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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Utilization of the LS-APGD microplasma/orbitrap-FTMS booster system for detection and isotopic analysis of neodymium nanoparticles

Detection and isotopic analysis of particle populations has seen rapid growth across several application areas, including environmental analysis, nuclear forensics, and food safety. The ability to characterize the particles' unique elemental and isotopic fingerprints could provide information related to formation, processing history, and transport. Regarding nuclear forensics, isotopic analysis of particles derived from diverse materials is often used as a tool to trace the origin and processing history. Mass spectrometric-based techniques currently used for particle population analysis often suffer from limited mass resolution, particularly when dealing with real-world samples that are affected by isobaric and polyatomic interferences from the matrix. To address these analytical challenges, we propose a novel method utilizing the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled to an ultrahigh resolution Orbitrap mass spectrometer, further enhanced with the FTMS X2T Booster data acquisition and processing unit. The FTMS Booster enables acquisition of extended transient times of up to 3 s, significantly improving mass resolution, thereby reducing or even eliminating the need for prior separation of isobaric or polyatomic interferences. Additionally, the detection of low-abundance isotopes was improved by increasing the signal-to-noise (S/N) ratio. As proof of concept, this study demonstrates the feasibility of the LS-APGD/Orbitrap-FTMS X2T Booster platform for direct analysis using a suspension of well-characterized ∼120 nm neodymium particles. The quality of the isotope ratios values obtained from a few hundred particles were in good agreement with those obtained from homogeneous ionic solutions. These results highlight the potential of the LS-APGD/Orbitrap platform for rapid, accurate, and interference-resilient isotope ratio analysis of particle populations without the need for dissolution and subsequent chemical separations, offering significant advantages for nuclear forensics, safeguards, and environmental applications. The effort here also points to further paths forward, hopefully towards single particle (SP) analysis using microplasma ionization and the ultrahigh resolving power of the Orbitrap mass analyzer.

FTMS X2T booster↗
DOE OSTI2021

Laminar and turbulent plasmoid ejection in a laboratory Parker Spiral current sheet

Quasi-periodic plasmoid formation at the tip of magnetic streamer structures is observed to occur in experiments on the Big Red Ball as well as in simulations of these experiments performed with the extended magnetohydrodynamics code, NIMROD. This plasmoid formation is found to occur on a characteristic time scale dependent on pressure gradients and magnetic curvature in both experiment and simulation. Single mode, or laminar, plasmoids exist when the pressure gradient is modest, but give way to turbulent plasmoid ejection when the system drive is higher, which produces plasmoids of many sizes. However, a critical pressure gradient is also observed, below which plasmoids are never formed. A simple heuristic model of this plasmoid formation process is presented and suggested to be a consequence of a dynamic loss of equilibrium in the high- $\beta$ region of the helmet streamer. This model is capable of explaining the periodicity of plasmoids observed in the experiment and simulations, and produces plasmoid periods of 90 minutes when applied to two-dimensional models of solar streamers with a height of $3R_\odot$ . This is consistent with the location and frequency at which periodic plasma blobs have been observed to form by Large Angle and Spectrometric Coronograph and Sun Earth Connection Coronal and Heliospheric Investigation instruments.

Physics↗
DOE OSTI2024

Expanding the Design Space of Polymer–Metal Organic Framework (MOF) Gels by Understanding Polymer–MOF Interactions

