A5044288224- Advanced NMR Techniques and Applications
- Electron Spin Resonance Studies
- Atomic and Subatomic Physics Research
- Solid-state spectroscopy and crystallography
- Enzyme Structure and Function
- Molecular spectroscopy and chirality
- NMR spectroscopy and applications
- Magnetism in coordination complexes
- Diamond and Carbon-based Materials Research
- Nonlinear Optical Materials Research
- High-pressure geophysics and materials
- Carbon Dioxide Capture Technologies
- Advanced MRI Techniques and Applications
- Innovative Microfluidic and Catalytic Techniques Innovation
- bioluminescence and chemiluminescence research
- Acoustic Wave Resonator Technologies
- Quantum, superfluid, helium dynamics
- Lanthanide and Transition Metal Complexes
- Spectroscopy and Quantum Chemical Studies
- Functional Brain Connectivity Studies
- Ammonia Synthesis and Nitrogen Reduction
- Supramolecular Self-Assembly in Materials
- Process Optimization and Integration
North Carolina State University
2020-2023
Molecular metabolic imaging in humans is dominated by positron emission tomography (PET). An emerging nonionizing alternative hyperpolarized MRI of 13C-pyruvate, which innocuous and has a central role metabolism. However, similar to PET, with dissolution dynamic nuclear polarization (d-DNP) complex costly, requires significant infrastructure. In contrast, Signal Amplification By Reversible Exchange (SABRE) fast, cheap, scalable hyperpolarization technique. SABRE SHield Enables Alignment...
Hyperpolarization chemistry based on reversible exchange of parahydrogen, also known as Signal Amplification By Reversible Exchange (SABRE), is a particularly simple approach to attain high levels nuclear spin hyperpolarization, which can enhance NMR and MRI signals by many orders magnitude. SABRE has received significant attention in the scientific community since its inception because relative experimental simplicity broad applicability wide range molecules, however vivo detection...
Optically-probed nitrogen-vacancy (NV) quantum defects in diamond can detect nuclear magnetic resonance (NMR) signals with high-spectral resolution from micron-scale sample volumes of about 10 picoliters. However, a key challenge for NV-NMR is detecting samples at millimolar concentrations. Here, we demonstrate an improvement proton concentration sensitivity $10^5$ over thermal polarization by hyperpolarizing spins through signal amplification reversible exchange (SABRE), enabling NMR small...
Abstract Signal Amplification By Reversible Exchange in SHield Enabled Alignment Transfer (SABRE‐SHEATH) is investigated to achieve rapid hyperpolarization of 13 C 1 spins [1‐ C]pyruvate, using parahydrogen as the source nuclear spin order. Pyruvate exchange with an iridium polarization transfer complex can be modulated via a sensitive interplay between temperature and co‐ligation DMSO H 2 O. Order‐unity (>50 %) catalyst‐bound C]pyruvate achieved less than 30 s by restricting chemical at...
Despite great successes in oncology, patient outcomes are often still discouraging, and hence the diagnostic imaging paradigm is increasingly shifting toward functional of pathology to better understand individual disease biology personalize therapies. The dissolution Dynamic Nuclear Polarization (d-DNP) hyperpolarization method has enabled unprecedented real-time MRI sensing metabolism tissue pH using hyperpolarized [1-13C]pyruvate as a biosensor with potential for diagnosis monitoring...
We introduce a Spin Transfer Automated Reactor (STAR) that produces continuous parahydrogen induced polarization (PHIP), which is stable for hours to days. use the PHIP variant called signal amplification by reversible exchange (SABRE), particularly well suited produce hyperpolarization. The STAR operated in conjunction with benchtop (1.1 T) and high field (9.4 NMR magnets, highlighting versatility of this system operate any or MRI system. uses semipermeable membranes efficiently deliver...
Hyperpolarized (HP) MRI using [1-13C]pyruvate is emerging as a promising molecular imaging approach. Among hyperpolarization methods, Signal Amplification By Reversible Exchange (SABRE) attractive because SABRE polarizes the substrates directly in room-temperature solutions avoiding complex hardware. Most experiments have historically been performed methanol, relatively toxic and difficult to remove solvent. Here we first demonstrate use of acetone-water-solvent system (Ace-SABRE) provide...
Hyperpolarized (HP) MRI using [1‐13C]pyruvate is emerging as a promising molecular imaging approach. Among hyperpolarization methods, Signal Amplification By Reversible Exchange (SABRE) attractive because SABRE polarizes the substrates directly in room‐temperature solutions avoiding complex hardware. Most experiments have historically been performed methanol, relatively toxic and difficult to remove solvent. Here we demonstrate use of 80/20 acetone‐water‐solvent system (Ace‐SABRE) provide...
Hyperpolarized (HP) MRI using [1‐13C]pyruvate is emerging as a promising molecular imaging approach. Among hyperpolarization methods, Signal Amplification By Reversible Exchange (SABRE) attractive because SABRE polarizes the substrates directly in room‐temperature solutions avoiding complex hardware. Most experiments have historically been performed methanol, relatively toxic and difficult to remove solvent. Here we demonstrate use of 80/20 acetone‐water‐solvent system (Ace‐SABRE) provide...
