The influence of water on protein properties.

The "dynamic" or "glass" transition in biomolecules is as important to their functioning as the folding process. This transition occurs in the low temperature regime and has been related to the onset of biochemical activity that is dependent on the hydration level. This protein transition is believed to be triggered by the strong hydrogen bond coupling in the hydration water. We study the vibrational bending mode and measure it using Fourier Transform Infrared spectroscopy. We demonstrate that at the molecular level the hydration water bending mode bonds the C=O and N-H peptide groups, and find that the temperature of the "dynamic" protein transition is the same as the fragile-to-strong dynamic transition in confined water. The fragile-to-strong dynamic transition in water governs the nature of the H bonds between water and peptides and appears to be universal in supercooled glass-forming liquids.

[1]  M. Leone,et al.  The boson peak of amyloid fibrils: probing the softness of protein aggregates by inelastic neutron scattering. , 2014, The journal of physical chemistry. B.

[2]  G. Schirò,et al.  Hydration dependence of myoglobin dynamics studied with elastic neutron scattering, differential scanning calorimetry and broadband dielectric spectroscopy. , 2014, Biophysical chemistry.

[3]  H. Stanley,et al.  The dynamical crossover in attractive colloidal systems. , 2013, The Journal of chemical physics.

[4]  A. Paciaroni,et al.  Nature of the water specific relaxation in hydrated proteins and aqueous mixtures , 2013 .

[5]  Sidney Yip,et al.  Multiscale materials modelling at the mesoscale. , 2013, Nature materials.

[6]  H. Stanley,et al.  The Boson peak in supercooled water , 2013, Scientific Reports.

[7]  G. Schirò,et al.  Physical origin of anharmonic dynamics in proteins: new insights from resolution-dependent neutron scattering on homomeric polypeptides. , 2012, Physical review letters.

[8]  J. C. Martinez-Garcia,et al.  The new insight into dynamic crossover in glass forming liquids from the apparent enthalpy analysis. , 2012, The Journal of chemical physics.

[9]  M. Vogel,et al.  Static and pulsed field gradient nuclear magnetic resonance studies of water diffusion in protein matrices. , 2011, The Journal of chemical physics.

[10]  S. H. Chen,et al.  The role of the dynamic crossover temperature and the arrest in glass-forming fluids , 2011, The European physical journal. E, Soft matter.

[11]  L. Pettersson,et al.  Spatially inhomogeneous bimodal inherent structure of simulated liquid water. , 2011, Physical chemistry chemical physics : PCCP.

[12]  H. Eugene Stanley,et al.  Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature , 2010, Proceedings of the National Academy of Sciences.

[13]  H. Stanley,et al.  Dynamical crossover and breakdown of the Stokes-Einstein relation in confined water and in methanol-diluted bulk water. , 2010, The journal of physical chemistry. B.

[14]  W. Doster,et al.  Dynamical transition of protein-hydration water. , 2009, Physical review letters.

[15]  John C. Mauro,et al.  Viscosity of glass-forming liquids , 2009, Proceedings of the National Academy of Sciences.

[16]  S. H. Chen,et al.  Evidence of dynamic crossover phenomena in water and other glass-forming liquids: experiments, MD simulations and theory , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[17]  H. Stanley,et al.  Appearance of a Fractional Stokes-Einstein Relation in Water and a Structural Interpretation of Its Onset , 2009 .

[18]  P. Baglioni,et al.  Proteins remain soft at lower temperatures under pressure. , 2009, The journal of physical chemistry. B.

[19]  J. Dyre,et al.  Little evidence for dynamic divergences in ultraviscous molecular liquids , 2008 .

[20]  P. Baglioni,et al.  The low-temperature dynamic crossover phenomenon in protein hydration water: simulations vs experiments. , 2008, The journal of physical chemistry. B.

[21]  Chung-Yuan Mou,et al.  The anomalous behavior of the density of water in the range 30 K < T < 373 K , 2007, Proceedings of the National Academy of Sciences.

[22]  Greg L. Hura,et al.  Effects of hydration water on protein methyl group dynamics in solution. , 2007, Physical review. E, Statistical, nonlinear, and soft matter physics.

[23]  A. Faraone,et al.  Evidence of the existence of the low-density liquid phase in supercooled, confined water , 2007, Proceedings of the National Academy of Sciences.

[24]  Chung-Yuan Mou,et al.  The violation of the Stokes–Einstein relation in supercooled water , 2006, Proceedings of the National Academy of Sciences.

