Citation: John T. King, Evan J. Arthur, Derek G. Osborne, Charles L. Brooks Ⅲ, Kevin J. Kubarych. Biomolecular hydration dynamics probed with 2D-IR spectroscopy: From dilute solution to a macromolecular crowd[J]. Chinese Chemical Letters, ;2015, 26(4): 435-438. doi: 10.1016/j.cclet.2015.03.005 shu

Biomolecular hydration dynamics probed with 2D-IR spectroscopy: From dilute solution to a macromolecular crowd

1.
a Department of Chemistry, University of Michigan, Ann Arbor, MI 48109, USA;
2.
b LSA Biophysics, University of Michigan, Ann Arbor, MI 48109, USA

Corresponding author: Kevin J. Kubarych,
Received Date: 26 November 2014
Available Online: 9 January 2015
Fund Project: This work has been supported by the National Science Foundation (No. CHE-0748501) (No. CHE-0748501) the National Institutes of Health (No. RR012255) (No. RR012255)

Although it is well known that water is essential for biological function, it has been a challenge to determine how water behaves near biomacromolecular interfaces, and what role water plays in influencing the dynamics of the biochemical machinery. By adopting a vibrational labeling strategy coupled with ultrafast two-dimensional infrared (2D-IR) spectroscopy, it has recently become possible to study hydration dynamics, site specifically at the surface of proteins and model membranes. We review our recent progress in measuring hydration dynamics in contexts ranging from small-molecule solutes to biomacromolecules in dilute, viscous, and crowded environments.
- Protein hydration dynamics,
- Membrane dynamics,
- Ultrafast infrared spectroscopy
1. [1]
  [1] D. Chandler, Interfaces and the driving force of hydrophobic assembly, Nature 437 (2005) 640-647.
2. [2]
  [2] D.G. Osborne, J.A. Dunbar, J.G. Lapping, A.M. White, K.J. Kubarych, Site-specific measurements of lipid membrane interfacial water dynamics with multidimensional infrared spectroscopy, J. Phys. Chem. B 117 (2013) 15407-15414.
3. [3]
  [3] J.T. King, E.J. Arthur, C.L. Brooks, K.J. Kubarych, Site-specific hydration dynamics of globular proteins and the role of constrained water in solvent exchange with amphiphilic cosolvents, J. Phys. Chem. B 116 (2012) 5604-5611.
4. [4]
  [4] J.T. King, K.J. Kubarych, Site-specific coupling of hydration water and protein flexibility studied in solution with ultrafast 2D-IR spectroscopy, J. Am. Chem. Soc. 134 (2012) 18705-18712.
5. [5]
  [5] E.J. Arthur, J.T. King, K.J. Kubarych, C.L. Brooks, Heterogeneous preferential solvation of water and trifluoroethanol in homologous lysozymes, J. Phys. Chem. B 118 (2014) 8118-8127.
6. [6]
  [6] J.T. King, E.J. Arthur, C.L. Brooks, K.J. Kubarych, Crowding induced collective hydration of biological macromolecules over extended distances, J. Am. Chem. Soc. 136 (2014) 188-194.
7. [7]
  [7] P. Ball, Water as an active constituent in cell biology, Chem. Rev. 108 (2008) 74- 108.
8. [8]
  [8] J.T. King, M.R. Ross, K.J. Kubarych, Water-assisted vibrational relaxation of a metal carbonyl complex studied with ultrafast 2D-IR, J. Phys. Chem. B 116 (2012) 3754- 3759.
9. [9]
  [9] P. Hamm, M.T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy, Cambridge University Press, New York, 2011.
10. [10]
  [10] S. Roberts, J. Loparo, A. Tokmakoff, Characterization of spectral diffusion from two-dimensional line shapes, J. Chem. Phys. 125 (2006) 084502.
11. [11]
