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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Unravelling Magnetic Nanochain Formation in Dispersion for In Vivo Applications

Self-assembly of iron oxide nanoparticles (IONPs) into 1D chains is appealing, because of their biocompatibility and higher mobility compared to 2D/3D assemblies while traversing the circulatory passages and blood vessels for in vivo biomedical applications. In this work, parameters such as size, concentration, composition, and magnetic field, responsible for chain formation of IONPs in a dispersion as opposed to spatially confining substrates, are examined. In particular, the monodisperse 27 nm IONPs synthesized by an extended LaMer mechanism are shown to form chains at 4 mT, which are lengthened with applied field reaching 270 nm at 2.2 T. The chain lengths are completely reversible in field. Using a combination of scattering methods and reverse Monte Carlo simulations the formation of chains is directly visualized. The visualization of real-space IONPs assemblies formed in dispersions presents a novel tool for biomedical researchers. This allows for rapid exploration of the behavior of IONPs in solution in a broad parameter space and unambiguous extraction of the parameters of the equilibrium structures. Additionally, it can be extended to study novel assemblies formed by more complex geometries of IONPs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Controlled release of hydrogen from composite nanoparticles

Multi-functional materials for use in reversible, high-capacity hydrogen separation and/or storage are described. Also described are systems incorporating the materials. The multi-functional materials combine a hydrogen-absorbing material with a high-efficiency and a non-contact energy-absorbing material in a composite nanoparticle. The non-contact energy-absorbing material include magnetic and/or plasmonic materials. The magnetic or plasmonic materials of the composite nanoparticles can provide localized heating to promote release of hydrogen from the hydrogen storage component of the composite nanoparticles.

Murph, Simona H.↗
DOE OSTI2021

Probing T Cell 3D Mechanosensing With Magnetically-Actuated Structures

The ability of cells to recognize and respond to the mechanical properties of their environment is of increasing importance in T cell physiology. However, initial studies in this direction focused on planar hydrogel and elastomer surfaces, presenting several challenges in interpretation including difficulties in separating mechanical stiffness from changes in chemistry needed to modulate this property. We introduce here the use of magnetic fields to change the structural rigidity of microscale elastomer pillars loaded with superparamagnetic nanoparticles, independent of substrate chemistry. This magnetic modulation of rigidity, embodied as the pillar spring constant, changed the interaction of mouse naïve CD4 + T cells from a contractile morphology to one involving deep embedding into the array. Furthermore, increasing spring constant was associated with higher IL-2 secretion, showing a functional impact on mechanosensing. The system introduced here thus separates local substrate stiffness and long-range structural rigidity, revealing new facets of T cell interaction with their environment.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Geometrically stabilized skyrmionic vortex in FeGe tetrahedral nanoparticles

The concept of topology has dramatically expanded the research landscape of magnetism, leading to the discovery of numerous magnetic textures with intriguing topological properties. A magnetic skyrmion is an emergent topological magnetic texture with a string-like structure in three dimensions and a disk-like structure in one and two dimensions. Skyrmions in zero dimensions have remained elusive due to challenges from many competing orders. Here, by combining electron holography and micromagnetic simulations, we uncover the real-space magnetic configurations of a skyrmionic vortex structure confined in a B20-type FeGe tetrahedral nanoparticle. An isolated skyrmionic vortex forms at the ground state and this texture shows excellent robustness against temperature without applying a magnetic field. Furthermore, our findings shed light on zero-dimensional geometrical confinement as a route to engineer and manipulate individual skyrmionic metastructures.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Structural Studies of Alloyed and Nanoparticle Transition Metal Dichalcogenides by Selenium-77 Solid-State Nuclear Magnetic Resonance Spectroscopy

