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Author

Ralph W. Adams

Other affiliations: University of York
Bio: Ralph W. Adams is an academic researcher from University of Manchester. The author has contributed to research in topics: Nuclear magnetic resonance spectroscopy & Hyperpolarization (physics). The author has an hindex of 29, co-authored 59 publications receiving 3212 citations. Previous affiliations of Ralph W. Adams include University of York.


Papers
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Journal ArticleDOI
27 Mar 2009-Science
TL;DR: It is shown here that a metal complex can facilitate the reversible interaction of para-hydrogen with a suitable organic substrate such that up to an 800-fold increase in proton, carbon, and nitrogen signal strengths are seen for the substrate without its hydrogenation.
Abstract: The sensitivity of both nuclear magnetic resonance spectroscopy and magnetic resonance imaging is very low because the detected signal strength depends on the small population difference between spin states even in high magnetic fields. Hyperpolarization methods can be used to increase this difference and thereby enhance signal strength. This has been achieved previously by incorporating the molecular spin singlet para-hydrogen into hydrogenation reaction products. We show here that a metal complex can facilitate the reversible interaction of para-hydrogen with a suitable organic substrate such that up to an 800-fold increase in proton, carbon, and nitrogen signal strengths are seen for the substrate without its hydrogenation. These polarized signals can be selectively detected when combined with methods that suppress background signals.

737 citations

Journal ArticleDOI
TL;DR: It is established here that [Ir(H)2(IMes)(py)3]Cl undergoes both pyridine (py) loss as well as the reductive elimination of H2 in a reversible process that delivers an 8100-fold increase in 1H NMR signal strength relative to non-hyperpolarized py at 3 T.
Abstract: While the characterization of materials by NMR is hugely important in the physical and biological sciences, it also plays a vital role in medical imaging This success is all the more impressive because of the inherently low sensitivity of the method We establish here that [Ir(H)2(IMes)(py)3]Cl undergoes both pyridine (py) loss as well as the reductive elimination of H2 These reversible processes bring para-H2 and py into contact in a magnetically coupled environment, delivering an 8100-fold increase in 1H NMR signal strength relative to non-hyperpolarized py at 3 T An apparatus that facilitates signal averaging has been built to demonstrate that the efficiency of this process is controlled by the strength of the magnetic field experienced by the complex during the magnetization transfer step Thermodynamic and kinetic data combined with DFT calculations reveal the involvement of [Ir(H)2(η2-H2)(IMes)(py)2]+, an unlikely yet key intermediate in the reaction Deuterium labeling yields an additional 60% i

295 citations

Journal ArticleDOI
TL;DR: A flexible and general pure shift experiment (PSYCHE) has been developed that offers superior sensitivity, spectral purity, and tolerance of strong coupling over existing methods for broadband homonuclear decoupling.
Abstract: All psyched up: A flexible and general pure shift experiment (PSYCHE) has been developed that offers superior sensitivity, spectral purity, and tolerance of strong coupling over existing methods for broadband homonuclear decoupling. The partial spectra of estradiol in [D6]DMSO obtained by normal 1H NMR spectroscopy and PSYCHE are shown for comparison.

232 citations

Journal ArticleDOI
TL;DR: The net effect of the polarization field strength on the resultant nuclear spin states is shown to be predictable but complex.
Abstract: When parahydrogen adds to a metal template containing a substrate of interest, the substrate and parahydrogen become coupled, and polarization is shared between the two without the incorporation of the parahydrogen into the substrate. A mechanism for this polarization transfer is presented in which the transfer is propagated through the scalar couplings. At zero field, polarization is transferred between two-, three-, and four-spin zero quantum states, but no single spin magnetization is created. The interplay between the chemical shift evolution and the evolution under scalar coupling at non-zero field generates additional longitudinal spin order and now includes single spin longitudinal z-magnetization. The additional chemical shift interaction introduces a field dependency to the nuclear spin states of the polarized substrate. The net effect of the polarization field strength on the resultant nuclear spin states is shown to be predictable but complex.