The fabrication of polymer-MOF composite gels holds great potential to provide emergent properties for drug delivery, environmental remediation, and catalysis. To leverage the full potential of these composites, we investigated how the presence and chemistry of polymers impact MOF formation within the composites and, in turn, how MOFs impact polymer gelation. We show that polymers with a high density of strongly metal-binding carboxylic acids inhibit MOF formation; however, reducing the density of carboxylic acids or substituting them with weaker metal-binding hydroxyl groups permits both MOF formation and gelation within composites. Preparing composites with poly(ethylene glycol) (PEG), which does not bind MOF zirconium (Zr)-oxo clusters, and observing gelation suggests that MOFs can entrap polymer chains to create cross-links in addition to cross-linking them through polymer-Zr-oxo interactions. Both simulations and experiments show composite hydrogels formed with poly(vinyl alcohol) (PVA) to be more stable than those made with PEG, which can reptate through MOF pores upon heating. We demonstrate the generalizability of this composite formation process across different Zr-based MOFs (UiO-66, NU-901, UiO-67, and MOF-525) and by spin-coating gels into conformable films. PVA-UiO-66 composite hydrogels demonstrated high sorption and sustained release of methylene blue relative to the polymer alone (3× loading, 28× slower release), and PVA-MOF-525 composite hydrogels capably sorb the therapeutic peptide Angiotensin 1–7. By understanding the influence of polymer-MOF interactions on the structure and properties of composite gels, this work informs and expands the design space of this emerging class of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Electrochemically-Formed Disordered Rock Salt ω-Li x V 9 Mo 6 O 40 as a Fast-Charging Li-Ion Electrode Material

Electrochemically-formed disordered rock salt compounds are an emerging class of Li-ion electrode materials for fast-charging energy storage. However, the specific factors that govern the formation process and the resulting charge storage performance are not well understood. Here, we characterize the transformation mechanism and charge storage properties of an electrochemically-formed disordered rock salt from V 9 Mo 6 O 40 (VMO). The crystal structure of VMO has similar motifs to that of α-V 2 O 5 , a well-studied analogue, but VMO has less mechanical flexibility due to additional corner-sharing octahedra in its structure. As a result, VMO undergoes a single-step transformation pathway, which we characterize through operando X-ray diffraction, and forms an unusual highly distorted lamellar microstructure, as we show with high-resolution transmission electron microscopy. The resulting Li x VMO material shows fast charging and other electrochemical characteristics and performance typical of many nanomaterials, even though the material is composed of relatively large particles.

25 ENERGY STORAGE↗
DOE OSTI2025

Volumetric Shaping of Nanoparticle-DNA Crystals by Light-Induced Milling

DNA-programmable self-assembly enables the formation of nanoparticle crystals with controlled lattice symmetry. While this approach offers the formation of complexly ordered nanostructures for optical, mechanical, and biological applications, a mesoscale control over such nanomaterials is limited. Directing the material formation process through the assembly pathway or external fields allows for modulating crystal morphology, but achieving arbitrary morphology remains challenging. Here, we present a photothermal method for shaping 3D DNA-programmable crystals of gold nanoparticles. Through local heating of nanoparticles due to plasmonic light absorption, we induce targeted volumetric dissolution of specifically defined crystal areas with micron-scale accuracy. This technique effectively prescribes crystal shaping and creates arbitrarily shaped voids within crystals. We further investigate both computationally and experimentally the key factors governing volumetric material subtraction. The developed automated light-milling platform enables the fabrication of nanomaterials exhibiting both DNA-programmable nanoscale order and custom-designed mesoscale architecture.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A New Cathode Material for a Li–O 2 Battery Based on Lithium Superoxide

Li–O 2 batteries suffer from large charge overpotentials due to the high charge transfer resistance of Li 2 O 2 discharge products. A potential solution to this problem is the development of LiO 2 -based batteries that possess low charge overpotentials due to the lower charge transfer resistance of LiO 2 . In this report, IrLi nanoparticles were synthesized and implemented for the first time as a LiO 2 battery cathode material. The IrLi nanoparticle synthesis was achieved by a temperature- and time-optimized thermal reaction between a precise ratio of iridium nanoparticles and lithium metal. Li–O 2 batteries employing the IrLi-rGO cathodes were cycled up to 100 cycles at moderate current densities with sustained low cell charge potentials (<3.5 V). Further, various characterization techniques, including SEM, DEMS, TEM, Raman, and titration, were used to demonstrate the LiO 2 discharge product and the absence of Li 2 O 2 . On the basis of first-principles calculations, it was concluded that the formation of crystalline LiO 2 can be stabilized by epitaxial growth on the (111) facets of IrLi nanoparticles present on the cathode surface. These findings demonstrate that, in addition to the previously studied Ir 3 Li intermetallic, the IrLi intermetallic also provides a means by which LiO 2 discharge products can be stabilized and confirms the importance of templating for the formation process.

