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At least 1,351 records · Page 75

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DOE OSTI2022

Bacterial Community Assembly, Succession, and Metabolic Function during Outdoor Cultivation of Microchloropsis salina

Outdoor cultivation of microalgae has promising potential for renewable bioenergy, but there is a knowledge gap on the structure and function of the algal microbiome that coinhabits these ecosystems. Here, we describe the assembly mechanisms, taxonomic structure, and metabolic potential of bacteria associated with Microchloropsis salina cultivated outdoors. Open mesocosms were inoculated with algal cultures that were either free of bacteria or coincubated with one of two different strains of alga-associated bacteria and were sampled across five time points taken over multiple harvesting rounds of a 40-day experiment. Using quantitative analyses of metagenome-assembled genomes (MAGs), we tracked bacterial community compositional abundance and taxon-specific functional capacity involved in algal-bacterial interactions. One of the inoculated bacteria (Alteromonas sp.) persisted and dispersed across mesocosms, whereas the other inoculated strain (Phaeobacter gallaeciensis) disappeared by day 17 while a taxonomically similar but functionally distinct Phaeobacter strain became established. The inoculated strains were less abundant than 6 numerically dominant newly recruited taxa with functional capacities for mutualistic or saprophytic lifestyles, suggesting a generalist approach to persistence. This includes a highly abundant unclassified Rhodobacteraceae species that fluctuated between 25% and 77% of the total community. Overall, we did not find evidence for priority effects exerted by the distinct inoculum conditions; all mesocosms converged with similar microbial community compositions by the end of the experiment. Instead, we infer that the 15 total populations were retained due to host selection, as they showed high metabolic potential for algal-bacterial interactions such as recycling alga-produced carbon and nitrogen and production of vitamins and secondary metabolites associated with algal growth and senescence, including B vitamins, tropodithietic acid, and roseobacticides.

rhodobacteraceae↗

DOE OSTI2025

Metagenome-assembled genomes from East River floodplain sediments near Crested Butte, CO, USA (June to September 2019)

Microorganisms play a key role in cycling nutrients and contaminants in the terrestrial environment depending on their genetic potential. Here, we present metagenome-assembled genomes (MAGs) for the bacterial and archaeal community in floodplain sediment samples taken in 2019 in June (flooded conditions) and September (drained conditions) at two locations (MCB1 and MCB3) near the Meander C/Pumphouse floodplain sites of the East River. Sediment cores were collected from 2 depths, a near-surface, generally unsaturated depth (30-40 centimeter (cm) depth below surface) and a deeper depth influenced by flooding with redoximorphic features (70-80 cm depth below surface). Sediments were homogenized from the 10 cm core for microbial analyses. A total of 24 metagenomes were sequenced through the Joint genome institute (JGI) corresponding to 8 samples sequenced in triplicate. These metagenomes can be found under Genomes Online Database (GOLD) sequencing project: Gs0141020. Metagenomes were assembled, binned, and refined using metawrap to generate MAGs (>50% complete and < 10% contamination based on checkM scores). This dataset includes a zip file of 436 MAG fasta files and a csv file with quality, taxonomic classification (Genome Taxonomy Database Release RS220), and metagenome accessions for MAGs. This dataset also includes a file-level metadata (flmd.csv) file that lists each file contained in the dataset with associated metadata and a data dictionary (dd.csv) file that contains column/row headers used throughout the files along with a definition, units, and data type.This work was supported by the Watershed Function Science Focus Area at Lawrence Berkeley National Laboratory funded by the US Department of Energy, Office of Science, Biological and Environmental Research under Contract No. DE-AC02-05CH11231. Part of this work was performed at SLAC Accelerator Laboratory funded by the US Department of Energy, Office of Science, Biological and Environmental Research under Contract No. DE-AC02-76SF00515.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Extensins: Self-Assembly, Crosslinking, and the Role of Peroxidases