Layered transition metal dichalcogenides (TMDCs) such as MoS 2 , MoSe 2 , and WSe 2 are under intense investigation because they are atomically thin semiconductors with photophysical properties that can be tuned by changing their composition or morphology. Mechanochemical processing has been proposed as a method to obtain alloyed TMDCs in the series Mo 1–x W x S y Se 2–y (x = 0–1; y = 0–2). However, elucidating the chemical transformations occurring at the atomic scale following mechanochemical processing can be challenging because the products are often amorphous or microcrystalline. To address this challenge, we probe TMDC mixing and alloying by using a combination of powder X-ray diffraction, Raman spectroscopy, diffuse reflectance spectroscopy, 77 Se solid-state nuclear magnetic resonance (SSNMR) spectroscopy, and planewave density functional theory (DFT) calculations. The nature of the milling material and reaction atmosphere are shown to be essential factors in limiting the formation of undesired oxide byproducts. We demonstrate acquisition of 77 Se SSNMR spectra using different combinations of Carr-Purcell Meiboom-Gill acquisition (CPMG) pulse sequences, magic angle spinning (MAS), and MAS dynamic nuclear polarization. Further, the combination of SSNMR with the other characterization methods clearly demonstrates that high energy impact ball milling induces molecular level alloying of Mo, W and chalcogen atoms in the family Mo 1–x W x S y Se 2–y . Gauge including projector augmented wave DFT calculations yield accurate 77 Se chemical shift (CS) tensor components. 77 Se SSNMR spectroscopy was also applied to study the structure of WSe 2 nanocrystals intercalated with ethylenediamine. The intercalated WSe 2 nanocrystals exhibit a more positive isotropic 77 Se CS as compared to bulk WSe 2 , however, the 77 Se CS anisotropy is the same, confirming the WSe 2 layers have a similar structure as in their bulk counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Structure-property correlations and scaling in the magnetic and magnetocaloric properties of GdCrO 3 particles

The structure, magnetic, and magnetocaloric (MC) properties of orthorhombic nanocrystalline GdCrO 3 with six particle sizes: < d > = 87, 103, 145, 224, 318, and 352 nm are reported. The particle size was tailored by annealing under different temperatures and estimated by scanning electron microscopy. With increase in < d >, Goldschmidt tolerance factor t, orthorhombic strain s, and out-of-plane Cr–O 1 –Cr bond angle first decrease, reaching minimum values for < d > = 224 nm, and then increase for sample with < d > = 318 nm and 352 nm, thus showing a V-shaped variation. Temperature dependence of the magnetization (M) reveals an antiferromagnetic transition at ${T}_{\text{N}}^{\text{Cr}}\sim 168$ K for < d > ≥ 224 nm and ${T}_{\text{N}}^{\text{Cr}}\sim 167$ K for < d > < 224 nm and an essentially d-independent spin-reorientation at T SR = 9 K. M measured at 5 K and 7 T first increases with increase in < d >, reaching maximum value for sample with < d > = 224 nm, and then decreases for samples with < d > = 318 nm and 352 nm, showing an inverted-V variation with < d >. Similar < d >-dependence is observed for the magnetic entropy change (MEC) and relative cooling power (RCP) showing a close relationship between the structural and magnetic properties of GdCrO 3 nanoparticles investigated here. The 224 nm sample with the minimum values of t, s, and Cr–O 1 –Cr bond angle exhibits the maximum value of MEC (–ΔS) = 37.8 J kg –1 K –1 at 5 K under a field variation (ΔH) of 7 T and its large estimated RCP of 623.6 J Kg –1 is comparable with those of typical MC materials. Both (–ΔS) and RCP are shown to scale with the saturation magnetization MS, suggesting that MS is the crucial factor controlling their magnitudes. Assuming (–ΔS) ~ (ΔH) n , the temperature dependence of n for the six samples are determined, n varying between 1.3 at 5 K to n = 2.2 at 130 K in line with its expected magnitudes based on mean-field theory. Furthermore, these results on structure-property correlations and scaling in GdCrO 3 suggest that its MC properties are tunable for potential low-temperature magnetic refrigeration applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Lattice symmetry breaking transition and critical size limit for ferroic orders in nanophase BiFeO3

Finite size effects on the ferroic orders in BiFeO 3 are studied by atomic pair distribution function analysis and magnetic measurements. While bulk rhombohedral BiFeO 3 exhibits ferroelectricity and antiferromagnetism with a cycloidal magnetic moment arrangement leading to zero magnetization and weak magnetoelectric coupling, BiFeO 3 nanoparticles with a size smaller than the spin cycloid period of 62 nm preserve their polar rhombohedral structure and develop ferromagnetism, thus exhibiting coexisting polarization and nonzero magnetization that enhances the magnetoelectric coupling. When the nanoparticles become smaller than 17 nm, however, their crystal lattice expands and becomes nonpolar cubic. They also become superparamagnetic and thus simultaneously cease exhibiting both ferroelectricity and ferromagnetism. Our findings shed light on the interaction between the lattice structure and ferroic orders in nanophase perovskites and also provide a rare example of a lattice symmetry breaking phase transition that determines their critical size.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

