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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

High‐Throughput Study of Amorphous Stability and Optical Properties of Superlattice‐Like Ge–Sb–Te Thin Films

A high‐throughput ion beam sputtering system is used to synthesize compositional gradient superlattice‐like (SLL) thin film libraries of Ge–Sb–Te alloys over the entire phase diagram. Here, the optical properties and structural evolution of the Ge–Sb–Te combinatorial SLL thin film are investigated. A systematic screening over the annealing temperature, annealing time, and modulation period has elucidated the critical factors that affect the stability of the metastable phase and optical properties. It is found that amorphous stability and optical constant are highly dependent on the modulation period and chemical composition of the thin film. This data‐driven approach offers new perspectives for accelerating the development of new materials with excellent optical and amorphous stability and for exploring their mechanisms, by greatly expanding the dataset of Ge–Sb–Te alloys with SLL structures through high‐throughput experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tailoring the γ-γ'-γ" dual superlattice microstructure of INCONEL® 725 by high temperature aging and Nb/Ta additions for superior creep properties

Next-generation energy systems require superior resistance to creep deformation due to the considerably prolonged exposure times at operating stress and temperature. To improve the elevated temperature properties of INCONEL® 725 (IN725), a corrosion resistant alloy, several variants with different Ti/Al ratio and judicious amounts of Nb and Ta were made. Furthermore, a high temperature aging (HTA) heat treatment, designed to promote favorable precipitate phase formation, was explored. These adjustments allowed to tailor the amount and type of precipitate strengthening which led to significant increases in time to failure. The Ti/Al ratio was used to favor the formation of γ' or γ" precipitates. Compact morphology precipitates, consisting of γ' precipitates surrounded by a γ" shell, were formed in alloys with a low Ti/Al ratio. The HTA increased the creep life of various alloy formulations up to a maximum improvement of 371% as compared to the standard aging heat treatment. The Nb and Ta additions had a similar effect on increasing creep life by promoting and stabilizing γ" precipitation. The positive effect of the additions was even more pronounced when coupled with the HTA. A phase stability study with up to 10,000 h exposure at 700°C revealed that the compact morphology helped in slightly reducing coarsening of the γ' precipitates, although the effect on creep was not significant. The findings of this study enable design of dual superlattice alloys through microstructural engineering that yields superior performance and can be applied to a wide range of alloys in the IN718 and derivatives family.

Antonov, Stoichko↗
DOE OSTI2020

Three-dimensional DNA-programmable nanoparticle superlattices

In recent decades, there have been considerable efforts made in the design and synthesis of materials comprised of functional nanoscale particles. However, there is an increasing need to establish platform approaches for creating large-scale three-dimensional (3D) organizations from these particles, with the ability to control and prescribe ordered structures. The use of DNA, as a means of programming interactions between nanocomponents, provides powerful and tailorable means for the rational self-assembly of nanomaterials. Here, the assembly pathway and assembled phases are highly dependent on both particle shape and interparticle interactions, governed by particle DNA coronas, binding modes, or linking mediators capable of complex topologies. This review highlights and discusses recent significant advancements in the field, as well as offers outlook towards future paths in the assembly of the DNA programmable three-dimensional nanoparticle superlattices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices

Polar vortices in oxide superlattices can be utilized as potential candidates for data storage applications due to their unique polarization topologies. The structure and dipole arrangement in polar vortices has been studied via X-ray scattering techniques, (scanning) transmission electron microscopy ((S)/TEM) and computational calculations. However, the fundamental correlation between the atomic structure and the electronic structure (which is manifested in the chemical bonding) has heretofore not been explored. Further, The hybridization between nominally empty $\textit{d}$ orbitals on the B-site with the occupied O 2$\textit{p}$ orbitals favors the condensation of a polar (ferroelectric) state in $\textit{AB}$O 3 perovskite oxides. The complex, continuously rotating local polarization texture of the vortices, in turn, can result in especially intricate $\textit{d}$- orbital interactions. Soft X-ray spectroscopy can probe these interactions at the transition metal $\textit{L}$-edge, but these techniques do not have the spatial resolution to resolve variations within one vortex (~5 nm region). Electron energy loss spectroscopy (EELS) in the STEM mode uses inelastically scattered electrons to probe the core-shell excitations (empty density of states) of transition metals at atomic resolution.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Two-Stage Assembly of Nanoparticle Superlattices with Multiscale Organization

