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  4. Determination and evaluation of the nonadditivity in wetting of molecularly heterogeneous surfaces
 
research article

Determination and evaluation of the nonadditivity in wetting of molecularly heterogeneous surfaces

Luo, Zhi  
•
Murello, Anna  
•
Wilkins, David M.  
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December 17, 2019
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)

The interface between water and folded proteins is very complex. Proteins have "patchy" solvent-accessible areas composed of domains of varying hydrophobicity. The textbook understanding is that these domains contribute additively to interfacial properties (Cassie's equation, CE). An ever-growing number of modeling papers question the validity of CE at molecular length scales, but there is no conclusive experiment to support this and no proposed new theoretical framework. Here, we study the wetting of model compounds with patchy surfaces differing solely in patchiness but not in composition. Were CE to be correct, these materials would have had the same solid-liquid work of adhesion (WSL) and time-averaged structure of interfacial water. We find considerable differences in WSL, and sum-frequency generation measurements of the interfacial water structure show distinctively different spectral features. Molecular-dynamics simulations of water on patchy surfaces capture the observed behaviors and point toward significant nonadditivity in water density and average orientation. They show that a description of the molecular arrangement on the surface is needed to predict its wetting properties. We propose a predictive model that considers, for every molecule, the contributions of its first-nearest neighbors as a descriptor to determine the wetting properties of the surface. The model is validated by measurements of WSL in multiple solvents, where large differences are observed for solvents whose effective diameter is smaller than similar to 6 angstrom. The experiments and theoretical model proposed here provide a starting point to develop a comprehensive understanding of complex biological interfaces as well as for the engineering of synthetic ones.

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Type
research article
DOI
10.1073/pnas.1916180116
Web of Science ID

WOS:000503281500031

Author(s)
Luo, Zhi  
Murello, Anna  
Wilkins, David M.  
Kovacik, Filip  
Kohlbrecher, Joachim
Radulescu, Aurel
Okur, Halil I.  
Ong, Quy K.  
Roke, Sylvie  
Ceriotti, Michele  
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Date Issued

2019-12-17

Publisher

National Academy of Sciences

Published in
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)
Volume

116

Issue

51

Start page

25516

End page

25523

Subjects

Multidisciplinary Sciences

•

Science & Technology - Other Topics

•

hydration

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hydrophobic

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wetting

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nanostructured

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ligand shell

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hydrophobicity

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proteins

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modulation

•

behavior

Note

This is an open access article under the terms of the Creative Commons Attribution License

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
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COSMO  
LBP  
Available on Infoscience
January 5, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/164341
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