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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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13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Ultrastrong colloidal crystal metamaterials engineered with DNA

Lattice-based constructs, often made by additive manufacturing, are attractive for many applications. Typically, such constructs are made from microscale or larger elements; however, smaller nanoscale components can lead to more unusual properties, including greater strength, lighter weight, and unprecedented resiliencies. Here, solid and hollow nanoparticles (nanoframes and nanocages; frame size: ~15 nanometers) were assembled into colloidal crystals using DNA, and their mechanical strengths were studied. Nanosolid, nanocage, and nanoframe lattices with identical crystal symmetries exhibit markedly different specific stiffnesses and strengths. Unexpectedly, the nanoframe lattice is approximately six times stronger than the nanosolid lattice. Nanomechanical experiments, electron microscopy, and finite element analysis show that this property results from the buckling, densification, and size-dependent strain hardening of nanoframe lattices. Last, these unusual open architectures show that lattices with structural elements as small as 15 nanometers can retain a high degree of strength, and as such, they represent target components for making and exploring a variety of miniaturized devices.

42 ENGINEERING↗
DOE OSTI2020

Dynamically controlled random lasing with colloidal titanium carbide MXene

Control of lasing properties through tailorable and dynamically tunable materials and reconfigurable compositions can augment the performance of random lasers for a wide range of applications. Here, a colloid of randomly dispersed weakly scattering single-layer titanium carbide (Ti 3 C 2 T x ) MXene flakes embedded within rhodamine 101 gain medium is experimentally shown to provide feedback for random lasing. Additionally, in contrast to previously reported random laser systems where the optical properties of scatterers are static, the relative permittivity of Ti 3 C 2 T x MXene flakes can be varied under optical pumping due to the saturable absorption properties. Numerical simulations indicate that the observed nonlinear response of Ti 3 C 2 T x MXene flakes enables dynamically tunable random lasing. Thus, pumping the Ti 3 C 2 T x MXene flakes with a second optical source decreases the gain threshold required to obtain random lasing. Also, using numerical simulations, it is shown that the control over the intensity of the second pump enables tuning the field distribution of the random lasing modes. Considering the diversity of the MXenes family, the proposed MXene colloidal metamaterial design opens up a new avenue to advanced control of lasing properties for photonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Mie-Resonant Three-Dimensional Metacrystals

Optical metamaterials, engineered to exhibit electromagnetic properties not found in natural materials, may enable new light-based applications including cloaking and optical computing. While there have been significant advances in the fabrication of two-dimensional metasurfaces, planar structures create nontrivial angular and polarization sensitivities, making omnidirectional operation impossible. Although three-dimensional (3D) metamaterials have been proposed, their fabrication remains challenging. In this work, we use colloidal crystal engineering with DNA to prepare isotropic 3D metacrystals from Au nanocubes. We show that such structures can exhibit refractive indices as large as ~8 in the mid-infrared, far greater than that of common high-index dielectrics. Additionally, we report the first observation of multipolar Mie resonances in metacrystals with well-formed habits, occurring in the mid-infrared for sub-micron metacrystals, which we measured using synchrotron infrared microspectroscopy. Finally, we predict that arrays of metacrystals could exhibit negative refraction. The results present a promising platform for engineering devices with unnatural optical properties.

3D metamaterials↗
DOE OSTI2020

Device-quality, reconfigurable metamaterials from shape-directed nanocrystal assembly

Significance Colloidal nanocrystals with defined sizes and shapes are ideal building blocks for nanofabrication. However, the ability to arbitrarily arrange them on surfaces with control over their orientation remains elusive. Here we report a shallow-template-assisted DNA-mediated assembly strategy to precisely arrange colloidal nanocrystals on surfaces, with single-particle control across submillimeter areas. In addition, the oligonucleotide bonds between the nanocrystals and substrate can be reversibly expanded and contracted enabling postsynthetic tunability of the assembled structures. Using this approach, we synthesized a nanocrystal-based, dynamically tunable metasurface (an anomalous reflector), thereby illustrating the potential for unique device construction via DNA programmable assembly.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Space-tiled colloidal crystals from DNA-forced shape-complementary polyhedra pairing