Hyperpolarized [1-13C]pyruvate is a revolutionary molecular probe enabling ultrafast metabolic MRI scans in 1 min. This technology now under evaluation over 30 clinical trials, which employ dissolution Dynamic Nuclear Polarization (d-DNP) to prepare batch of the contrast agent; however, d-DNP slow and expensive. The emerging SABRE-SHEATH hyperpolarization technique enables fast (under min) robust production hyperpolarized via simultaneous chemical exchange parahydrogen pyruvate on IrIMes...
An intensified continuous flow strategy is developed and utilized for scalable extraction of switchable hydrophilicity solvents triggered by carbon dioxide.
Signal amplification by reversible exchange (SABRE) is a robust and inexpensive hyperpolarization (HP) technique to enhance nuclear magnetic resonance (NMR) spectroscopy imaging (MRI) signals using parahydrogen (pH2 ). The substrate scope of SABRE continually expanding. Here, we present the polarization three antifungal drugs (voriconazole, clotrimazole, fluconazole) elicit detailed HP mechanisms for 1 H 15 N nuclei. In this exploratory work, values ~1% were achieved 50% pH2 in solution 3-mM...
Hyperpolarization chemistry based on reversible exchange of parahydrogen, also known as Signal Amplification By Reversible Exchange (SABRE), is a particularly simple approach to attain high levels nuclear spin hyperpolarization, which can enhance NMR and MRI signals by many orders magnitude. SABRE has received significant attention in the scientific community since its inception because relative experimental simplicity broad applicability wide range molecules, however vivo detection...
Hyperpolarization modalities overcome the sensitivity limitations of NMR and unlock new applications. Signal amplification by reversible exchange (SABRE) is a particularly cheap, quick, robust hyperpolarization modality. Here, we employ SABRE for simultaneous chemical parahydrogen nitrile-containing anticancer drugs (letrozole or anastrozole) to enhance
Abstract An in‐depth theoretical analysis of key chemical equilibria in Signal Amplification by Reversible Exchange (SABRE) is provided, employing density functional theory calculations to characterize the likely reaction network. For all reactions network, potential energy surface probed identify minimum pathways. Energy barriers and transition states are calculated, harmonic state applied calculate exchange rates that approximate experimental values. The network can be modulated potentials...
Hyperpolarization of 13C-pyruvate via Signal Amplificaton By Reversibble Exchange (SABRE) is an important recent discovery because both the relative simplicity hyperpolarization and central biological relevance pyruvate as a biomolecular probe for in vitro or vivo studies. Here, we analyze [1,2-13C2]pyruvate-SABRE spin system its field dependence theoretically experimentally. We provide first-principles analysis governing 4-spin dihydride-13C2 Hamiltonian numerical dynamics simulations...
Signal Amplification by Reversible Exchange (SABRE) is a relatively simple and fast hyperpolarization technique that has been used to hyperpolarize the α‐ketocarboxylate pyruvate, central metabolite leading hyperpolarized MRI contrast agent. In this work, we show SABRE can readily be extended 13C nuclei at natural abundance on many other α‐ketocarboxylates. Hyperpolarization observed optimized pyruvate (P13C=17%) 2‐oxobutyrate (P13C=25%) with alkyl chains in R‐group, oxaloacetate (P13C=11%)...
Hyperpolarized (HP) 13C-labeled probes are emerging as promising agents to noninvasively image pH in vivo. HP [1,5-13C2]Z-OMPD (Z-4-methyl-2-oxopent-3-enedioic acid) particular has recently been used simultaneously report on kidney perfusion, filtration, and homeostasis, addition the ability detect local tumor acidification. In previous studies, dissolution dynamic nuclear polarization was hyperpolarize Z-OMPD. Here, we pioneered hyperpolarization of via SABRE-SHEATH (signal amplification by...
Despite its enormous utility in structural characterization, nuclear magnetic resonance (NMR) spectroscopy is inherently limited by low spin polarization. One method to address the polarization para-hydrogen (p-H2) induced (PHIP) which uses singlet isomer of H2 generate disparate populations amplify associated NMR signals. PHIP often relies on thermal catalysis or, more infrequently, UV-activated catalytic hydrogenation. Light-activated hydrogenation enables direct and timed control over...
Signal Amplification By Reversible Exchange in Shields Enable Alignment Transfer to Heteronuclei (SABRE-SHEATH) was employed boost 15N magnetic resonance sensitivity on common anti-cancer agents. The SABRE-SHEATH hyperpolarization dynamics of letrozole and anastrozole were independently optimized with respect solution temperature polarization transfer field. These studies enabled single scan detection the drugs at natural isotopic abundance working mM concentrations for over 30 minutes,...
We present the first in vivo hyperpolarized MR using Signal Amplification By Reversible Exchange.
Current metabolic imaging in humans is dominated by positron emission tomography (PET) methods. An emerging non-ionizing alternative for molecular hyperpolarized MRI. In particular, of 13C-pyruvate a leading candidate because pyruvate innocuous and has central role metabolism. However, simi-lar to PET, MRI with dynamic nuclear polarization (DNP) complex, costly requires complex in-frastructure. contrast, signal amplification reversible exchange (SABRE) fast, cheap, scalable...