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Mapping Out Protein Hydration Dynamics by Overhauser Dynamic Nuclear Polarization

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Protein NMR

Part of the book series: Biological Magnetic Resonance ((BIMR,volume 32))

Abstract

Water molecules in the immediate vicinity of biomolecular surfaces (e.g., protein, lipid membranes, and DNA) are essential to mediate biological activities, such as enzyme activity, ligand binding, allosteric effect, or molecular recognition. For instance, the formation of a functional enzyme-substrate complex may be mediated by the retardation of water mobility at the active site of the enzyme. Hydrated water could also facilitate specific protein function, such as channel gating, whose kinetics has been found to be critically correlated with the rate of water fluctuations. Additionally, water is generally thought to be a catalyst for the hydrogen-bond rearrangements of a protein. The prevailing view is that water molecules actively contribute to the hydrophobic effect involved in protein-folding and ligand-binding events by modulating protein conformational changes through the formation or breaking of hydrogen bonds at protein–water interfaces. Interestingly, the diffusion dynamics of hydration water that entails hydrogen-bond rearrangement of the dynamic protein–water network may be critically coupled to protein dynamics, not only at the interfaces, but also at the core. A combination of the rapid hydrogen-bond rearrangements and the fast hydration dynamics at protein–water interfaces are suggested to be essential in increasing the protein structural flexibility and facilitating protein-ligand recognition.

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Notes

  1. 1.

    This condition is valid if I is proton and S is electron.

  2. 2.

    Here, S spin typically represents electron spin of nitroxide radical for ODNP

  3. 3.

    w 0, w 1 and w 2 are denoted as nuclear-electron zero-, single-, and double-quantum transition rates.

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Acknowledgment

This work was supported by the 2011 NIH Innovator award to SH, the cluster of Excellence RESOLV (EXC 1069) funded by the Deutsche Forschungsgemeinschaft and the WCU Program (R33-2008-000-10163-0) of KAIST to JS.

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Authors and Affiliations

  1. Department of Chemistry and Biochemistry, University of California, 93106, Santa Barbara, CA, USA

    Chi-Yuan Cheng, Jinsuk Song, John M. Franck & Songi Han

  2. Department of Chemical Engineering, University of California, 93106, Santa Barbara, CA, USA

    Songi Han

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  1. Chi-Yuan Cheng
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  2. Jinsuk Song
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  3. John M. Franck
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  4. Songi Han
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Correspondence to Songi Han .

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  1. Department of Chemistry and Biochemistry, University of Denver, Denver, Colorado, USA

    Lawrence Berliner

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Cheng, CY., Song, J., Franck, J., Han, S. (2015). Mapping Out Protein Hydration Dynamics by Overhauser Dynamic Nuclear Polarization. In: Berliner, L. (eds) Protein NMR. Biological Magnetic Resonance, vol 32. Springer, Boston, MA. https://doi.org/10.1007/978-1-4899-7621-5_2

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