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At least 55 records · Page 3

Th IV –Desferrioxamine: characterization of a fluorescent bacterial probe

Diversifying our ability to guard against emerging pathogenic threats is essential for keeping pace with global health challenges, including those presented by drug-resistant bacteria. Some modern diagnostic and therapeutic innovations to address this challenge focus on targeting methods that exploit bacterial nutrient sequestration pathways, such as the desferrioxamine (DFO) siderophore used by Staphylococcus aureus (S. aureus) to sequester Fe III . Building on recent studies that have shown DFO to be a versatile vehicle for chemical delivery, we show proof-of-principle that the Fe III sequestration pathway can be used to deliver a potential radiotherapeutic. Our approach replaces the FeIII nutrient sequestered by H 4 DFO + with Th IV and made use of a common fluorophore, FITC, which we covalently bonded to DFO to provide a combinatorial probe for simultaneous chelation paired with imaging and spectroscopy, H 3 DFO_FITC. Combining insight provided from FITC-based imaging with characterization by NMR spectroscopy, we demonstrated that the fluorescent DFO_FITC conjugate retained the Th IV chelation properties of native H4DFO+. Fluorescence microscopy with both [Th(DFO_FITC)] and [Fe(DFO_FITC)] complexes showed similar uptake by S. aureus and increased intercellular accumulation as compared to the FITC and unchelated H 3 DFO_FITC controls. Collectively, these results demonstrate the potential for the newly developed H 3 DFO_FITC conjugate to be used as a targeting vector and bacterial imaging probe for S. aureus. The results presented within provide a framework to expand H 4 DFO + and H 3 DFO_FITC to relevant radiotherapeutics (like 227Th).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamic Nuclear Polarization Enhanced Nuclear Spin Optical Rotation

Here, nuclear spin optical rotation (NSOR) has been investigated as a magneto-optical effect, which holds the potential for applications, including hybrid optical-nuclear magnetic resonance (NMR) spectroscopy and gradientless imaging. The intrinsic nature of NSOR renders its detection relatively insensitive, which has prevented it moving from a proof of concept to a method supporting chemical characterizations. In this work, the dissolution dynamic nuclear polarization technique is introduced to provide nuclear spin polarization, increasing the signal-to-noise ratio by several thousand times. NSOR signals of 1 H and 19 F nuclei are observed in a single scan for diluted compounds, which has made this effect suitable for the determination of electronic transitions from a specific nucleus in a large molecule.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Elucidating Drought-Tolerance Mechanisms in Plant Roots through 1H NMR Metabolomics in Parallel with MALDI-MS, and NanoSIMS Imaging Techniques

As direct mediators between plants and soil, roots play an important role in metabolic responses to environmental stresses such as drought, yet these responses are vastly uncharacterized on a plant-specific level, especially for co-occurring species. Here, we aim to examine the effects of drought on root metabolic profiles and carbon allocation pathways of three tropical rainforest species by combining cutting-edge metabolomic and imaging technologies in an in situ position-specific 13C-pyruvate root-labeling experiment. Further, washed (rhizosphere-depleted) and unwashed roots were examined to test the impact of microbial presence on root metabolic pathways. Drought had a species-specific impact on the metabolic profiles and spatial distribution in Piper sp. and Hibiscus rosa sinensis roots, signifying different defense mechanisms; Piper sp. enhanced root structural defense via recalcitrant compounds including lignin, while H. rosa sinensis enhanced biochemical defense via secretion of antioxidants and fatty acids. In contrast, Clitoria fairchildiana, a legume tree, was not influenced as much by drought but rather by rhizosphere presence where carbohydrate storage was enhanced, indicating a close association with symbiotic microbes. This study demonstrates how multiple techniques can be combined to identify how plants cope with drought through different drought-tolerance strategies and the consequences of such changes on below-ground organic matter composition.