The extensin (EXT) network is elaborated by the covalent intermolecular crosslinking of EXT glycoprotein monomers, and its proper assembly is important for numerous aspects of basic wall architecture and cellular defense. In this review, we discuss new advances in the secretion of EXT monomers and the molecular drivers of EXT network self-assembly. Many of the functions of EXTs are conferred through covalent crosslinking into the wall, so we also discuss the different types of known intermolecular crosslinks, the enzymes that are involved, as well as the potential for additional crosslinks that are yet to be identified. EXTs also function in wall architecture independent of crosslinking status, and therefore, we explore the role of non-crosslinking EXTs. As EXT crosslinking is upregulated in response to wounding and pathogen infection, we discuss a potential regulatory mechanism to control covalent crosslinking and its relationship to the subcellular localization of the crosslinking enzymes.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

Ideas For Infusing In-Space Servicing, Assembly and Manufacturing Concepts into Nuclear Electric Propulsion Architectures

NASA is currently investigating nuclear electric propulsion (NEP) for human Mars transport within the space nuclear propulsion portfolio. NEP spacecraft have the following characteristics, they: 1) include very large structures (~100-meter length); 2) are comprised of many components/modules; and 3) have very long lifetimes (e.g., 50 years for fuel rods). Thus, NEP spacecraft can be classified as a “persistent asset,” which is any zero-g or planetary surface system that benefits from in-space assembly (ISA) or multiple visits for servicing, repairs, and upgrades. NEP spacecraft will benefit from taking advantage of, and incorporating, In-space Servicing, Assembly, and Manufacturing (ISAM) capabilities in the spacecraft architecture from the onset, enabling system maintenance, repair, and evolution. ISA has a long history of being proposed for, and studied as, a means for achieving large systems in space. More recently, the benefits of ISA have been recognized by NASA, the Department of Defense (DOD), other government agencies, and commercial space companies, and thus, ISAM is being actively pursued at a national level. Past and current strategies for achieving large structures in space have relied largely on two strategies; the first is to launch monolithic structures (designed to meet launch vehicle requirements for payload size and mass) that are docked or berthed to other monolithic structures on-orbit to form a larger structure (e.g., the International Space Station [ISS]); the second is folding and packaging large structures to fit inside a payload fairing and deploying the full-sized structure (unaided) once on-orbit (e.g., the James Webb Space Telescope [JWST]). To date, conceptual architecture studies performed for NEP spacecraft capable of human-rated Mars transport have only included a combination of the two previously mentioned strategies. This paper will propose ideas for infusing ISAM strategies into NEP vehicle architectures that leverage existing and near future technologies and enable the resulting NEP systems to be realized in a more time- and cost-efficient manner.

in-space assembly↗

NASA NTRSDate not supplied

Ideas for Infusing In-Space Servicing, Assembly, and Manufacturing Concepts into Nuclear Electric Propulsion Architectures

in-space assembly↗

DOE OSTI2023

Ballistic Ejection of Microdroplets from Overpacked Interfacial Assemblies

Spontaneous emulsification, resulting from the assembly and accumulation of surfactants at liquid–liquid interfaces, is an interfacial instability where microdroplets are generated and diffusively spread from the interface until complete emulsification. Here, it is shown that an external magnetic field can modulate the assembly of paramagnetic nanoparticle surfactants (NPSs) at liquid–liquid interfaces to trigger an oversaturation in the areal density of the NPSs at the interface, as evidenced by a marked reduction in the interfacial tension, γ, and corroborated with a magnetostatic continuum theory. Despite the significant reduction in γ, the presence of the magnetic field does not cause stable interfaces to become unstable. Upon rapid removal of the field, however, an explosive ejection of a plume of microdroplets from the surface occurs, a dynamical interfacial instability which is termed explosive emulsification. Further, this explosive event rapidly reduces the areal density of the NPSs to its pre-field level, stabilizing the interface. The ability to externally suppress or trigger the explosive emulsification and controlled generation of tens of thousands of microdroplets, uncovers an efficient energy storage and release process, that has potential applications for controlled and directed delivery of chemicals and remotely controlled soft microrobots, taking advantage of the ferromagnetic nature of the microdroplets.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Solvent-Induced Self-Assembly Strategy to Synthesize Well-Defined Hierarchically Porous Polymers

