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Title: Description of Hydration Water in Protein (Green Fluorescent Protein) Solution

Abstract

The structurally and dynamically perturbed hydration shells that surround proteins and biomolecules have a substantial influence upon their function and stability. This makes the extent and degree of water perturbation of practical interest for general biological study and industrial formulation. Here, we present an experimental description of the dynamical perturbation of hydration water around green fluorescent protein in solution. Less than two shells (~5.5 Å) were perturbed, with dynamics a factor of 2–10 times slower than bulk water, depending on their distance from the protein surface and the probe length of the measurement. Furthermore, this dependence on probe length demonstrates that hydration water undergoes subdiffusive motions (τ ∝ q–2.5 for the first hydration shell, τ ∝ q–2.3 for perturbed water in the second shell), an important difference with neat water, which demonstrates diffusive behavior (τ ∝ q–2). Our results help clarify the seemingly conflicting range of values reported for hydration water retardation as a logical consequence of the different length scales probed by the analytical techniques used.

Authors:
 [1];  [2];  [3];  [4];  [3];  [5];  [3];  [6];  [5];  [3];  [1];  [7];  [1];  [7]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Shull Wollan Center and Biology and Soft Matter Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biology and Soft Matter Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  5. (United States). Dept. of Biochemistry and Cellular and Molecular Biology
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Molecular Biophysics
  7. (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1341561
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 3; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Perticaroli, Stefania, Ehlers, Georg, Stanley, Christopher B., Mamontov, Eugene, O’Neill, Hugh, Univ. of Tennessee, Knoxville, TN, Zhang, Qiu, Cheng, Xiaolin, Univ. of Tennessee, Knoxville, TN, Myles, Dean A. A., Katsaras, John, Univ. of Tennessee, Knoxville, TN, Nickels, Jonathan D., and Univ. of Tennessee, Knoxville, TN. Description of Hydration Water in Protein (Green Fluorescent Protein) Solution. United States: N. p., 2016. Web. doi:10.1021/jacs.6b08845.
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Perticaroli, Stefania, Ehlers, Georg, Stanley, Christopher B., Mamontov, Eugene, O’Neill, Hugh, Univ. of Tennessee, Knoxville, TN, Zhang, Qiu, Cheng, Xiaolin, Univ. of Tennessee, Knoxville, TN, Myles, Dean A. A., Katsaras, John, Univ. of Tennessee, Knoxville, TN, Nickels, Jonathan D., & Univ. of Tennessee, Knoxville, TN. Description of Hydration Water in Protein (Green Fluorescent Protein) Solution. United States. https://doi.org/10.1021/jacs.6b08845
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Perticaroli, Stefania, Ehlers, Georg, Stanley, Christopher B., Mamontov, Eugene, O’Neill, Hugh, Univ. of Tennessee, Knoxville, TN, Zhang, Qiu, Cheng, Xiaolin, Univ. of Tennessee, Knoxville, TN, Myles, Dean A. A., Katsaras, John, Univ. of Tennessee, Knoxville, TN, Nickels, Jonathan D., and Univ. of Tennessee, Knoxville, TN. Wed . "Description of Hydration Water in Protein (Green Fluorescent Protein) Solution". United States. https://doi.org/10.1021/jacs.6b08845. https://www.osti.gov/servlets/purl/1341561.
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@article{osti_1341561,
title = {Description of Hydration Water in Protein (Green Fluorescent Protein) Solution},
author = {Perticaroli, Stefania and Ehlers, Georg and Stanley, Christopher B. and Mamontov, Eugene and O’Neill, Hugh and Univ. of Tennessee, Knoxville, TN and Zhang, Qiu and Cheng, Xiaolin and Univ. of Tennessee, Knoxville, TN and Myles, Dean A. A. and Katsaras, John and Univ. of Tennessee, Knoxville, TN and Nickels, Jonathan D. and Univ. of Tennessee, Knoxville, TN},
abstractNote = {The structurally and dynamically perturbed hydration shells that surround proteins and biomolecules have a substantial influence upon their function and stability. This makes the extent and degree of water perturbation of practical interest for general biological study and industrial formulation. Here, we present an experimental description of the dynamical perturbation of hydration water around green fluorescent protein in solution. Less than two shells (~5.5 Å) were perturbed, with dynamics a factor of 2–10 times slower than bulk water, depending on their distance from the protein surface and the probe length of the measurement. Furthermore, this dependence on probe length demonstrates that hydration water undergoes subdiffusive motions (τ ∝ q–2.5 for the first hydration shell, τ ∝ q–2.3 for perturbed water in the second shell), an important difference with neat water, which demonstrates diffusive behavior (τ ∝ q–2). Our results help clarify the seemingly conflicting range of values reported for hydration water retardation as a logical consequence of the different length scales probed by the analytical techniques used.},
doi = {10.1021/jacs.6b08845},
journal = {Journal of the American Chemical Society},
number = 3,
volume = 139,
place = {United States},
year = {Wed Oct 26 00:00:00 EDT 2016},
month = {Wed Oct 26 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/jacs.6b08845
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