Drought, Carbon cycle, MALDI-MSI, Metabolomics, Na↗

Conceptual design of HTS magnets for fusion nuclear science facility

Second-generation high temperature superconductors (HTS) are available for producing >20 T at the magnet bore compared to 13–16 T for lower temperature superconducting (LTS) toroidal field magnets proposed in recent fusion energy systems studies (FESS) of Fusion Nuclear Science Facility (FNSF). HTS may enable higher fusion power density and smaller device size. High current density cables of multi-layered REBCO tapes have achieved >10 kA at 4–20 K operation in short sample tests for fusion. High current density cables are required for engineering design of FNSF to allow space for interior plasma components. High current density HTS magnets are particularly attractive in reducing the size of a fusion device, beneficial for compact tokamaks, due to their space constraints. Successful HTS magnet development may enable the design of smaller and cheaper fusion pilot plants with a mission of demonstrating net electricity. It may also offer significant cost and performance advantages in non-fusion applicants such as nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI). Furthermore, we developed HTS magnet design concepts for a compact FNSF radial build in order to define the coil size, winding pack mechanical loading and engineering requirements. Partnering with vendors in the US, PPPL is also testing high current cable prototypes aiming at enabling low cost cable technology toward 100 A/mm 2 engineering current density over the winding pack desired in high field model coil development for compact fusion pilot plants.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Making Superconducting Welds between Superconducting Wires

A technique for making superconducting joints between wires made of dissimilar superconducting metals has been devised. The technique is especially suitable for fabrication of superconducting circuits needed to support persistent electric currents in electromagnets in diverse cryogenic applications. Examples of such electromagnets include those in nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) systems and in superconducting quantum interference devices (SQUIDs). Sometimes, it is desirable to fabricate different parts of a persistent-current-supporting superconducting loop from different metals. For example, a sensory coil in a SQUID might be made of Pb, a Pb/Sn alloy, or a Cu wire plated with Pb/Sn, while the connections to the sensory coil might be made via Nb or Nb/Ti wires. Conventional wire-bonding techniques, including resistance spot welding and pressed contact, are not workable because of large differences between the hardnesses and melting temperatures of the different metals. The present technique is not subject to this limitation. The present technique involves the use (1) of a cheap, miniature, easy-to-operate, capacitor-discharging welding apparatus that has an Nb or Nb/Ti tip and operates with a continuous local flow of gaseous helium and (2) preparation of a joint in a special spark-discharge welding geometry. In a typical application, a piece of Nb foil about 25 m thick is rolled to form a tube, into which is inserted a wire that one seeks to weld to the tube (see figure). The tube can be slightly crimped for mechanical stability. Then a spark weld is made by use of the aforementioned apparatus with energy and time settings chosen to melt a small section of the niobium foil. The energy setting corresponds to the setting of a voltage to which the capacitor is charged. In an experiment, the technique was used to weld an Nb foil to a copper wire coated with a Pb/Sn soft solder, which is superconducting. The joint was evaluated as part of a persistent-current circuit having an inductance of 1 mH. A current was induced in a loop, and no attenuation of the current after a time interval 1,000 s was discernible in a measurement having a fractional accuracy of 10(exp -4): This observation supports the conclusion that the weld had an electrical resistance <10(exp -10) omega.

Penanen, Konstantin I.↗

Gradient-based surface nuclear magnetic resonance for groundwater investigation

In medical magnetic resonance imaging, spatial localization (imaging) is based upon the application of controlled magnetic field gradients on top of the main magnetic field to spatially modulate the frequency and/or phase of the nuclear magnetic resonance (NMR) signal across the volume of investigation. In this work, we have applied similar physical principles to produce controlled magnetic field gradients during surface NMR-based groundwater investigations. In this approach, a gradient pulse of variable amplitude or duration is applied immediately after the excitation pulse to cause predictable phase encoding of the NMR signal as a function of depth. This approach is also applicable to emerging surface NMR detection methods that use a prepolarization field with fast nonadiabatic turn-off to generate detectable NMR signals from the shallow subsurface. In this case, the gradient pulse is applied after terminating the prepolarization field and provides a heretofore unavailable means of localizing the NMR response as a function of depth. The application of gradients can also be combined with tip-angle-based modulation to yield higher imaging resolution than can be achieved through either gradient- or tip-angle-based imaging alone. We implemented this new gradient-based capability into a surface NMR gradient generation accessory that is compatible with the GMR-Flex instrument and developed surface NMR-specific forward modeling and linear inverse models. We validated the accuracy of this novel gradient-based sNMR technology using computer simulations, experiments using a small pool filled with a discrete layer of bulk water, and field experiments at well-characterized groundwater test sites along Ebey Island, WA, and Larned, KS. The gradient-based sNMR imaging observations were compared with high-resolution direct push NMR results observed at these sites. The results of computer simulations and field experiments indicate improvements in both the detection (signal-to-noise ratio) and spatial resolution of shallow subsurface water content using gradient-based surface NMR, compared with traditional surface NMR imaging methods.