The safety of magnetic resonance imaging contrast agents

Gadolinium-based contrast agents are increasingly used in clinical practice. While these pharmaceuticals are verified causal agents in nephrogenic systemic fibrosis, there is a growing body of literature supporting their role as causal agents in symptoms associated with gadolinium exposure after intravenous use and encephalopathy following intrathecal administration. Gadolinium-based contrast agents are multidentate organic ligands that strongly bind the metal ion to reduce the toxicity of the metal. The notion that cationic gadolinium dissociates from these chelates and causes the disease is prevalent among patients and providers. We hypothesize that non-ligand-bound (soluble) gadolinium will be exceedingly low in patients. Soluble, ionic gadolinium is not likely to be the initial step in mediating any disease. The Kidney Institute of New Mexico was the first to identify gadolinium-rich nanoparticles in skin and kidney tissues from magnetic resonance imaging contrast agents in rodents. In 2023, they found similar nanoparticles in the kidney cells of humans with normal renal function, likely from contrast agents. We suspect these nanoparticles are the mediators of chronic toxicity from magnetic resonance imaging contrast agents. This article explores associations between gadolinium contrast and adverse health outcomes supported by clinical reports and rodent models.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Localized and Collective Dynamics in Liquid-like Polyethylenimine-Based Nanoparticle Organic Hybrid Materials

In this work, broadband dielectric spectroscopy, rheology, and nuclear magnetic resonance spectroscopy are employed to study molecular dynamics in a nanoparticle organic hybrid materials(NOHMs)system comprising 20 wt% silica nanoparticles ionically-bonded to a polyethylenimine canopy. By comparing the neat polymer (used as a canopy) to the derivative NOHMs, we find that timescales characterizing segmental dynamics in the NOHM are identical to those for the neat polymer. Detailed analysis of the carbon-spin lattice relaxation times yields mechanistic insights into localized and collective dynamics, in quantitative agreement with dielectric results. Interestingly, the NOHMs retain liquid-like characteristics unlike conventional polymer nanocomposites but exhibit higher viscosity due to additional contributions from tethered polymer chains, and mesoscopic structuring. These findings demonstrate the potential of achieving unique and desired material properties via NOHMs by an informed choice of the canopy material.

36 MATERIALS SCIENCE↗
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

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light–matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Nanoscale Size Effects on Push–Pull Fe–O Hybridization through the Multiferroic Transition of Perovskite ϵ-Fe 2 O 3

Multiferroics have tremendous potential to revolutionize logic and memory devices through new functionalities and energy efficiencies. To reach their optimal capabilities will require better understanding and enhancement of the ferroic orders and couplings. In this work, we use ϵ-Fe 2 O 3 as a model system with a simplifying single magnetic ion. Using 15, 20, and 30 nm nanoparticles, we identify that a modified and size-dependent Fe–O hybridization changes the spin–orbit coupling and strengthens it via longer octahedra chains. Fe–O hybridization is modified through the incommensurate phase, with a unique two-step rearrangement of the electronic environment through this transition with attraction and then repulsion of electrons around tetrahedral Fe. Interestingly, size effects disappear in the high-temperature phase where the strongest Fe–O hybridization occurs. By manipulating this hybridization, we tune and control the multiferroic properties.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Exploring Critical Synthetic Parameters for Nanoscale ε-Fe 2 O 3 and Their Influence on Magnetic Behaviors

An intermediate polymorph of iron oxide, ε-Fe 2 O 3 , has attracted significant attention due to its giant coercive field ( H c ) and potential applications in high-frequency millimeter-wave absorption and high-density magnetic recording. However, the fabrication of ε-Fe 2 O 3 with high phase purity is still a challenge due to complicated synthetic procedures and a large variety of reaction parameters. In this study, we have identified critical reaction parameters to improve the phase purity of ε-Fe 2 O 3 , and the effects of all possible reaction parameters have been tested through systematic studies. A combination of structural and magnetic characterization techniques provides us with an accurate and reliable phase purity analysis of the ε-Fe 2 O 3 phase. Specifically, we observed that (1) the reaction temperature and time and (2) the addition of Ba are critical parameters to improve the phase purity. We identified the optimal conditions that maximize the coercivity and phase purity, giving insight into the effects of each parameter on the γ- to ε- to α-phase-transition pathway. We obtained nearly single-phase ε-Fe 2 O 3 (~87 wt % with ~13 wt % α-phase) with a large coercivity of H c = 20.6 kOe, enabling us to obtain pure ε-Fe 2 O 3 by a simple magnetic separation protocol, and tuned the H c of the ε-Fe 2 O 3 nanoparticles in the range of 4.0–20.6 kOe by controlling the reaction parameters. Furthermore, the structural properties of the resulting ε-Fe 2 O 3 nanoparticles are confirmed by characterizing their chemical and magnetic properties using X-ray absorption spectroscopy and X-ray magnetic circular dichroism measurements.