Self-assembly processes, while promising for enabling the fabrication of complexly organized nanomaterials from nanoparticles, are often limited in creating structures with multiscale order. These limitations are due to difficulties in practically realizing the assembly processes required to achieve such complex organizations. For a long time, a hierarchical assembly attracted interest as a potentially powerful approach. However, due to the experimental limitations, intermediate-level structures are often heterogeneous in composition and structure, which significantly impacts the formation of large-scale organizations. Here, we introduce a two-stage assembly strategy: DNA origami frames scaffold a coordination of nanoparticles into designed 3D nanoclusters, and then these clusters are assembled into ordered lattices whose types are determined by the clusters’ valence. Through modulating the nanocluster architectures and intercluster bindings, we demonstrate the successful formation of complexly organized nanoparticle crystals. To conclude, the presented two-stage assembly method provides a powerful fabrication strategy for creating nanoparticle superlattices with prescribed unit cells.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Superradiance and Exciton Delocalization in Perovskite Quantum Dot Superlattices

Achieving superradiance in solids is challenging due to fast dephasing processes from inherent disorder and thermal fluctuations. Perovskite quantum dots (QDs) are an exciting class of exciton emitters with large oscillator strength and high quantum efficiency, making them promising for solid-state superradiance. However, a thorough under-standing of the competition between coherence and dephasing from phonon scattering and energetic disorder is currently unavailable. Here, we present an investigation of exciton coherence in perovskite QD solids using temperature-dependent photoluminescence line width and lifetime measurements. Our results demonstrate that excitons are coherently delocalized over 3 QDs at 11 K in superlattices leading to superradiant emission. Scattering from optical phonons leads to the loss of coherence and exciton localization to a single QD at temperatures above 100 K. Further, at low temperatures, static disorder and defects limit exciton coherence. These results highlight the promise and challenge in achieving coherence in perovskite QD solids.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Thermodynamics of Light-Induced Nanoscale Polar Structures in Ferroelectric Superlattices

Here we study the thermodynamics of nanoscale polar structures in PbTiO 3 /SrTiO 3 ferroelectric superlattices induced by above-bandgap optical excitation using a phase-field model explicitly considering both structural and electronic processes. We demonstrate that the light-excited carriers provide the charge compensation of polarization bound charges and the lattice thermal energy, both of which are key to the thermodynamic stabilization of a previously observed supercrystal, a three dimensionally periodic nanostructure, within a window of substrate strains, while different mechanical and electrical boundary conditions can stabilize a number of other nanoscale polar structures by balancing the competing short-range exchange interactions responsible for the domain wall energy and longrange electrostatic and elastic interactions. The insights into the light-induced formation and richness of nanoscale structures from this work offer theoretical guidance for exploring and manipulating the thermodynamic stability of nanoscale polar structures employing a combination of thermal, mechanical, and electrical stimuli as well as light.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ionic-like Superlattices by Charged Nanoparticles: A Step Toward Photonics Applications

Controlling interactions among nanoparticles is paramount to achieving assemblies vital to technologies seeking to exploit their cutting-edge collective properties. Although various techniques have been advanced, robust ones are necessary for upscaling nanoparticle assembly and crystallization. Here, we show that by grafting gold nanoparticles (AuNPs) with charge-end-group-thiolated poly(ethylene glycol), we control the charge of each AuNP. Such control facilitates the formation of various two-dimensional structures of oppositely charged binary constituents at vapor/liquid interfaces. Using surface-sensitive synchrotron X-ray diffraction techniques, we established the formation of distinct checkerboard square lattice structures at a range of pH values and molar ratios of the constituents. By regulating pH, the superlattices can transform from a square to a hexagonal lattice, or vice versa, and to a single-component superstructure at the interface. In conclusion, our recipe for the control of charges and their consequent interactions among nanoparticles can be readily exploited in the assembly of photonics and plasmonics devices in two and three dimensions.