Geochemistry & Geophysics↗

Twin Boundaries Contribute to The First Cycle Irreversibility of LiNiO 2

Abstract LiNiO 2 remains a target for layered oxide Li‐ion cathode development as it can theoretically deliver the highest energy density of this materials class. In practice, LiNiO 2 suffers from poor capacity retention due to electrochemically‐induced structural changes. While the impact of Ni off‐stoichiometry on the electrochemical performance has been extensively studied, that of planar defects present in the as‐synthesized cathode is not well understood. Advanced ex situ and operando structure probes are used to identify and quantify point and planar defects present in as‐synthesized Li 1‐y Ni 1+y O 2 cathodes and monitor their evolution during the first cycle. Specifically, a 7 Li nuclear magnetic resonance (NMR) signature characteristic of Li environments near twin boundaries is identified; an assignment supported by first‐principles calculations and scanning transmission electron microscopy (STEM) images of twin boundary defects. The NMR results suggest that the concentration of twin boundaries depends on the amount of Ni excess. Moreover, operando magnetometry and ex situ synchrotron X‐ray diffraction and NMR demonstrate that these planar defects impede Li reinsertion into the bulk cathode at reasonable discharge rates and contribute to the first cycle irreversible capacity. These findings provide new design rules for Li 1‐y Ni 1+y O 2 cathodes, whereby a reduced concentration of twin boundaries in the pristine material leads to reduced kinetic limitations and improved cathode utilization.

Nguyen, H.↗

Toward Ultra‐High‐Quality‐Factor Wireless Masing Magnetic Resonance Sensing

It has recently been shown that a bolus of hyperpolarized nuclear spins can yield stimulated emission signals similar in nature to maser signals, potentially enabling new ways of sensing hyperpolarized contrast media, including most notably [1- 13 C]pyruvate that is under evaluation in over 50 clinical trials for metabolic imaging of cancer. The stimulated NMR signal emissions lasting for minutes do not require radio-frequency excitation, offering unprecedented advantages compared to conventional MR sensing. However, creating nuclear spin maser emission is challenging in practice due to stringent fundamental requirements, making practical in vivo applications hardly possible using conventional passive MR detectors. Here, in this study, we demonstrate the utility of a wireless NMR maser detector, the quality factor of which was enhanced 22-fold (to 1,670) via parametric pumping. This active-feedback technique breaks the intrinsic fundamental limit of NMR detector circuit quality factor. We show the use of parametric pumping to reduce the threshold requirement for inducing nuclear spin masing at 300 MHz resonance frequency in a preclinical MRI scanner. Indeed, stimulated emission from hyperpolarized protons was obtained under highly unfavorable conditions of low magnetic field homogeneity (T 2 * of 3 ms). Greater gains of the quality factor of the MR detector (up to 1 million) were also demonstrated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Biomedical Investigations with Laser-Polarized Noble Gas Magnetic Resonance

We are developing laser-polarized noble gas nuclear magnetic resonance (NMR) as a novel biomedical imaging tool for ground-based and eventually space-based application. This emerging multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI) (e.g., of lung ventilation) as well as studies of tissue perfusion. In addition, laser-polarized noble gases (He-3 and Xe-129) do not require a large magnetic field for sensitive detection, opening the door to practical MRI at very low magnetic fields with an open, lightweight, and low-power device. We are pursuing two specific aims in this research. The first aim is to develop a low-field (< 0.01 T) instrument for noble gas MRI of humans, and the second aim is to develop functional MRI of the lung using laser-polarized Xe-129 and related techniques.