25 ENERGY STORAGE↗
DOE OSTI2024

Mechanistic Insights into the Origins of Selectivity in a Cu-Catalyzed C–H Amidation Reaction

The catalytic transformation of C-H to C-N bonds offers rapid access to fine chemicals and high-performance materials, but achieving high selectivity from undirected aminations of unactivated C(sp 3 )-H bonds remains an outstanding challenge. Here, we report the origins of the reactivity and selectivity of a Cu-catalyzed C-H amidation of simple alkanes. Using a combination of experimental and computational mechanistic studies and energy decomposition techniques, we uncover a switch in mechanism from inner-sphere to outer-sphere coupling between alkyl radicals and the active Cu(II) catalyst with increasing substitution of the alkyl radical. The combination of computational predictions and detailed experimental validation shows that simultaneous minimization of both Cu-C covalency and alkyl radical size increases the rate of reductive elimination and that both strongly electron-donating and electron-withdrawing substituents on the catalyst accelerate the selectivity-determining C-N bond formation process as a result of a change in mechanism. These findings offer design principles for the development of improved catalyst scaffolds for radical C-H functionalization reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Multi‐Species Energy‐Banded Ions in the Ionosphere During the 21 January 2005 Magnetic Storm: Low‐Altitude Edge of the Warm Plasma Cloak

During the 21–22 January 2005 magnetic storm, the FAST satellite observed warm (< few keV) ions in discrete energy bands on the dayside at ∼3,000 km altitude for more than 6.5 hr. We suggest that the ionospheric energy-banded ions represent the low-altitude edge of the warm plasma cloak observed simultaneously by magnetospheric satellites. This is a clear example of the multi-species ion energy bands (10 eV to several keV) observed during strong magnetic storms by the FAST satellite, stretching from the diffuse auroral region to the plasmapause with lifetimes up to 12 hr. The close association of these energy-banded ions with magnetic storms, their broad latitudinal extent, and the presence of multiple ion species in the same energy band, rather than at the same velocity, indicate that this is a distinct phenomenon from other types of energy-banded ions. During the 21–22 January 2005 magnetic storm, the dayside ion energy band structures, centered at 10 eV (H + ), 40 eV (H + and He + ), and 160 eV (H + , He + , and O + ), were consistent with a “time-of-flight and velocity filter” formation process acting on a near-cusp, impulsive outflow of a <200 eV multi-species ion-source population, poleward and in the same hemisphere as FAST. Understanding the sources and dynamics of warm energy-banded ions and their linkage to the warm plasma cloak is important because during superstorms these ions are transported to L values as low as L ∼ 1.2 in the dawn sector, significantly altering the energetics of the mid-latitude ionosphere.

58 GEOSCIENCES↗
DOE OSTI2020

In situ synchrotron pair distribution function analysis to monitor synthetic pathways under electromagnetic excitation

Electromagnetic (EM) fields, specifically microwave radiation (MWR), can significantly influence the synthesis of ceramic oxide materials and promote rapid, low-temperature growth. However, the mechanisms by which EM fields affect the phase formation process are not well understood. A major limitation to increasing this understanding has been the lack of information regarding dynamic changes in local atomic structure during MWR exposure compared to conventional hydrothermal synthesis routes. Here, we utilize in situ synchrotron X-ray pair distribution function (PDF) analysis to monitor MWR-assisted SnO 2 nanoparticle synthesis. A clear impact of the EM field is demonstrated, with MWR inducing changes in nearest neighbor distances and peaks in oxygen atomic displacement that do not occur during synthesis without MWR exposure. The observed local structural disorder serves as a precursor to rapid rutile SnO 2 nanoparticle crystallization, suggesting that EM field-assisted growth is mediated by changes to the oxygen sublattice. These findings further our understanding of the mechanisms underlying MWR-assisted synthesis and represent a step towards utilizing EM fields to engineer tailored atomic structures for a broad range of applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Insights into the copolymerization of metal–organic nanotubes from ligand mixtures using small angle neutron scattering

