NR 2 ). The bimetallic complexes show solvation-dependent absorption and emission that is analyzed in detail. It is found that the molar absorptivity of the bimetallic complexes is correlated with the energy barrier to rotation of the metal–ligand bond. The bimetallic cMa complexes also exhibit short emission lifetimes (τ = 200–300 ns) with high photoluminescence efficiencies (Φ PL > 95%). The radiative rates of bimetallic cMa complexes are 3–4 times faster than that of the corresponding monometallic complexes. Analysis of temperature-dependent luminescence data indicates that the lifetime for the singlet state (τS 1 ) of bimetallic cMa complexes is near 12 ns with a ΔE ST of 40–50 meV. Here the presented compounds provide a general design for cMa complexes to achieve small values for ΔE ST while retaining high radiative rates. Solution-processed organic light-emitting devices (OLEDs) made using two of the complexes as luminescent dopants show high efficiency and low roll-off at high luminance.

14 SOLAR ENERGY↗
DOE OSTI2023

Atomic-scale in situ observation of electron beam and heat induced crystallization of Ge nanoparticles and transformation of Ag@Ge core-shell nanocrystals

Crystallization of amorphous materials by thermal annealing has been investigated for numerous applications in the fields of nanotechnology, such as thin-film transistors and thermoelectric devices. The phase transition and shape evolution of amorphous germanium (Ge) and Ag@Ge core–shell nanoparticles with average diameters of 10 and 12 nm, respectively, were investigated by high-energy electron beam irradiation and in situ heating within a transmission electron microscope. The transition of a single Ge amorphous nanoparticle to the crystalline diamond cubic structure at the atomic scale was clearly demonstrated. Depending on the heating temperature, a hollow Ge structure can be maintained or transformed into a solid Ge nanocrystal through a diffusive process during the amorphous to crystalline phase transition. Selected area diffraction patterns were obtained to confirm the crystallization process. In addition, the thermal stability of Ag@Ge core–shell nanoparticles with an average core of 7.4 and a 2.1 nm Ge shell was studied by applying the same beam conditions and temperatures. The results show that at a moderate temperature (e.g., 385 °C), the amorphous Ge shell can completely crystallize while maintaining the well-defined core–shell structure, while at a high temperature (e.g., 545 °C), the high thermal energy enables a freely diffusive process of both Ag and Ge atoms on the carbon support film and leads to transformation into a phase segregated Ag–Ge Janus nanoparticle with a clear interface between the Ag and Ge domains. In conclusion, this study provides a protocol as well as insight into the thermal stability and strain relief mechanism of complex nanostructures at the single nanoparticle level with atomic resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Active motion of multiphase oil droplets: emergent dynamics of squirmers with evolving internal structure

Synthetic soft matter systems, when driven beyond equilibrium by active processes, offer the potential to achieve dynamical states and functions of a complexity found in living matter. Emulsions offer the basis of a simple yet versatile system for identification of the physicochemical principles underlying active soft matter, but how multiple internal phases within emulsion droplets (e.g., Janus morphologies) organize to impact emergent dynamics is not understood. Here, we create multiphase oil droplets with ultralow interfacial tensions but distinct viscosities, and drive them into motion in aqueous micellar solutions. Preferential solubilization of select components of the oil both drives the droplet motion and yields a progression of internal phase morphological states with distinct symmetries. In this work, we find the active droplets to exhibit five dynamical states during morphogenesis. By quantifying microscopic flow fields, we show that it is possible to map the diverse droplet behaviors to squirmer models of spherical microswimmers in Stokes flow, thus showing that multiphase droplets offer the basis of a versatile platform with which to study and engineer the hydrodynamics of microswimmers.