Walsworth, Ronald L.↗

Biomedical Investigations with Laser-Polarized Noble Gas Magnetic Resonance

We pursued advanced technology development of laser-polarized noble gas nuclear magnetic resonance (NMR) as a novel biomedical imaging tool for ground-based and eventually space-based application. This new multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI)-e.g., of lung ventilation-as well as studies of tissue perfusion. In addition, laser-polarized noble gases (3He and 129Xe) do not require a large magnetic field for sensitive detection, opening the door to practical MRI at very low magnetic fields with an open, lightweight, and low-power device. We pursued two technology development specific aims: (1) development of low-field (less than 0.01 T) noble gas MRI of humans; and (2) development of functional MRI of the lung using laser-polarized noble gas and related techniques.

Walsworth, Ronald L.↗

Development of Laser-Polarized Noble Gas Magnetic Resonance Imaging (MRI) Technology

We are developing technology for laser-polarized noble gas nuclear magnetic resonance (NMR), with the aim of enabling it as a novel biomedical imaging tool for ground-based and eventually space-based application. This emerging multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI)-e.g., of lung ventilation, perfusion, and gas-exchange. In addition, laser-polarized noble gases (3He and 1BXe) do not require a large magnetic field for sensitive NMR detection, opening the door to practical MRI with novel, open-access magnet designs at very low magnetic fields (and hence in confined spaces). We are pursuing two specific aims in this technology development program. The first aim is to develop an open-access, low-field (less than 0.01 T) instrument for MRI studies of human gas inhalation as a function of subject orientation, and the second aim is to develop functional imaging of the lung using laser-polarized He-3 and Xe-129.

Walsworth, Ronald L.↗

New Window into the Human Body

Michael Vannier, MD, a former NASA engineer, recognized the similarity between NASA's computerized image processing technology and nuclear magnetic resonance. With technical assistance from Kennedy Space Center, he developed a computer program for Mallinckrodt Institute of Radiology enabling Nuclear Magnetic Resonance (NMR) to scan body tissue for earlier diagnoses. Dr. Vannier feels that "satellite imaging" has opened a new window into the human body.

Source record↗

The superior hydrothermal stability of Pd/SSZ-39 in low temperature passive NOx adsorption (PNA) and methane combustion

We successfully synthesized uniform SSZ-39 with an average crystal size of about a micron. Pd (0.7 - 3 wt%) was supported on SSZ-39 with Si/Al ratio ~12. The as-synthesized materials were characterized by FTIR, XRD, Helium Ion Microscopy, HAADF-STEM imaging, 27 Al, 29 Si and H solid state NMR spectroscopic techniques. FTIR studies with CO and NO probe molecules reveal that the 0.7 wt% Pd/SSZ-39 material with Si/Al ~12 has the majority of Pd dispersed atomically as isolated Pd(II) and Pd(II)-OH centers, and thus can be used as a low-temperature passive NOx adsorber. Pd(II)-NO, Pd(II)(OH)(NO) and Pd(II)(CO)(NO) complexes form during PNA in this material. We compare this PNA material directly with the Pd/SSZ-13 system (with Si/Al ratio ~12) and show its superior hydrothermal stability. Remarkably, Pd/SSZ-39 with Si/Al ratio ~12 survives hydrothermal aging up to 815 ºC in 10% H 2 O/Air vapor for 16 hours without significant loss in activity. The SSZ-39 crystal structure remains intact during hydrothermal aging up to 1,000 ºC as we elucidate it with XRD and HAADF-STEM imaging/EDS mapping. However, changes to the framework during such harsh hydrothermal treatment significantly change the NOx release profiles during PNA as evidenced by high-field 27 Al NMR on fresh and aged Pd/SSZ-39 samples as well as PNA performance measurements. Besides PNA application, these hydrothermally very stable materials (3 wt% Pd on SSZ-39 with Si/Al ratio ~12) can be used as a robust methane combustion catalyst under industrially relevant conditions (GHSV~600,000hr -1 ). This catalyst shows minimal deactivation after both harsh hydrothermal aging at 750 and 800 ºC, and prolonged time on stream (105 hrs) at 425 °C. In contrast, both 3wt% Pd/alumina and 3wt% SSZ-13 supported samples lose a significant portion of their activity. Our study opens new avenues to prepare the most hydrothermally stable known Pd/zeolite materials with applications for adsorption and catalytic hydrocarbon combustion under industrially relevant conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamic Nuclear Polarization Enhanced 113 Cd Solid-State Nuclear Magnetic Resonance Spectroscopy Reveals CdSe Nanocrystals with Triangular Two-Dimensional Projections are Terminated by {100} Facets