Metal–organic nanotubes (MONTs) are porous, tunable 1D nanomaterials akin to metal–organic frameworks (MOFs). MONTs are synthesized via metal salts and coordinating ligands akin to MOFs, but crucially they are anisotropic, unlike most MOFs. Recently, MONTs have been shown to form statistically random copolymers; however, their mechanism of growth remains largely unexplored. Full realization of the potential of MONTs necessitates a thorough understanding of the mechanism of MONT growth. Herein, small-angle neutron scattering (SANS) was employed to investigate the copolymerization mechanism of two 1,2,4-ditriazole ligands and to quantify the inclusion of a solvent within the MONT pores. The results show parallelepiped-shaped structures are initially formed, which then aggregate to form larger lamellar structures. Additional experimentation with a deuterated ligand showed that the reactivities of all ligands are approximately equal, causing random ligand distribution within the resulting MONT. Finally, the results quantify the amount of solvent incorporated within the nanostructure pores at different stages of the formation process. These results show that early in the reaction the MONTs contain ca. 45% solvent, and they contain ca. 55% solvent late in the reaction when the MONTs are nearly fully formed.

Haque, Md Ashraful [Univ. of Tennessee, Knoxville,↗
DOE OSTI2020

Chapter 12: Photoelectron Spectroscopy Methods in Solar Cell Research

Photoelectron spectroscopy (PES), also referred to as photoemission spectroscopy, is a direct experimental method for assessing the chemical and electronic properties of materials. The technique is becoming increasingly important in the research of photovoltaic (PV) devices--where, more specifically, X-ray photoelectron spectroscopy (XPS) is used primarily to measure the chemical properties such as composition and contamination of solar cell materials, whereas ultraviolet photoelectron spectroscopy (UPS) reveals key electronic properties such as work function and electronic energy-level positions. PES is a surface-sensitive technique ideally suited for the analysis of thin films and interfaces, either completed ones or during their formation process. Because the new generation of PV devices comprise a multitude of complex interfaces--each of which plays a critical role for performance and functionality--PES analysis of functional cell components has gained even more relevance.

photoelectron spectroscopy↗
DOE OSTI2020

Surface and grain boundary carbon heterogeneity in CH 3 NH 3 PbI 3 perovskites and its impact on optoelectronic properties

Rivaling state-of-the-art crystalline silicon, organic-inorganic hybrid perovskites have been intensely studied in recent years. Surface and interfacial engineering have been a focus for performance improvement. Even though significant progress has been made during the last decade in terms of the diversity and capability of perovskite-based devices, the structure-property relationship, particularly at the surface, which governs the real-world performance of these applications, is still unresolved. In the article, this issue was addressed by employing synchrotron-related experimental measurements, and a mechanism that correlates microstructure with surface chemistry was resolved. As a powerful and highly sensitive spectromicroscopy, soft x ray photoemission electron microscopy (X-PEEM) was used to probe the surface of perovskite films varying in post solvent annealing. Furthermore, static and in situ grazing incidence hard x ray diffraction (GIXD) was used to track the grain growth dynamics during the film formation process. It was found that the nature of the surfaces was dictated by the local chemistry that varied due to mass flow during the development of the microstructure. Combining optical and electronic characterizations, it was confirmed that a more homogenous chemistry, i.e., uniform chemical components and properties, along with reduced strain and grain boundary energies, yielded more defect-tolerant films. Grain boundaries were more favorable for screening carriers than those in the control film. Our findings underscore the importance of the uniformity in the surface for developing a chemistry-structure-property relationship in perovskite materials, as well as engineering local chemistry toward high-performance and stable devices.