Porous polymers with well-orchestrated nanomorphologies are useful in many fields, but high surface area, hierarchical structure, and ordered pores are difficult to be satisfied in one polymer simultaneously. A solvent-induced self-assembly strategy to synthesize hierarchical porous polymers with tunable morphology, mesoporous structure, and microporous pore wall is reported. The poly(ethylene oxide)-b-polystyrene (PEO-b-PS) diblock copolymer micelles are cross-linked via Friedel–Crafts reaction, which is a new way to anchor micelles into porous polymers with well-defined structure. Varying the polarity of the solvent has a dramatic effect upon the oleophobic/oleophylic interaction, and the self-assembly structure of PEO-b-PS can be tailored from aggregated nanoparticles to hollow spheres even mesoporous bulk. A morphological phase diagram is accomplished to systematically evaluate the influence of the composition of PEO-b-PS and the mixed solvent component on the pore structure and morphology of products. The hypercrosslinked hollow polymer spheres provide a confined microenvironment for the in situ reduction of K 2 PdCl 4 to ultrasmall Pd nanoparticles, which exhibit excellent catalytic performance in solvent-free catalytic oxidation of hydrocarbons and alcohols.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Self-Assembled Ordered Three-Phase Au-BaTiO 3 -ZnO Vertically Aligned Nanocomposites Achieved by a Templating Method

Complex multiphase nanocomposite designs present enormous opportunities for developing next-generation integrated photonic and electronic devices. Here, a unique three-phase nanostructure combining a ferroelectric BaTiO 3 , a wide-bandgap semiconductor of ZnO, and a plasmonic metal of Au toward multifunctionalities is demonstrated. By a novel two-step templated growth, a highly ordered Au–BaTiO 3 –ZnO nanocomposite in a unique “nanoman”-like form, i.e., self-assembled ZnO nanopillars and Au nanopillars in a BaTiO 3 matrix, is realized, and is very different from the random three-phase ones with randomly arranged Au nanoparticles and ZnO nanopillars in the BaTiO 3 matrix. The ordered three-phase “nanoman”-like structure provides unique functionalities such as obvious hyperbolic dispersion in the visible and near-infrared regime enabled by the highly anisotropic nanostructures compared to other random structures. Such a self-assembled and ordered three-phase nanocomposite is obtained through a combination of vapor–liquid–solid (VLS) and two-phase epitaxy growth mechanisms. In this study, we open up new possibilities in the design, growth, and application of multiphase structures and provides a new approach to engineer the ordering of complex nanocomposite systems with unprecedented control over electron–light–matter interactions at the nanoscale.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Wafer-Scale Fabrication of High-Performance n-Type Polymer Monolayer Transistors Using a Multi-Level Self-Assembly Strategy

Wafer–scale fabrication of high–performance uniform organic electronic materials is of great challenge and has rarely been realized before. Previous large–scale fabrication methods always lead to different layer thickness and thereby poor film and device uniformity. Herein, the first demonstration of 4 in. wafer–scale, uniform, and high–performance n–type polymer monolayer films is reported, enabled by controlling the multi–level self–assembly process of conjugated polymers in solution. Since the self–assembly process happened in solution, the uniform 2D polymer monolayers can be facilely deposited on various substrates, and theoretically without size limitations. Polymer monolayer transistors exhibit high electron mobilities of up to 1.88 cm 2 V –1 s –1 , which is among the highest in n–type monolayer organic transistors. This method allows to easily fabricate n–type conjugated polymers with wafer–scale, high uniformity, low contact resistance, and excellent transistor performance (better than the traditional spin–coating method). Furthermore this work provides an effective strategy to prepare large–scale and uniform 2D polymer monolayers, which could enable the application of conjugated polymers for wafer–scale sophisticated electronics.

2D organic materials↗

DOE OSTI2025

Manipulating the Assembly and Architecture of Fibrillar Silk

Silk is a unique and exceptionally strong biological material. However, no synthetic method has yet come close to replicating the properties of natural silk. This shortfall is attributed to an insufficient understanding of both silk nanofibril structure and the mechanism of formation. Here in situ atomic force microscopy (AFM) and photo-induced force microscopy (PiFM) is utilized to investigate the formation process and define the basic structural paradigm of individual silk nanofibrils. By visualizing the multistage process of silk nanofibril formation, the importance of conformational transformations along the assembly pathway is revealed. Unfolded silk structures initially accumulate into amorphous clusters, which then evolve into crystal nuclei via conformational transformation into β-crystallites. Nanofibril elongation then occurs through the attachment of silk molecules at a single end of the nanofibril tip; this is facilitated through the formation of a new amorphous cluster that then repeats the aforementioned conformational transformation. However, enzymatic digestion of the amorphous regions leads to direct, rapid elongation of β-crystalline fibers. These findings imply that the energy landscape is characterized by shallow minima associated with intermediate states, which can be eliminated by introducing β-crystallites, and motivate research into the directed modification of the silk assembly pathway to select for features beneficial to specific applications.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Photothermally Directed Assembly of Block Copolymers

