Detecting the First Hydration Shell Structure around Biomolecules at Interfaces.

Autor:	Konstantinovsky D; Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States.; Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, Connecticut 06520, United States., Perets EA; Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States., Santiago T; Department of Chemistry, University at Buffalo, Buffalo, New York 14260, United States., Velarde L; Department of Chemistry, University at Buffalo, Buffalo, New York 14260, United States., Hammes-Schiffer S; Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States., Yan ECY; Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States.
Jazyk:	angličtina
Zdroj:	ACS central science [ACS Cent Sci] 2022 Oct 26; Vol. 8 (10), pp. 1404-1414. Date of Electronic Publication: 2022 Sep 06.
DOI:	10.1021/acscentsci.2c00702
Abstrakt:	Understanding the role of water in biological processes remains a central challenge in the life sciences. Water structures in hydration shells of biomolecules are difficult to study in situ due to overwhelming background from aqueous environments. Biological interfaces introduce additional complexity because biomolecular hydration differs at interfaces compared to bulk solution. Here, we perform experimental and computational studies of chiral sum frequency generation (chiral SFG) spectroscopy to probe chirality transfer from a protein to the surrounding water molecules. This work reveals that chiral SFG probes the first hydration shell around the protein almost exclusively. We explain the selectivity to the first hydration shell in terms of the asymmetry induced by the protein structure and specific protein-water hydrogen-bonding interactions. This work establishes chiral SFG as a powerful technique for studying hydration shell structures around biomolecules at interfaces, presenting new possibilities to address grand research challenges in biology, including the molecular origins of life. Competing Interests: The authors declare no competing financial interest. (© 2022 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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