42 ENGINEERING↗
DOE OSTI2021

Fusion gain from cylindrical liner-driven implosions of field reversed configurations

MagLIF experiments [M.R. Gomez et al., Phys. Plasmas 22, 056306 (2015)] on Z have demonstrated the basic principles of Magneto-Inertial Fusion (MIF) for wall confined plasmas. Other MIF schemes have been proposed based on the liner implosion of closed field magnetically confined plasmas such as Field Reversed Configurations (FRCs) [T. P. Intrator et al., Phys. Plasmas 15, 042505 (2008)]. We present a semi-analytical model of liner driven FRC implosions that predicts the fusion gain of such systems. The model predicts a fusion gain near unity for an FRC imploded by a liner driven by the Z Machine. We show that FRCs could be formed and imploded at the Z facility using the AutoMag liner concept [S. A. Slutz et al., Phys. Plasmas 24, 012704 (2017)]. Furthermore, an initial bias magnetic field can be supplied by the external magnets used in MagLIF experiments. The reverse field is then supplied by an AutoMag liner, which has helical conducting paths imbedded in an insulating substance. Experiments [Shipley et al., Phys. Plasmas 26, 052705 (2019)] have demonstrated that AutoMag can generate magnetic fields greater than 30 Tesla inside of the liner. We have performed 2D Radiation MHD simulations of the formation and implosion of an FRC, which are in good agreement with the analytical model. The FRC formation process could be studied on small pulsed power machines delivering about 1 MA.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Probing the ultrafast gain and refractive index dynamics of a VECSEL

Typically, strong gain saturation and gain dynamics play a crucial role in semiconductor laser mode-locking. While there have been several investigations of the ultrafast gain dynamics in vertical-external-cavity surface-emitting lasers (VECSELs), little is known about the associated refractive index changes. Yet, such refractive index changes do not only have a profound impact on the pulse formation process leading to self-phase modulation, which needs to be compensated by dispersion, but they are also of particular relevance for assessing the feasibility of Kerr-lens mode-locking of VECSELs. Here, we measure both refractive index as well as gain dynamics of a VECSEL chip using the ultrafast beam deflection method. We find that, in contrast to the gain dynamics, the refractive index dynamics is dominated by an instantaneous (100 fs) and a very slow component (100 ps). The time-resolved measurement of nonlinear refraction allows us to predict a pulse-length dependent, effective nonlinear refractive index n 2,eff , which is shown to be negative and on the order of 10 -16 m 2 =W for short pulse lengths (100 fs). It becomes positive for large excitation fluences and large pulse lengths (few ps). These results agree with some previous reports of self-mode-locked VECSELs for which the cavity design and pulse properties determine sign and strength of the nonlinear refractive index when assuming Kerr-lens mode-locking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Viscous effects on plasmoid formation from nonlinear resistive tearing growth in a Harris sheet

Abstract In this work, the evolution of a highly unstable m = 1 resistive tearing mode, leading to plasmoid formation in a Harris sheet, is studied in the framework of full MHD model using the Non-Ideal Magnetohydrodynamics with Rotation, Open Discussion simulation. Following the initial nonlinear growth of the primary m = 1 island, the X-point develops into a secondary elongated current sheet that eventually breaks into plasmoids. Two distinctive viscous regimes are found for the plasmoid formation and saturation. In the low viscosity regime (i.e. P r ≲ 1), the plasmoid width increases sharply with viscosity, whereas in the viscosity dominant regime (i.e. P r ≳ 1), the plasmoid size gradually decreases with viscosity. Such a finding quantifies the role of viscosity in modulating the plasmoid formation process through its effects on the plasma flow and the reconnection itself.