  [11] D.G. Osborne, J.T. King, J.A. Dunbar, A.M. White, K.J. Kubarych, Ultrafast 2DIR probe of a host-guest inclusion complex: structural and dynamical constraints of nanoconfinement, J. Chem. Phys. 138 (2013) 144501.
12. [12]
  [12] D.G. Osborne, K.J. Kubarych, Rapid and accurate measurement of the frequency- frequency correlation function, J. Phys. Chem. A 117 (2012) 5891-5898.
13. [13]
  [13] J.T. King, M.R. Ross, K.J. Kubarych, Ultrafast alpha-like relaxation of a fragile glassforming liquid measured using two-dimensional infrared spectroscopy, Phys. Rev. Lett. 108 (2012) 157401.
14. [14]
  [14] J.T. King, C.R. Baiz, K.J. Kubarych, Solvent-dependent spectral diffusion in a hydrogen bonded ‘‘Vibrational Aggregate'', J. Phys. Chem. A 114 (2010) 10590- 10604.
15. [15]
  [15] J.F. Brookes, K.M. Slenkamp, M.S. Lynch, M. Khalil, Effect of solvent polarity on the vibrational dephasing dynamics of the nitrosyl stretch in an FeII complex revealed by 2D IR spectroscopy, J. Phys. Chem. A 117 (2013) 6234-6243.
16. [16]
  [16] J. Qvist, E. Persson, C. Mattea, B. Halle, Time scales of water dynamics at biological interfaces: peptides, proteins and cells, Faraday Discuss. 141 (2009) 131-144.
17. [17]
  [17] W.H. Qiu, Y.T. Kao, L.Y. Zhang, et al., Protein surface hydration mapped by sitespecific mutations, Proc. Natl. Acad. Sci. U. S. A. 103 (2006) 13979-13984.
18. [18]
  [18] S.K. Pal, J. Peon, A.H. Zewail, Ultrafast surface hydration dynamics and expression of protein functionality: alpha-chymotrypsin, Proc. Natl. Acad. Sci. U. S. A. 99 (2002) 15297-15302.
19. [19]
  [19] F. Sterpone, G. Stirnemann, D. Laage, Magnitude and molecular origin of water slowdown next to a protein, J. Am. Chem. Soc. 134 (2012) 4116-4119.
20. [20]
  [20] A.C. Fogarty, D. Laage, Water dynamics in protein hydration shells: the molecular origins of the dynamical perturbation, J. Phys. Chem. B 118 (2014) 7715-7729.
21. [21]
  [21] T. Knubovets, J.J. Osterhout, P.J. Connolly, A.M. Klibanov, Structure, thermostability, and conformational flexibility of hen egg-white lysozyme dissolved in glycerol, Proc. Natl. Acad. Sci. U. S. A. 96 (1999) 1262-1267.
22. [22]
  [22] A.P. Minton, The influence of macromolecular crowding and macromolecular confinement on biochemical reactions in physiological media, J. Biol. Chem. 276 (2001) 10577-10580.
23. [23]
  [23] M. Sarkar, J. Lu, G.J. Pielak, Protein crowder charge and protein stability, Biochemistry 53 (2014) 1601-1606.
24. [24]
  [24] S. Ebbinghaus, S.J. Kim, M. Heyden, et al., An extended dynamical hydration shell around proteins, Proc. Natl. Acad. Sci. U. S. A. 104 (2007) 20749-20752.
25. [25]
  [25] V.C. Nibali, M. Havenith, New insights into the role of water in biological function: studying solvated biomolecules using terahertz absorption spectroscopy in conjunction with molecular dynamics simulations, J. Am. Chem. Soc. 136 (2014) 12800-12807.
26. [26]
  [26] C.R. Baiz, D. Schach, A. Tokmakoff, Ultrafast 2D IR microscopy, Opt. Express 22 (2014) 18724-18735.
27. [27]
  [27] T. Ando, J. Skolnick, Crowding and hydrodynamic interactions likely dominate in vivo macromolecular motion, Proc. Natl. Acad. Sci. U. S. A. 107 (2010) 18457- 18462.
28. [28]
  [28] A. Gershenson, L.M. Gierasch, Protein folding in the cell: challenges and progress, Curr. Opin. Struct. Biol. 21 (2011) 32-41.
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沈阳化工大学材料科学与工程学院沈阳 110142