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

Superlattices are Greener on the Other Side: How Light Transforms Self-Assembled Mixed Halide Perovskite Nanocrystals

Perovskite nanocrystal superlattices (NC SLs) are the nearest real-world approximations to monodisperse NC ensembles. NC SLs thus represent ideal model systems for evaluating the optical and structural stability of CsPb(I 1– x Br x ) 3 NCs at a macroscopic level. Here, photoinduced changes to CsPb(I 1– x Br x ) 3 NC SLs (0 < x < 1.0) are probed via in situ photoluminescence, X-ray diffraction, and electron microscopy. We find that prolonged (~10–20 h) ultraviolet–visible irradiation causes irreversible PL blueshifts, photobrightening, and crystal structure contractions. These changes stem from gradual photoinduced I 2 sublimation, which transforms CsPb(I 1– x Br x ) 3 into CsPbBr 3 . Despite eliminating half of the initial halides from individual CsPb(I 0.53 Br 0.47 ) 3 particles, NCs within SLs remarkably preserve their initial crystallinity, cuboidal shapes, edge lengths, and size distributions. This work illustrates compositional control toward generating precisely engineered perovskite NC SLs. It also highlights iodide photo-oxidation as a hurdle that must be overcome if mixed halide perovskite nanomaterials are to be applied beyond fundamental studies.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Phase Diagram and Structure Map of Binary Nanoparticle Superlattices from a Lennard-Jones Model

A first-principles prediction of the binary nanoparticle phase diagram assembled by solvent evaporation has eluded theoretical approaches. In this paper, we show that a binary system interacting through the Lennard-Jones (LJ) potential contains all experimental phases in which nanoparticles are effectively described as quasi hard spheres. We report a phase diagram consisting of 53 equilibrium phases, whose stability is quite insensitive to the microscopic details of the potentials, thus giving rise to some type of universality. Furthermore, we show that binary lattices may be understood as consisting of certain particle clusters, i.e., motifs, that provide a generalization of the four conventional Frank–Kasper polyhedral units. Our results show that metastable phases share the very same motifs as equilibrium phases. Finally, we discuss the connection with packing models, phase diagrams with repulsive potentials, and the prediction of likely experimental superlattices.

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

Confined Growth of DNA-Assembled Superlattice Films

Here, we study the assembly of DNA-functionalized nanocubes under lateral confinement in microscale square trenches on a DNA-functionalized substrate. Microfocus small-angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) are used to characterize the superlattices (SLs). The results indicate that nanocubes form simple-cubic SLs with square-prism morphology and a (100) out-of-plane orientation to maximize DNA bonding. In-plane, SLs align with the template, exposing their {100} side facets, and the degree of alignment depends on trench size. Interestingly, the distribution of in-plane orientations determined from SAXS and SEM do not agree, indicating that the internal and external structures of the SLs differ. To understand this discrepancy, X-ray ptychography is employed to image the internal structures of the SLs, revealing that SLs which appear to be single-crystalline in SEM may have subsurface grain boundaries, depending on trench size. SEM reveals that the SLs grow via nucleation and growth of randomly oriented domains, which then coalesce; this mechanism explains the observed dependence of alignment and defect structure on size. Interestingly, crystallization occurs via an unusual growth mode, whereby continuous SL layers grow on top of several misoriented islands. Overall, this work elucidates the effect of lateral confinement on the crystallization of DNA-functionalized nanoparticles and shows how X-ray ptychography can be used to gain insight into nanoparticle crystallization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

In Situ X-ray Scattering Reveals Coarsening Rates of Superlattices Self-Assembled from Electrostatically Stabilized Metal Nanocrystals Depend Nonmonotonically on Driving Force

Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with promising functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases in situ and in real time of an electrostatically stabilized Au NC solution before, during, and after it is quenched to form SLs using small-angle X-ray scattering. By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics of the colloidal and SL phases as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their diameter. We find the degree of SL order is primarily determined by fast (subsecond) initial nucleation and growth kinetics, while coarsening at later times depends nonmonotonically on the driving force for self-assembly. We validate these results by direct comparison with simulations and use them to suggest dynamic design principles to optimize the crystallinity within a finite time window. The combination of this measurement methodology, quantitative analysis, and simulation should be generalizable to elucidate and better control the microscopic self-assembly pathways of a wide range of bottom-up assembled systems and architectures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nanoparticle Superlattices through Template-Encoded DNA Dendrimers

The chemical interactions that lead to the emergence of hierarchical structures are often highly complex and difficult to program. In this paper, the synthesis of a series of superlattices based upon 30 different structurally reconfigurable DNA dendrimers is reported, each of which presents a well-defined number of single-stranded oligonucleotides (i.e., sticky ends) on its surface. Such building blocks assemble with complementary DNA-functionalized gold nanoparticles (AuNPs) to yield five distinct crystal structures, depending upon choice of dendrimer and defined by phase symmetry. These DNA dendrimers can associate to form micelle-dendrimers, whereby the extent of association can be modulated based upon surfactant concentration and dendrimer length to produce a low-symmetry Ti5Ga4-type phase that has yet to be reported in the field of colloidal crystal engineering. Taken together, colloidal crystals that feature three different types of particle bonding interactions.template-dendron, dendrimer-dendrimer, and DNA-modified AuNP-dendrimer.are reported, illustrating how sequence-defined recognition and dynamic association can be combined to yield complex hierarchical materials.

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

Self-Assembly of Atomically Aligned Nanoparticle Superlattices from Pt–Fe 3 O 4 Heterodimer Nanoparticles

Multicomponent nanoparticle superlattices (SLs) promise the integration of nanoparticles (NPs) with remarkable electronic, magnetic, and optical properties into a single structure. Here, we demonstrate that heterodimers consisting of two conjoined NPs can self-assemble into novel multicomponent SLs with a high degree of alignment between the atomic lattices of individual NPs, which has been theorized to lead to a wide variety of remarkable properties. Specifically, by using simulations and experiments, we show that heterodimers composed of larger Fe 3 O 4 domains decorated with a Pt domain at one vertex can self-assemble into an SL with long-range atomic alignment between the Fe 3 O 4 domains of different NPs across the SL. The SLs show an unanticipated decreased coercivity relative to nonassembled NPs. In situ scattering of the self-assembly reveals a two-stage mechanism of self-assembly: translational ordering between NPs develops before atomic alignment. Here our experiments and simulation indicate that atomic alignment requires selective epitaxial growth of the smaller domain during heterodimer synthesis and specific size ratios of the heterodimer domains as opposed to specific chemical composition. This composition independence makes the self-assembly principles elucidated here applicable to the future preparation of multicomponent materials with fine structural control.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Dynamic Nanocrystal Superlattices with Thermally Triggerable Lubricating Ligands

The size-dependent and collective physical properties of nanocrystals (NCs) and their self-assembled superlattices (SLs) enable the study of mesoscale phenomena and the design of metamaterials for a broad range of applications. However, the limited mobility of NC building blocks in dried NCSLs often hampers the potential for employing postdeposition methods to produce high-quality NCSLs. In this study, we present tailored promesogenic ligands that exhibit a lubricating property akin to thermotropic liquid crystals. The lubricating ability of ligands is thermally triggerable, allowing the dry solid NC aggregates deposited on the substrates with poor ordering to be transformed into NCSLs with high crystallinity and preferred orientations. The interplay between the dynamic behavior of NCSLs and the molecular structure of the ligands is elucidated through a comprehensive analysis of their lubricating efficacy using both experimental and simulation approaches. Coarse-grained molecular dynamic modeling suggests that a shielding layer from mesogens prevents the interdigitation of ligand tails, facilitating the sliding between outer shells and consequently enhancing the mobility of NC building blocks. Further, the dynamic organization of NCSLs can also be triggered with high spatial resolution by laser illumination. The principles, kinetics, and utility of lubricating ligands could be generalized to unlock stimuli-responsive metamaterials from NCSLs and contribute to the fabrication of NCSLs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Dynamic Transformation of High-Architectural Nanocrystal Superlattices upon Solvent Molecule Exposure