183 citations


Cited by
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28 Jul 2005
TL;DR: PfPMP1)与感染红细胞、树突状组胞以及胎盘的单个或多个受体作用,在黏附及免疫逃避中起关键的作�ly.
Abstract: 抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1(PfPMP1)与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用,在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员,通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

18,940 citations

Journal ArticleDOI
TL;DR: Two classes of lanthanide probes are focused on that are subsets of the larger area of metalloimaging: luminescent and magnetic lanthanides.
Abstract: The chemistry of the less familiar elements is a fascinating topic especially for the inorganic minded. The lanthanides, or rare earths, comprise the 5d block of the periodic table and represent a huge array of applications from catalysis to lasers, and of course, imaging agents.1 Recent advances in luminescence and magnetic resonance microscopy have, in part, been stimulated by extraordinary success in the development of new lanthanide probes. The unique properties of the lanthanides provide for a deep tool chest for the chemist, biologist and the imaging scientist to exploit, and that exploitation is in full swing. In this review we focus on two classes of lanthanide probes that are subsets of the larger area of metalloimaging: luminescent and magnetic lanthanides. In Section 2 we discuss the general design and photophysical properties of lanthanides and how these parameters are tuned to develop bioresponsive probes for optical imaging. In Section 3 we provide a brief description of how MR images are acquired and the how MRI contrast agents are engineered to respond to biological events of interest. These guiding principles have driven research that has produced a truly diverse number of new agents that are target specific and bioresponsive (or bioactivatable). While other imaging modalities utilize lanthanide-based probes, these topics are beyond the scope of this review. We direct the reader to explore some excellent reviews in the important areas of radiometals and multimodal imaging.2–5

901 citations

Journal ArticleDOI
TL;DR: In the in vivo T(1)-weighted magnetic resonance imaging (MRI), ESIONs showed longer circulation time than the clinically used gadolinium complex-based contrast agent, enabling high-resolution imaging and demonstrating the potential of ESions as T( 1) MRI contrast agents in clinical settings.
Abstract: Uniform and extremely small-sized iron oxide nanoparticles (ESIONs) of < 4 nm were synthesized via the thermal decomposition of iron–oleate complex in the presence of oleyl alcohol. Oleyl alcohol lowered the reaction temperature by reducing iron–oleate complex, resulting in the production of small-sized nanoparticles. XRD pattern of 3 nm-sized nanoparticles revealed maghemite crystal structure. These nanoparticles exhibited very low magnetization derived from the spin-canting effect. The hydrophobic nanoparticles can be easily transformed to water-dispersible and biocompatible nanoparticles by capping with the poly(ethylene glycol)-derivatized phosphine oxide (PO-PEG) ligands. Toxic response was not observed with Fe concentration up to 100 μg/mL in MTT cell proliferation assay of POPEG-capped 3 nm-sized iron oxide nanoparticles. The 3 nm-sized nanoparticles exhibited a high r1 relaxivity of 4.78 mM–1 s–1 and low r2/r1 ratio of 6.12, demonstrating that ESIONs can be efficient T1 contrast agents. The high r...

771 citations

Journal ArticleDOI
TL;DR: Challenges for CEST Agents and Hyperpolarized Probes: Use of Gd Contrast Agents with HyperPolarized Substances 3038.
Abstract: 3.3. Magnetic Particle Imaging 3029 4. Challenges for CEST Agents 3029 4.1. Technical Issues 3029 4.2. Chemical Issues 3031 4.3. Biological Issues 3032 5. Challenges for Heteronuclear MR Imaging 3033 5.1. F-Based Probes 3033 6. Challenges for Hyperpolarized Probes 3034 6.1. Brute Force 3034 6.2. Optical Pumping and Spin Exchange 3035 6.3. Dynamic Nuclear Polarization (DNP) 3035 6.4. para-Hydrogen Induced Polarization (PHIP) 3037 6.5. Use of Gd Contrast Agents with Hyperpolarized Substances 3038

714 citations