Block copolymers self-assemble into nanoscale morphologies, spontaneously ordering under thermal annealing conditions owing to the chemical incompatibility between the blocks. Although the morphologies that form can be rationalized based on equilibrium arguments, the structures seen experimentally are strongly influenced by kinetic effects including process history. Recently, a variety of photothermal processing techniques have been used to control block copolymer ordering. Photothermal methods provide access to extreme conditions, including high temperatures, large heating rates, and sharp thermal gradients. Furthermore, this can be used to greatly accelerate block copolymer ordering kinetics, to pattern material order, or to probe fundamental aspects of self-assembly by exploring process histories.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

Robustness of Optical Response for Self-Assembled Plasmonic Metamaterials with Morphological Disorder and Surface Roughness

Bottom-up fabrication of metallized biotemplated nanostructures to form specific plasmonic nanoresonators holds promise as a means of achieving large-scale optical metamaterials. However, in contrast to top-down methods, the stochastic growth of self-assembled nanoresonators is prone to significant disorder and surface roughness, which naturally raise an important question about the robustness of their resonant properties in terms of structural imperfections. An aggregated-random-sphere model is developed to mimic the nucleated growth of metallized DNA origami assembly, leading to meta-atoms with realistic, experimentally observed morphological disorder and surface roughness. Using the well-known split-ring-resonator (SRR) motif as an example, the resonant properties of meta-atoms under different levels of roughness are investigated and a strong tolerance of optical response against morphological disorder is revealed. It is found that in SRRs, even with dramatic roughness introduced, the expected resonances are still observed, despite broadening line shapes compared to ideal smooth structure. Only for extreme disorder, which causes drastic segmentation of SRRs, does the resonant response disappear. Finally, the demonstrations are very encouraging for the prospects of bottom-up fabrication toward versatile functional metamaterials and metadevices.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Near‐Unity Superradiant Emission from Delocalized Frenkel Excitons in a Two‐Dimensional Supramolecular Assembly

Abstract Three general effective strategies are shown to mitigate nonradiative losses in the superradiant emission from supramolecular assemblies. J‐aggregates of 5,5′,6,6′‐tetrachloro‐1,1′‐diethyl‐3,3′‐di(4–sulfobutyl)‐benzimidazolocarbocyanine (TDBC) are used to elucidate the nature of nonradiative processes. Self‐annealing at room temperature (RT), photo‐brightening, and purification of the dye monomers are shown to all lead to substantial increases in emission quantum yields (QYs) and a concomitant lengthening of the emission lifetime, with purification having the largest effect. Structural and optical measurements are used to support a microscopic model that emphasizes the deleterious effects of a small number of impurity and defect sites that serve as nonradiative recombination centers. This understanding has yielded a molecular fluorophore in solution at RT with an unprecedented combination of fast emissive lifetime and high QY. Superradiant emission with a QY of 82% and a lifetime of 174 ps is obtained from J‐aggregates of TDBC in solution at RT. This combination of high QY and fast lifetime at RT makes supramolecular assemblies of purified TDBC a model system for the study of fundamental superradiance phenomena. High QY J‐aggregates are uniquely suited for the development of applications that require high speed and high brightness fluorophores such as devices for high‐speed optical communication.