Generating space-filling arrangements of most discrete polyhedra nanostructures of the same shape is not possible. However, if the appropriate individual building blocks are selected (e.g., cubes), or multiple shapes of the appropriate dimensions are matched (e.g., octahedra and tetrahedra) and their pairing interactions are subsequently forced, space-filled architectures may be possible. With flexible molecular ligands (polyethylene glycol–modified DNA), the shape of a polyhedral nanoparticle can be deliberately altered and used to realize geometries that favor space tessellation. In this work, 10 new colloidal crystals were synthesized from DNA-modified nanocrystal building blocks that differed in shapes and sizes, designed to form space-filling architectures with micron-scale dimensions. The insights and capabilities provided by this new strategy substantially expand the scope of colloidal crystals possible and provide an expanded tool kit for researchers interested in designing metamaterials.

Science & Technology - Other Topics↗
DOE OSTI2026

Reconfigurable self-assembly of porous anisotropic colloids in nematic liquid crystals

Dispersions of anisotropic nanoparticles in liquid crystalline hosts recently yielded new soft condensed matter states, like the thermally reconfigurable monoclinic and orthorhombic biaxial nematic liquid crystals, with a plethora of unusual phases and phase transformations. Our current study shows that the nanoscale porous nature of colloids with micrometer-range overall dimensions also enables highly reconfigurable orientations and assemblies of the microparticles, allowing for realization of condensed matter states with unusual combinations of low-symmetry nematic or smectic order and fluidity. Much like the anisotropic nanoparticles studied previously, these nanoporous anisotropic colloids exhibit thermally reconfigurable oriented alignment with respect to the far-field director, as well as diverse low-symmetry liquid crystalline phase behaviors. Furthermore, our findings open doors to fundamental and applied uses of low-symmetry molecular-colloidal orientationally ordered states of matter with uninhibited fluidity, as well as liquid crystals with partial positional ordering, like low-symmetry smectics, which could lead to applications in metamaterial designs, electro-optics, photonics, etc.

colloidal dispersion↗
DOE OSTI2023

Design of functional materials based on new principles of disorder

The main goal of the project for many years was to study and understand the jamming transition and the properties of the marginally jammed state, and to apply that understanding to real systems, including atomic, molecular, metallic and polymeric glasses, colloidal suspensions, granular materials, foams and emulsions, as well as the dynamics of systems driven away from the static jammed state by applying temperature or strain. As we gained greater insight into the jamming problem, we applied it to other big problems that had not previously been recognized as being related to jamming, such as memory formation, metamaterials design and learning.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Finely tunable dynamical coloration using bicontinuous micrometer-domains

Nanostructures similar to those found in the vividly blue wings of Morpho butterflies and colorful photonic crystals enable structural color through constructive interference of light waves. Different from commonly studied structure-colored materials using periodic structures to manipulate optical properties, we report a previously unrecognized approach to precisely control the structural color and light transmission via a novel photonic colloidal gel without long-range order. Nanoparticles in this gel form micrometer-sized bicontinuous domains driven by the microphase separation of binary solvents. This approach enables dynamic coloration with a precise wavelength selectivity over a broad range of wavelengths extended well beyond the visible light that is not achievable with traditional methods. The dynamic wavelength selectivity is thermally tunable, reversible, and the material fabrication is easily scalable.

42 ENGINEERING↗
DOE OSTI2022

In-situ imaging of nucleation and growth of superlattices from nanoscale colloidal nanoparticles

Nanoparticle-based superlattices have attracted extensive research efforts due to their versatile composition and packing-dependent optical, magnetic, electronic, catalytic, mechanical properties. Yet the experimental understanding of the thermodynamics and pathways of the crystallization processes for these systems, which govern their ultimate morphology, size, and packing structure, has for long remained underexplored. Here, this minireview highlights recent integration of liquid-phase transmission electron microscopy, which allows for real-space, real-time direct imaging of the crystallization processes at the single-particle level, with simulation and the conceptual framework established by pioneers such as Dr. A. A. Chernov. Different aspects of superlattice formation were revealed by direct imaging for the first time, such as the existence of prenucleation precursor in nonclassical crystallization, surface energy-dependent growth, and coalescence, allowing for the charting of phase coordinates and thermodynamic quantities at the nanoscale. We discuss the similarities and differences of crystal growth behaviors in atomic and nanoparticle systems, as well as engineering opportunities to fashion, shape, and achieve quality control in superlattice formation from nanoparticles, for next-generation optical and mechanical metamaterials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Transport of polymer-coated metal–organic framework nanoparticles in porous media