36 MATERIALS SCIENCE↗
DOE OSTI2025

One-dimensional heterocyclic carbene–Au metal–organic frameworks bridging ultra-high vacuum models and scalable liquid-phase growth

The controlled design of molecule–metal interfaces is central to the development of functional nanomaterials for catalysis, sensing, and molecular electronics. Here we show that the adsorption of a Janus-type diimidazolium precursor on gold yields one-dimensional (1D) N-heterocyclic carbene (NHC)–Au–NHC metal organic frameworks (MOFs) featuring positively charged gold nodes. Using synchrotron X-ray photoemission spectroscopy (XPS), near edge X-ray adsorption fine structure (NEXAFS) spectroscopy and scanning tunnelling microscopy (STM), we demonstrate that thermal activation promotes counterion removal and drives the formation of extended 1D arrays, characterized by ∼1.0 nm Au–Au spacing and adatom densities up to 0.6 atom nm −2 (∼4% of surface atoms). Importantly, we translate this ultra-high vacuum (UHV) benchmark into a scalable solution-phase protocol in ethanol, enabling 1D-MOF growth under mild, base-free, open-air conditions. The resulting films retain structural and electronic signatures of UHV-grown systems, bridging model studies and practical synthesis. This approach establishes NHC–metal frameworks as accessible, tunable platforms for catalysis and materials design.

Gold adatoms↗
DOE OSTI2022

Laser synthesis and processing of atomically thin 2D materials

Recent advances in laser synthesis and processing of 2D materials are described that address key issues of scalable synthesis, precise heterogeneity control, and transformative manufacturing. Here, laser spectroscopy is used to remotely characterize and optimize the structure and functionality of 2D materials, enabling their in-situ diagnostic-based synthesis and processing.

2D materials↗
DOE OSTI2025

Atomically Precise Nanoclusters as Co‐Catalysts for Light‐Activated Microswimmer Motility

Microswimmers are self-propelled particles that navigate fluid environments, offering significant potential for applications in environmental pollutant decomposition, biosensing, and targeted drug delivery. Their performance relies on engineered catalytic surfaces. Gold nanoclusters (AuNCs), with atomically precise structures, tunable optical properties, and high surface area-to-volume ratio, provide a new optimal catalyst for enhancing microswimmer propulsion. Unlike bulk gold or nanoparticles, AuNCs may deliver tunable photocatalytic activity and increased catalytic specificity, making them ideal co-catalysts for hybrid microswimmers. For the first time, this study combines AuNCs with TiO 2 /Cr 2 O 3 Janus microswimmers, combining the unique properties of both materials. This hybrid system capitalizes on the tuned optical properties of AuNCs and their role as co-catalysts with TiO 2 , driving enhanced photocatalytic performance under ultraviolet (UV) excitation. Using motion analysis, it is shown that the AuNC-microswimmers exhibit significantly greater propulsion and mean squared displacement (MSD) as compared to controls. These findings suggest that the integration of nanoclusters with semiconductor materials enables state of the art, light-switchable microswimmers. These AuNC-microswimmer systems may thus offer new opportunities for environmental catalysis and other applications, providing precise control over catalytic and motile behaviors at the microscale.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Reconfigurable Liquids Stabilized by DNA Surfactants

Polyelectrolyte microcapsules can be produced either by the layer-by-layer assembly technique or the formation of polyelectrolyte complexes at the liquid-liquid interface. In this work, we describe the design and construction of DNA microcapsules using the cooperative assembly of DNA and amine-functionalized polyhedral oligomeric silsesquioxane (POSS-NH 2 ) at the oil-water interface. "Janus-like" DNA surfactants (DNASs) assemble in situ at the interface, forming an elastic film. By controlling the jamming and unjamming behavior of DNASs, the interfacial assemblies can assume three different physical states: solid-like, elastomer-like, and liquid-like, similar to that seen with thermoplastics upon heating, that change from a glassy to a rubbery state, and then to a viscous liquid. By the interfacial jamming of DNASs, the liquid structures can be locked-in and reconfigured, showing promising potentials for drug delivery, biphasic reactors, and programmable liquid constructs.

36 MATERIALS SCIENCE↗