The cluster-based body-centered-cubic superlattice (cBCC SL) represents one of the most complicated structures among reported nanocrystal assemblies, comprised of 72 truncated tetrahedral quantum dots per unit cell. Our previous report revealed that truncated tetrahedral quantum dots within cBCC SLs possessed highly controlled translational and orientational order owing to an unusual energetic landscape based on the balancing of entropic and enthalpic contributions during the assembly process. However, the cBCC SL’s structural transformability and mechanical properties, uniquely originating from such complicated nanostructures, have yet to be investigated. Herein, we report that cBCC SLs can undergo dynamic transformation to face-centered-cubic SLs in response to post-assembly molecular exposure. We monitored the dynamic transformation process using in situ synchrotron-based small-angle X-ray scattering, revealing a dynamic transformation involving multiple steps underpinned by interactions between incoming molecules and TTQDs’ surface ligands. Furthermore, our mechanistic study demonstrated that the precise configuration of TTQDs’ ligand molecules in cBCC SLs was key to their high structural transformability and unique jelly-like soft mechanical properties. While ligand molecular configurations in nanocrystal SLs are often considered minor features, our findings emphasize their significance in controlling weak van der Waals interactions between nanocrystals within assembled SLs, leading to previously unremarked superstructural transformability and unique mechanical properties. Finally, our findings promote a facile route toward further creation of soft materials, nanorobotics, and out-of-equilibrium assemblies based on nanocrystal building blocks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Growth of Nanocrystal Superlattices from Liquid Crystals

The growth of superlattices (SLs) made from self-assembled nanocrystals (NCs) is a powerful method for creating new materials and gaining insight into fundamental molecular dynamics. Previous explorations of NCSL syntheses have mostly compared them to crystallization. However, NCSL synthesis has not broadly shown cooling crystallization from saturated solutions as a reversible crystallization–dissolution process. We demonstrate the reversible growth of NCSLs by dispersing NCs in liquid crystal (LC) “smart solvents,” and harnessing the transitions between the isotropic and nematic phases of the LCs. The growth mode and morphology can be tuned. Furthernore, this process is a model platform for studying crystallization and demonstrates great potential in manufacturing NCSLs as colloidal crystals through liquid-phase epitaxy or colloidal synthesis.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Dielectric catastrophe at the Wigner-Mott transition in a moiré superlattice

The bandwidth-tuned Wigner-Mott transition is an interaction-driven phase transition from a generalized Wigner crystal to a Fermi liquid. Because the transition is generally accompanied by both magnetic and charge-order instabilities, it remains unclear if a continuous Wigner-Mott transition exists. Here, we demonstrate bandwidth-tuned metal-insulator transitions at fixed fractional fillings of a MoSe 2 /WS 2 moiré superlattice. The bandwidth is controlled by an out-of-plane electric field. The dielectric response is probed optically with the 2s exciton in a remote WSe 2 sensor layer. The exciton spectral weight is negligible for the metallic state with a large negative dielectric constant. It continuously vanishes when the transition is approached from the insulating side, corresponding to a diverging dielectric constant or a ‘dielectric catastrophe’ driven by the critical charge dynamics near the transition. Our results support the scenario of continuous Wigner-Mott transitions in two-dimensional triangular lattices and stimulate future explorations of exotic quantum phases in their vicinities.

42 ENGINEERING↗