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1ВОДНЫЕ РАСТВОРЫ В БИОЛОГИЧЕСКИХ СИСТЕМАХ
WATCHING LOW-FREQUENCY VIBRATIONS OF WATER IN BIOMOLECULAR RECOGNITION BY THz SPECTROSCOPY
Yao Xu, Martina Havenith
Lehrstuhl für Physikalische Chemie II, Ruhr Universität, 44801 Bochum, Germany Email address: yao.xu@rub.de Martina.Havenith@rub.de
Terahertz (THz) spectroscopy has turned out to be a powerful tool which is able to shed new light on the role of water in biomolecular processes. The low frequency spectrum of the solvated biomolecule in combination with MD simulations provides deep insights into the collective hydrogen bond dynamics on the sub-ps time scale. The absorption spectrum between 1 THz and 10 THz of solvated biomolecules is sensitive to changes in the fast fluctuations of the water network. Systematic studies on mutants of antifreeze proteins indicate a direct correlation between biological activity and a retardation of the (sub)-ps hydration dynamics at the protein binding site, i.e., a "hydration funnel".1 Kinetic THz absorption studies2 probe the temporal changes of THz absorption during a biological process, and give access to the kinetics of the coupled proteinhydration dynamics. When combined with simulations, the observed results can be explained in terms of a two-tier model involving a local binding and a long-range influence on the hydration bond dynamics of the water around the binding site that highlights the significance of the changes in the hydration dynamics at recognition site for biomolecular recognition.3 Water is shown to assist molecular recognition processes.4
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[2] Grossman, M.; Born, B.; Heyden, M.; Tworowski, D.; Fields, G. B.; Sagi, I.; Havenith, M. Correlated Structural Kinetics and Retarded Solvent Dynamics at the Metalloprotease Active Site. Nat. Struct. Mol. Biol. 18 (10), 1102-1108, (2011).
[3] Xu, Y.; Havenith, M. Perspective: Watching Low-Frequency Vibrations of Water in Biomolecular Recognition by THz Spectroscopy. J. Chem. Phys. 143 (17), 170901, (2015).
[4] Bellissent-Funel, M.-C.; Hassanali, A.; Havenith, M.; Henchman, R.; Pohl, P.; Sterpone, F.; van der Spoel, D.; Xu, Y.; Garcia, A. E. Water Determines the Structure and Dynamics of Proteins. Chem. Rev. 116 (13), 7673-7697, (2016).