Physics↗
DOE OSTI2020

Progenitor, precursor, and evolution of the dusty remnant of the stellar merger M31-LRN-2015

ABSTRACT M31-LRN-2015 is a likely stellar merger discovered in the Andromeda Galaxy in 2015. We present new optical to mid-infrared photometry and optical spectroscopy for this event. Archival data show that the source started to brighten ∼2 yr before the nova event. During this precursor phase, the source brightened by ∼3 mag. The light curve at 6 and 1.5 months before the main outburst may show periodicity, with periods of 16 ± 0.3 and 28.1 ± 1.4 d, respectively. This complex emission may be explained by runaway mass-loss from the system after the binary undergoes Roche lobe overflow, leading the system to coalesce in tens of orbital periods. While the progenitor spectral energy distribution shows no evidence of pre-existing warm dust in the system, the remnant forms an optically thick dust shell at approximately four months after the outburst peak. The optical depth of the shell increases dramatically after 1.5 yr, suggesting the existence of shocks that enhance the dust formation process. We propose that the merger remnant is likely an inflated giant obscured by a cooling shell of gas with mass ∼0.2 M⊙ ejected at the onset of the common envelope phase.

(ISM:) dust, extinction↗
DOE OSTI2021

Pisces VII: discovery of a possible satellite of Messier 33 in the DESI legacy imaging surveys

ABSTRACT We report deep imaging observations with DOLoRes@TNG of an ultra-faint dwarf satellite candidate of the Triangulum galaxy (M33) found by visual inspection of the public imaging data release of the DESI Legacy Imaging Surveys. Pisces VII/Triangulum (Tri) III is found at a projected distance of $72\, {\rm kpc}$ from M33, and using the tip of the red giant branch method, we estimate a distance of $D=1.0^{+0.3}_{-0.2}\, {\rm Mpc}$, meaning the galaxy could either be an isolated ultra-faint or the second known satellite of M33. We estimate an absolute magnitude of MV = −6.1 ± 0.2 if Pisces VII/Tri II is at the distance of M33, or as bright as MV = −6.8 ± 0.2 if the galaxy is isolated. At the isolated distance, it has a physical half-light radius of $r_{\rm h}=131\pm 61\, {\rm pc}$ consistent with similarly faint galaxies around the Milky Way. As the tip of the red giant branch is sparsely populated, constraining a precision distance is not possible, but if Pisces VII/Tri III can be confirmed as a true satellite of M33, it is a significant finding. With only one potential satellite detected around M33 previously (Andromeda XXII/Tri I), it lacks a significant satellite population in stark contrast to the similarly massive Large Magellanic Cloud. The detection of more satellites in the outskirts of M33 could help to better illuminate if this discrepancy between expectation and observations is due to a poor understanding of the galaxy formation process, or if it is due to the low luminosity and surface brightness of the M33 satellite population which has thus far fallen below the detection limits of previous surveys. If it is truly isolated, it would be the faintest known field dwarf detected to date.

Martínez-Delgado, David↗
DOE OSTI2021

Investigation of Rocket Effect in BRC 18 using Gaia EDR3

ABSTRACT Bright-rimmed clouds (BRCs) are ideal candidates to study radiation-driven implosion mode of star formation as they are potential sites of triggered star formation, located at the edges of Hii regions, showing evidence of ongoing star formation processes. BRC 18 is located towards the eastern edge of relatively closer (∼400 pc) H ii region excited by λ Ori. We made R-band polarimetric observations of 17 candidate young stellar objects (YSOs) located towards BRC 18 to investigate any preferred orientation of the discs with respect to the ambient magnetic field and the direction of energetic photons from λ Ori. We found that the discs are oriented randomly with respect to the projected magnetic field. Using distances and proper motions from the Gaia EDR3 of the candidate YSOs, we investigated the possible acceleration of BRC 18, away from λ Ori due to the well-known ‘Rocket Effect’, by assuming that both the candidate YSOs and BRC 18 are kinematically coupled. The relative proper motions of the candidate YSOs are found to show a trend of moving away from λ Ori. We computed the offset between the angle of the direction of the ionization front and the relative proper motion of the candidate YSOs and found it to lie close to being parallel to each other. Additionally, we found 12 sources that are co-moving with the known candidate YSOs towards BRC 18. These co-moving sources are most likely to be young and are missed in previous surveys conducted to identify potential YSOs of the region.

Saha, Piyali (ORCID:0000000200281354)↗