36 MATERIALS SCIENCE↗
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↗
DOE OSTI2020

Competing ferro- and antiferromagnetic exchange drives shape-selective $\mathrm{Co_3O_4}$ nanomagnetism

We have synthesized three different shapes of Co 3 O 4 nanoparticles to investigate the relationships between the surface Co 2+ and Co 3+ bonding quantified by exploiting the known exposed surface planes, terminations, and coordiations of Co 3 O 4 nanoparticle spheres, cubes and plates. Subsequently this information is related to the unusual behaviour observed in the magnetism. The competition of exchange interactions at the surface provides the mechanism for different behaviours in the shapes. The cubes display weakened antiferromagnetic interactions in the form of a spin-flop that occurs at the surface, while the plates show distinct ferromagnetic behaviour due to the strong competition between the interactions. We elucidate the spin properties which are highly sensitive to bonding and crystal field environments. This work provides a new window into the mechanisms behind surface magnetism.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Insights into ε - Fe 2 O 3 interactions via Cr doping

We report innovative materials, particularly multiferroics, have the potential to transform technology. Full optimization of their usage will require an in-depth understanding of the underlying electronic and magnetic interactions. One such material is ε-Fe 2 O 3 . However, because this hard ferrimagnet with strong magnetoelectric coupling is composed of only Fe 3+ , distinguishing the role of the various sites is incredibly challenging. To overcome this challenge, Cr 3+ ions were doped into the DOh1 sites of ε-Fe 2 O 3 nanoparticles, effectively creating electron deficient defects. The ε-(Fe 1-x Cr x ) 2 O 3 (x = 0.01 to 0.12) nanoparticles have reduced μ 0 H C (T) and M S (T) as the Cr concentration increases. The impact of Cr doping on the local electronic and magnetic structure is characterized. At 10 K, subtle changes are measured, with the T d site electrons becoming increasingly localized as the concentration of electron-deficient DOh1 sites increases. Far more dramatic changes occur at 300 K, when the T d site of the ε-(Fe 1-x Cr x ) 2 O 3 splits into two distinct local environments with Fe 2+ and Fe 4+ character. The nature of this splitting suggests that dynamic electron interactions play a significant role in ε-Fe 2 O 3 ’s magnetic anisotropy and magnetoelectric properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Low-temperature MnBi alloys: Electronic and magnetic properties, constitution, morphology and fabrication (Review article)

The article reviews the rich phenomena of physical properties of MnBi. The diverse phenomena include strong spin-orbit interaction, anomalous temperature dependence of the coercivity and the magneto-crystalline anisotropy field, unique magneto-optical properties. Issues addressed include the nature of the electronic ground states of MnBi, the electronic and magnetic structures, Fermi surface, magneto-crystalline anisotropy, x-ray magnetic dichroism. The discussion includes key experiments, such as optical and magneto-optical spectroscopic measurements, de Haas-van Alphen (dHvA) measurements, x-ray photoemission and x-ray absorption spectroscopy measurements as well as x-ray magnetic circular dichroism. The effect of the spin-orbit (SO) interaction and Coulomb repulsion U were found to be crucial for the Fermi surface, cyclotron masses, magneto-optical properties, and x-ray magnetic circular dichroism. The microscopic origin of unique magneto-crystalline anisotropy and giant Kerr effect in MnBi is analyzed in detail. The huge Kerr effect in MnBi is caused by the combination of a sizable magnetic moment on manganese, the large spin-orbit coupling of bismuth, and a strong hybridization between the manganese 3d and the bismuth 6p states. The magneto-optically active states are mainly the 6p states of Bi. We show that the observed temperature dependence of the magneto-crystalline anisotropy can be explained taking into account the spin-orbit interaction together with strong Coulomb electron-electron interaction. The SO coupling of Bi is equally responsible for the large magneto-crystalline anisotropy energy as is the exchange splitting of Mn. The fabrication, morphology, and constitution of low-temperature MnBi alloys in bulk, thin films, and nanoparticles are discussed. The nanocomposite permanent magnetic materials based on MnBi, (Co, Fe) and Nd 2 Fe 14 B are also discussed.

36 MATERIALS SCIENCE↗