Sensitivity enhancement in solution NMR: Emerging ideas and new frontiers

Lee, Jung Ho; Okuno, Yusuke; Cavagnero, Silvia

doi:10.1016/j.jmr.2014.01.005

Cited by 156 publications

(165 citation statements)

References 154 publications

(199 reference statements)

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“…[1,2] In liquid state NMR, dissolution dynamic nuclear polarization (D-DNP) is interesting for its versatility in polarizing various molecules and nuclei. A distinguishing feature of D-DNP is the separation of a location for hyperpolarization from a location for performing the NMR experiment.…”

Section: Introductionmentioning

confidence: 99%

Implementation and Characterization of Flow Injection in Dissolution Dynamic Nuclear Polarization NMR Spectroscopy

Chen¹,

Hilty²

2015

ChemPhysChem

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Dissolution dynamic nuclear polarization (D-DNP) offers a substantial signal increase for liquid state NMR. A challenge in realizing the possible gain lies in the transfer of the hyperpolarized sample to the NMR detector without loss of hyperpolarization. Here, we demonstrate that a flow injection method using high pressure liquid leads to improved performance compared to the more common gas driven injection, by suppressing residual fluid motions during the NMR experiment while still achieving short injection time. Apparent diffusion coefficients were determined from pulsed field gradient echo measurements, and were shown to fall below 1.5x the value of a static sample within 0.8 s. Due to the single-scan nature of D-DNP, pulsed field gradients are often the only choice for coherence selection or encoding, but their application requires stationary fluid. Sample delivery driven by a high-pressure liquid will improve the applicability of these types of advanced experiments in D-DNP.

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Section: Introductionmentioning

confidence: 99%

Implementation and Characterization of Flow Injection in Dissolution Dynamic Nuclear Polarization NMR Spectroscopy

Chen¹,

Hilty²

2015

ChemPhysChem

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“…The main DNP methods employed today are dissolution DNP [54], MAS-DNP [90] and Overhauser DNP [50]. Details of these methods can be found elsewhere [91,92]. Dissolution DNP is used for metabolic imaging, biomolecular NMR [63,64] and biological assays [65,66] while MAS-DNP has found its applications in surface chemistry, protein structure determination and polymer studies [41,40].…”

Section: Introductionmentioning

confidence: 99%

Rapid-melt Dynamic Nuclear Polarization

Sharma¹,

Janssen²,

Leggett³

et al. 2015

Journal of Magnetic Resonance

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“…Observable phenomena include magnetic field effects 1-3 and magnetic isotope effects 4 on chemical reactivity, and the production of large electron 5,6 and nuclear 7,8 spin hyperpolarizations -effects that collectively constitute the field of spin chemistry. 9 The most intensively studied entities that exhibit these behaviours are the radical pairs that are formed as transient intermediates in thermal and photochemical reactions in condensed phases.…”

Section: Introductionmentioning

confidence: 99%

Asymmetric recombination and electron spin relaxation in the semiclassical theory of radical pair reactions

Lewis

Manolopoulos

Hore

2014

The Journal of Chemical Physics

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We describe how the semiclassical theory of radical pair recombination reactions recently introduced by two of us [D. E. Manolopoulos and P. J. Hore, J. Chem. Phys. 139, 124106 (2013)] can be generalised to allow for different singlet and triplet recombination rates. This is a non-trivial generalisation because when the recombination rates are different the recombination process is dynamically coupled to the coherent electron spin dynamics of the radical pair. Furthermore, because the recombination operator is a two-electron operator, it is no longer sufficient simply to consider the two electrons as classical vectors: one has to consider the complete set of 16 two-electron spin operators as independent classical variables. The resulting semiclassical theory is first validated by comparison with exact quantum mechanical results for a model radical pair containing 12 nuclear spins. It is then used to shed light on the spin dynamics of a carotenoid-porphyrin-fullerene (CPF) triad containing considerably more nuclear spins which has recently been used to establish a 'proof of principle' for the operation of a chemical compass [K. Maeda et al., Nature 453, 387 (2008)]. We find in particular that the intriguing biphasic behaviour that has been observed in the effect of an Earth-strength magnetic field on the time-dependent survival probability of the photo-excited C ·+ PF ·− radical pair arises from a delicate balance between its asymmetric recombination and the relaxation of the electron spin in the carotenoid radical.

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Sensitivity enhancement in solution NMR: Emerging ideas and new frontiers

Cited by 156 publications

References 154 publications

Implementation and Characterization of Flow Injection in Dissolution Dynamic Nuclear Polarization NMR Spectroscopy

Implementation and Characterization of Flow Injection in Dissolution Dynamic Nuclear Polarization NMR Spectroscopy

Rapid-melt Dynamic Nuclear Polarization

Asymmetric recombination and electron spin relaxation in the semiclassical theory of radical pair reactions

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