Abstract Injecting fluids into deep underground geologic structures is a critical component to development of long-term strategies for managing greenhouse gas emissions and facilitating energy extraction operations. Recently, we reported that metal–organic frameworks are low-frequency, absorptive-acoustic metamaterial that may be injected into the subsurface to enhance geophysical monitoring tools used to track fluids and map complex structures. A key requirement for this nanotechnology deployment is transportability through porous geologic media without being retained by mineral-fluid interfaces. We used flow-through column studies to estimate transport and retention properties of five different polymer-coated MIL-101(Cr) nanoparticles (NP) in siliceous porous media. When negatively charged polystyrene sulfonate coated nanoparticles (NP-PSS-70K) were transported in 1 M NaCl, only about 8.4% of nanoparticles were retained in the column. Nanoparticles coated with polyethylenimine (NP-PD1) exhibited significant retention (> 50%), emphasizing the importance of complex nanoparticle-fluid-rock interactions for successful use of nanofluid technologies in the subsurface. Nanoparticle transport experiments revealed that nanoparticle surface characteristics play a critical role in nanoparticle colloidal stability and as well the transport.

58 GEOSCIENCES↗
DOE OSTI2021

Low-Density 2D Superlattices Assembled via Directional DNA Bonding

It is critical to assemble nanoparticles (NPs) into superlattices with controlled symmetries and spacings on substrates for metamaterials applications, where such structural parameters dictate their properties. Here, we use DNA to assemble anisotropic NPs of three shapes-cubes, octahedra, and rhombic dodecahedra-on substrates and investigate their thermally induced reorganization into two-dimensional (2D) crystalline films. We report two new low-density 2D structures, including a honeycomb lattice based on octahedral NPs. The low-density lattices favored here are not usually seen when particles are crystallized via other bottom-up assembly techniques. Furthermore, we show that, consistent with the complementary contact model, a primary driving force for crystallization is the formation of directional, face-to-face DNA bonds between neighboring NPs and between NPs and the substrate. Finally, our results can be used to deliberately prepare crystalline NP films with novel morphologies.

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

Nanoparticle self-assemblies with modern complexity

Thanks to decades of tireless efforts, nanoparticle assemblies have reached at an extremely high level of controllability, sophistication, and complexity, with new insights provided by integration with graph theory, cutting-edge characterization, and machine learning (ML)-based computation and modeling, as well as with ever-diversifying applications in energy, catalysis, biomedicine, optics, electronics, magnetics, organic biosynthesis, and quantum technology. Nanoparticle assemblies can be crystalline, known as superlattices or supracrystals. Their assembly entails a transition from disorder—dispersed nanoparticles—to order, which can be achieved through classical nucleation pathways or nonclassical pathways via prenucleation precursors or particle aggregation. Further, the periodic lattices allow facile manipulations of electrons, phonons, photons, and even spins, leading to advanced device components and metamaterials. Meanwhile, aperiodic assemblies out of nanoparticles, such as gels, networks, and amorphous solids, also start to attract attentions. Despite the loss of periodicity, symmetry-lowering or symmetry-breaking three-dimensional (3D) structures emerge with unique properties, such as chiroptical activity, topological mechanical strength, and quantum entanglement. Real-space imaging such as electron microscopy and X-ray based tomography methods are utilized to characterize these complex structures, while mathematical tools such as graph theories are in need to describe such complex structures. This issue aims to provide a timely review of the efforts in this greatly broadened materials design space including experiment, simulation, theory, and applications. Nine top experts (and their teams) from four countries deliver six review papers, summarizing fundamental mechanistic understandings of nanoparticle assemblies, highlighted with the developments of state-of-the-art in situ characterization tools and ML-assisted reverse engineering, and newly emergent applications of nanoarchitectures.

36 MATERIALS SCIENCE↗