Publications by authors named "Nicholas Whiting"

The para spin isomer of hydrogen gas possesses high nuclear spin order that can enhance the NMR signals of a variety of molecular species. Hydrogen is routinely enriched in the para spin state by lowering the gas temperature while flowing through a catalyst. Although parahydrogen enrichments approaching 100% are achievable near the H liquefaction temperature of 20 K, many experimentalists operate at liquid nitrogen temperatures (77 K) due to the lower associated costs and overall simplicity of the parahydrogen generator.

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The application of parahydrogen gas to enhance the magnetic resonance signals of a diversity of chemical species has increased substantially in the last decade. Parahydrogen is prepared by lowering the temperature of hydrogen gas in the presence of a catalyst; this enriches the para spin isomer beyond its normal abundance of 25% at thermal equilibrium. Indeed, parahydrogen fractions that approach unity can be attained at sufficiently low temperatures.

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With an increase in the severity of environmental pollution caused by microbeads, the development of biodegradable microcapsules that can be applied in diverse fields has attracted significant attention. The degradation processes are directly related to biodegradable microcapsule creation with high stability and persistence. In this study, biodegradable microcapsules are synthesized via a complex coacervation approach using gelatin and alginate as the capsule main wall materials; additionally, enzyme-induced decomposition mechanisms are proposed by observing spectral changes in proton nuclear magnetic resonance (H NMR) analyses.

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Si silica nanoparticles (SiO NPs) are promising magnetic resonance imaging (MRI) probes that possess advantageous properties for in vivo applications, including suitable biocompatibility, tailorable properties, and high water dispersibility. Dynamic nuclear polarization (DNP) is used to enhance Si MR signals via enhanced nuclear spin alignment; to date, there has been limited success employing DNP for SiO NPs due to the lack of endogenous electronic defects that are required for the process. To create opportunities for SiO-based Si MRI probes, we synthesized variously featured SiO NPs with selective Si isotope enrichment on homogeneous and core@shell structures (shell thickness: 10 nm, core size: 40 nm), and identified the critical factors for optimal DNP signal enhancement as well as the effective hyperpolarization depth when using an exogenous radical.

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The embedding of radicals at different locations within core@shell silica nanoparticles contributes to enhanced polarization capability and can be self-polarized without adding external radicals. With grafting the radical source homogenously inside of the nanoparticles, a significant Si hyperpolarization signal enhancement of 49.4 was obtained.

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The isomeric enrichment of parahydrogen (pH) gas is readily accomplished by lowering the gas temperature in the presence of a catalyst. This enrichment is often pursued at two distinct temperatures: ∼51% pH is generated at liquid nitrogen temperatures (77 K), while nearly 100% pH can be produced at 20 K. While the liquid nitrogen cooled generator is attractive due to the low cost of entry, there are benefits to having access to greater than 51% pH for enhanced NMR applications.

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Medical imaging devices often use automated processing that creates and displays a self-normalized image. When improperly executed, normalization can misrepresent information or result in an inaccurate analysis. In the case of diagnostic imaging, a false positive in the absence of disease, or a negative finding when disease is present, can produce a detrimental experience for the patient and diminish their health prospects and prognosis.

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Silicon particles have garnered attention as promising biomedical probes for hyperpolarized Si magnetic resonance imaging and spectroscopy. However, due to the limited levels of hyperpolarization for nanosized silicon particles, microscale silicon particles have primarily been the focus of dynamic nuclear polarization (DNP) applications, including magnetic resonance imaging (MRI). To address these current challenges, we developed a facile synthetic method for partially Si-enriched porous silicon nanoparticles (NPs) (160 nm) and examined their usability in hyperpolarized Si MRI agents with enhanced signals in spectroscopy and imaging.

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Spin-exchange optical pumping (SEOP) can enhance the NMR sensitivity of noble gases by up to five orders of magnitude at Tesla-strength magnetic fields. SEOP-generated hyperpolarised (HP) Xe is a promising contrast agent for lung imaging but an ongoing barrier to widespread clinical usage has been economical production of sufficient quantities with high Xe polarisation. Here, the 'standard model' of SEOP, which was previously used in the optimisation of continuous-flow Xe polarisers, is modified for validation against two Xe-rich stopped-flow SEOP datasets.

