Issue 19, 2020

Decoding the molecular water structure at complex interfaces through surface-specific spectroscopy of the water bending mode

Abstract

The structure of interfacial water determines atmospheric chemistry, wetting properties of materials, and protein folding. The challenge of investigating the properties of specific interfacial water molecules has frequently been confronted using surface-specific sum-frequency generation (SFG) vibrational spectroscopy using the O–H stretch mode. While perfectly suited for the water–air interface, for complex interfaces, a potential complication arises from the contribution of hydroxyl or amine groups of non-water species present at the surface, such as surface hydroxyls on minerals, or O–H and N–H groups contained in proteins. Here, we present a protocol to extract the hydrogen bond strength selectively of interfacial water, through the water bending mode. The bending mode vibrational frequency distribution provides a new avenue for unveiling the hydrogen bonding structure of interfacial water at complex aqueous interfaces. We demonstrate this method for the water–CaF2 and water–protein interfaces. For the former, we show that this method can indeed single out water O–H groups from surface hydroxyls, and that with increasing pH, the hydrogen-bonded network of interfacial water strengthens. Furthermore, we unveil enhanced hydrogen bonding of water, compared to bulk water, at the interface with human serum albumin proteins, a prototypical bio-interface.

Graphical abstract: Decoding the molecular water structure at complex interfaces through surface-specific spectroscopy of the water bending mode

Supplementary files

Article information

Article type
Paper
Submitted
05 Mar 2020
Accepted
23 Apr 2020
First published
23 Apr 2020
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2020,22, 10934-10940

Decoding the molecular water structure at complex interfaces through surface-specific spectroscopy of the water bending mode

T. Seki, C. Yu, X. Yu, T. Ohto, S. Sun, K. Meister, E. H. G. Backus, M. Bonn and Y. Nagata, Phys. Chem. Chem. Phys., 2020, 22, 10934 DOI: 10.1039/D0CP01269F

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