[25]  S. H. A. Chen,et al.  Observation of fragile-to-strong dynamic crossover in protein hydration water. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[26]  J. Onuchic,et al.  Water mediation in protein folding and molecular recognition. , 2006, Annual review of biophysics and biomolecular structure.

[27]  D. Thirumalai,et al.  Dynamic transition in tRNA is solvent induced. , 2006, Journal of the American Chemical Society.

[28]  A. Cooper,et al.  Heat capacity effects in protein folding and ligand binding: a re-evaluation of the role of water in biomolecular thermodynamics. , 2005, Biophysical chemistry.

[29]  宁北芳,et al.  疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A , 2005 .

[30]  S. Woutersen,et al.  Vibrational relaxation of the H2O bending mode in liquid water. , 2004, The Journal of chemical physics.

[31]  Pablo G. Debenedetti,et al.  Supercooled and glassy water , 2003 .

[32]  A. L. Stevens,et al.  Polarization-selective femtosecond Raman spectroscopy of low-frequency motions in hydrated protein films , 2003 .

[33]  V. Daggett,et al.  The hydration of amides in helices; a comprehensive picture from molecular dynamics, IR, and NMR , 2003, Protein science : a publication of the Protein Society.

[34]  Richard A. L. Jones,et al.  Surface-mediated folding and misfolding of proteins at lipid/water interfaces , 2002 .

[35]  D. Tobias,et al.  Role of protein-water hydrogen bond dynamics in the protein dynamical transition. , 2002, Physical review letters.

[36]  G. Zaccai,et al.  How soft is a protein? A protein dynamics force constant measured by neutron scattering. , 2000, Science.

[37]  J. Pelton,et al.  Spectroscopic methods for analysis of protein secondary structure. , 2000, Analytical biochemistry.

[38]  S. Cannistraro,et al.  Neutron scattering evidence of a boson peak in protein hydration water. , 1999, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[39]  G. Careri.  Cooperative charge fluctuations by migrating protons in globular proteins. , 1998, Progress in biophysics and molecular biology.

[40]  R. Dyer,et al.  Fast events in protein folding: relaxation dynamics of secondary and tertiary structure in native apomyoglobin. , 1997, Proceedings of the National Academy of Sciences of the United States of America.

[41]  F. Stillinger,et al.  A Topographic View of Supercooled Liquids and Glass Formation , 1995, Science.

[42]  R. Raines,et al.  Amide-Amide and Amide-Water Hydrogen Bonds: Implications for Protein Folding and Stability. , 1994, Journal of the American Chemical Society.

[43]  G. Zaccaı̈,et al.  Thermal motions and function of bacteriorhodopsin in purple membranes: effects of temperature and hydration studied by neutron scattering. , 1993, Proceedings of the National Academy of Sciences of the United States of America.

[44]  G. Petsko,et al.  Crystalline ribonuclease A loses function below the dynamical transition at 220 K , 1992, Nature.

[45]  Professor Dr. George A. Jeffrey,et al.  Hydrogen Bonding in Biological Structures , 1991, Springer Berlin Heidelberg.

[46]  G. Careri,et al.  Protein hydration and function. , 1991, Advances in protein chemistry.

[47]  M. Sundaralingam,et al.  Water-inserted alpha-helical segments implicate reverse turns as folding intermediates. , 1989, Science.

[48]  Frauenfelder,et al.  Glassy behavior of a protein. , 1989, Physical review letters.

[49]  Wolfgang Doster,et al.  Dynamical transition of myoglobin revealed by inelastic neutron scattering , 1989, Nature.

[50]  Frank H. Stillinger,et al.  Supercooled liquids, glass transitions, and the Kauzmann paradox , 1988 .

[51]  G. Walrafen,et al.  Temperature dependence of the low‐ and high‐frequency Raman scattering from liquid water , 1986 .

[52]  E. Knapp,et al.  A consistent picture of protein dynamics. , 1984, Proceedings of the National Academy of Sciences of the United States of America.

[53]  Nivedita Borkakoti,et al.  Solvent-induced distortions and the curvature of α-helices , 1983, Nature.

[54]  Hans Frauenfelder,et al.  Temperature-dependent X-ray diffraction as a probe of protein structural dynamics , 1979, Nature.

[55]  L. Pauling,et al.  The structure of proteins; two hydrogen-bonded helical configurations of the polypeptide chain. , 1951, Proceedings of the National Academy of Sciences of the United States of America.