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Porous silicon nanoparticles have recently garnered attention as potentially-promising biomedical platforms for drug delivery and medical diagnostics. Here, we demonstrate porous silicon nanoparticles as contrast agents for Si magnetic resonance imaging. Size-controlled porous silicon nanoparticles were synthesized by magnesiothermic reduction of silica nanoparticles and were surface activated for further functionalization.

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This article reviews existing and emerging techniques of interrogating metabolism in brain cancer from well-established proton magnetic resonance spectroscopy to the promising hyperpolarized metabolic imaging and chemical exchange saturation transfer and emerging techniques of imaging inflammation. Some of these techniques are at an early stage of development and clinical trials are in progress in patients to establish the clinical efficacy. It is likely that in vivo metabolomics and metabolic imaging is the next frontier in brain cancer diagnosis and assessing therapeutic efficacy; with the combined knowledge of genomics and proteomics a complete understanding of tumorigenesis in brain might be achieved.

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Silicon-based nanoparticles are ideally suited for use as biomedical imaging agents due to their biocompatibility, biodegradability, and simple surface chemistry that facilitates drug loading and targeting. A method of hyperpolarizing silicon particles using dynamic nuclear polarization, which increases magnetic resonance imaging signals by several orders-of-magnitude through enhanced nuclear spin alignment, has recently been developed to allow silicon particles to function as contrast agents for in vivo magnetic resonance imaging. The enhanced spin polarization of silicon lasts significantly longer than other hyperpolarized agents (tens of minutes, whereas [Formula: see text] for other species at room temperature), allowing a wide range of potential applications.

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Visualizing the movement of angiocatheters during endovascular interventions is typically accomplished using x-ray fluoroscopy. There are many potential advantages to developing magnetic resonance imaging-based approaches that will allow three-dimensional imaging of the tissue/vasculature interface while monitoring other physiologically-relevant criteria, without exposing the patient or clinician team to ionizing radiation. Here we introduce a proof-of-concept development of a magnetic resonance imaging-guided catheter tracking method that utilizes hyperpolarized silicon particles.

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Here we provide a full report on the construction, components, and capabilities of our consortium's "open-source" large-scale (~1L/h) (129)Xe hyperpolarizer for clinical, pre-clinical, and materials NMR/MRI (Nikolaou et al., Proc. Natl.

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The exquisite NMR spectral sensitivity and negligible reactivity of hyperpolarized xenon-129 (HP(129)Xe) make it attractive for a number of magnetic resonance applications; moreover, HP(129)Xe embodies an alternative to rare and nonrenewable (3)He. However, the ability to reliably and inexpensively produce large quantities of HP(129)Xe with sufficiently high (129)Xe nuclear spin polarization (P(Xe)) remains a significant challenge--particularly at high Xe densities. We present results from our "open-source" large-scale (∼1 L/h) (129)Xe polarizer for clinical, preclinical, and materials NMR and MRI research.

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The (129)Xe nuclear spin polarization (P(Xe)) that can be achieved via spin-exchange optical pumping (SEOP) is typically limited at high in-cell xenon densities ([Xe](cell)), due primarily to corresponding reductions in the alkali metal electron spin polarization (e.g. P(Rb)) caused by increased non-spin-conserving Rb-Xe collisions.

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Volume holographic gratings (VHGs) can be exploited to narrow the spectral output of high-power laser-diode arrays (LDAs) by nearly an order of magnitude, permitting more efficient generation of laser-polarized noble gases for various applications. A approximately 3-fold improvement in (129)Xe nuclear spin polarization, P(Xe), (compared to a conventional LDA) was achieved with the VHG-LDA's center wavelength tuned to a wing of the Rb D(1) line. Additionally, an anomalous dependence of P(Xe) on the xenon density within the OP cell is reported-including high P(Xe) values (>10%) at high xenon partial pressures (approximately 1000 torr).

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