Surface structure plays an important role in particle growth and determining the chemical and photophysical properties of semiconductor nanocrystals (NCs). Therefore, there is a need for structural tools that can characterize and detect different surface facets. Here, we sought to investigate the structure of {111} CdSe facets by applying dynamic nuclear polarization (DNP) enhanced 113 Cd and 77 Se solid-state nuclear magnetic resonance (SSNMR) spectroscopy to zinc-blende CdSe NCs that exhibit triangular two-dimensional (2D) projections within transmission electron microscope (TEM) images. It was originally hypothesized in the literature that these CdSe NCs were tetrahedral in shape and terminated by facets from the {111} family of lattice planes of the zinc-blende structure. Surprisingly, we observe 113 Cd NMR spectra indicating that the primary facets are from the {100} family of lattice planes. We also obtained DNP-enhanced 113 Cd and 77 Se SSNMR spectra of recently reported right trigonal bipyramidal (rTriBP) CdSe NCs grown by seeded growth. The 113 Cd NMR spectra rTriBP CdSe NCs are consistent with {100} surface facets. TEM images show that rTriBP NCs may also exhibit triangular 2D projections that are similar to the so-called tetrahedral NCs. Based upon these results, we conclude that the so-called tetrahedral NCs are predominantly terminated by {100} surface facets and most likely have the same shape as rTriBP NCs. These results highlight the need for multiple complementary techniques when assigning the shape and surface termination of NCs.

Santhiran, Anuluxan [Ames Laboratory (AMES), Ames,↗

Low field SQUID MRI devices, components and methods

Low field SQUID MRI devices, components and methods are disclosed. They include a portable low field (SQUID)-based MRI instrument and a portable low field SQUID-based MRI system to be operated under a bed where a subject is adapted to be located. Also disclosed is a method of distributing wires on an image encoding coil system adapted to be used with an NMR or MRI device for analyzing a sample or subject and a second order superconducting gradiometer adapted to be used with a low field SQUID-based MRI device as a sensing component for an MRI signal related to a subject or sample.

Penanen, Konstantin I.↗

Low field SQUID MRI devices, components and methods

Low field SQUID MRI devices, components and methods are disclosed. They include a portable low field (SQUID)-based MRI instrument and a portable low field SQUID-based MRI system to be operated under a bed where a subject is adapted to be located. Also disclosed is a method of distributing wires on an image encoding coil system adapted to be used with an NMR or MRI device for analyzing a sample or subject and a second order superconducting gradiometer adapted to be used with a low field SQUID-based MRI device as a sensing component for an MRI signal related to a subject or sample.

Penanen, Konstantin I.↗

Low Field Squid MRI Devices, Components and Methods

Low field SQUID MRI devices, components and methods are disclosed. They include a portable low field (SQUID)-based MRI instrument and a portable low field SQUID-based MRI system to be operated under a bed where a subject is adapted to be located. Also disclosed is a method of distributing wires on an image encoding coil system adapted to be used with an NMR or MRI device for analyzing a sample or subject and a second order superconducting gradiometer adapted to be used with a low field SQUID-based MRI device as a sensing component for an MRI signal related to a subject or sample.

Penanen, Konstantin I.↗

Low Field Squid MRI Devices, Components and Methods

Low field SQUID MRI devices, components and methods are disclosed. They include a portable low field (SQUID)-based MRI instrument and a portable low field SQUID-based MRI system to be operated under a bed where a subject is adapted to be located. Also disclosed is a method of distributing wires on an image encoding coil system adapted to be used with an NMR or MRI device for analyzing a sample or subject and a second order superconducting gradiometer adapted to be used with a low field SQUID-based MRI device as a sensing component for an MRI signal related to a subject or sample.

Penanen, Konstantin I.↗