36 MATERIALS SCIENCE↗

DOE OSTI2018

A Facile Approach to Improve Interchain Packing Order and Charge Mobilities by Self‐Assembly of Conjugated Polymers on Water

Abstract Development of facile and economic approaches for assembling organic semiconductors into more ordered structures toward high charge mobilities is highly demanding for the fabrication of organic circuits. Here a simple and facile approach is reported to prepare conjugated polymer thin films with improved crystallinities and charge mobilities by self‐assembling semiconducting polymers on water. The formation of polymer thin films with more ordered structures is attributed to coffee ring effect induced by solvent‐evaporation on water, and the hydrophobic nature of conjugated polymers that forces the polymer chains to pack densely and orderly on water surface. This approach is applicable to typical semiconducting polymers, and charge mobilities of their thin films are boosted remarkably. Finally, this new method can be utilized to easily fabricate the array of field‐effect transistors with high charge mobilities in an economic way.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Formation of Polymeric Nanocubes by Self-Assembly and Crystallization of Dithiolane-Containing Triblock Copolymers

Template–free fabrication of non–spherical polymeric nanoparticles is desirable for various applications, but has had limited success owing to thermodynamic favorability of sphere formation. Herein we present a simple way to prepare cubic nanoparticles of block copolymers by self–assembly from aqueous solutions at room temperature. Nanocubes with edges of 40–200 nm are formed spontaneously on different surfaces upon water evaporation from micellar solutions of triblock copolymers containing a central poly(ethylene oxide) block and terminal trimethylene carbonate/dithiolane blocks. These polymers self–assemble into 28±5 nm micelles in water. Upon drying, micelle aggregation and a kinetically controlled crystallization of central blocks evidently induce solid cubic particle formation. An approach for preserving the structures of these cubes in water by thiol– or photo–induced crosslinking was developed. In conclusion, the ability to solubilize a model hydrophobic drug, curcumin, was also explored.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

2D Crystal Engineering of Nanosheets Assembled from Helical Peptide Building Blocks

The successful integration of 2D nanomaterials into functional devices hinges on developing fabrication methods that afford hierarchical control across length scales of the entire assembly. We demonstrate structural control over a class of crystalline 2D nanosheets assembled from collagen triple helices. By lengthening the triple helix unit through sequential additions of Pro-Hyp-Gly triads, we achieved sub-angstrom tuning over the 2D lattice. These subtle changes influence the overall nanosheet size, which can be adjusted across the mesoscale size regime. The internal structure was observed by cryo-TEM with direct electron detection, which provides realspace high-resolution images, in which individual triple helices comprising the lattice can be clearly discerned. These results establish a general strategy for tuning the structural hierarchy of 2D nanomaterials that employ rigid, cylindrical structural units.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Using KBase to Assemble and Annotate Prokaryotic Genomes

The DOE Systems Biology Knowledgebase is an open–access bioinformatics software and data platform for analyzing plants, microbes, and their communities. KBase enables scientists to create, execute, collaborate on, and share reproducible analyses of their biological data in the context of public data and private collaborator data. For microbiologists researching prokaryotes, KBase offers analysis tools for performing quality control and assessment of Next–Generation Sequencing reads, de novo assembly, genome annotation, and tools for analyzing structural and functional features of genomes. As a result, this unit demonstrates an example workflow for taking a comparative and iterative approach to assembly and annotation of prokaryotic genomes using KBase that can be used by microbiologists seeking to perform isolate analysis in a rapid and reproducible fashion.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Co-Assembly of Carbon Nanotube Porins into Biomimetic Peptoid Membranes

Robust and cost-effective membrane-based separations are essential to solving many global crises, such as the lack of clean water. Even though the current polymer-based membranes are widely used for separations, their performance and precision can be enhanced by using a biomimetic membrane architecture that consists of highly permeable and selective channels embedded in a universal membrane matrix. Researchers have shown that artificial water and ion channels, such as carbon nanotube porins (CNTPs), embedded in lipid membranes can deliver strong separation performance. However, their applications are limited by the relative fragility and low stability of the lipid matrix. In this work, we demonstrate that CNTPs can co-assemble into two-dimension (2D) peptoid membrane nanosheets, opening up a way to produce highly programmable synthetic membranes with superior crystallinity and robustness. A combination of molecular dynamics (MD) simulations, Raman spectroscopy, X-ray diffraction (XRD), and atomic force microscopy (AFM) measurements to verify the co-assembly of CNTP and peptoids are used and show that it does not disrupt peptoid monomer packing within the membrane. In conclusion, these results provide a new option for designing affordable artificial membranes and highly robust nanoporous solids.

36 MATERIALS SCIENCE↗