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@ARTICLE{Luo:867367,
      author       = {Luo, Zhi and Murello, Anna and Wilkins, David M. and
                      Kovacik, Filip and Kohlbrecher, Joachim and Radulescu, Aurel
                      and Okur, Halil I. and Ong, Quy K. and Roke, Sylvie and
                      Ceriotti, Michele and Stellacci, Francesco},
      title        = {{D}etermination and evaluation of the nonadditivity in
                      wetting of molecularly heterogeneous surfaces},
      journal      = {Proceedings of the National Academy of Sciences of the
                      United States of America},
      volume       = {116},
      number       = {51},
      issn         = {1091-6490},
      address      = {Washington, DC},
      publisher    = {National Acad. of Sciences},
      reportid     = {FZJ-2019-06043},
      pages        = {25516-25523},
      year         = {2019},
      abstract     = {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 ∼6 Å.
                      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.},
      cin          = {JCNS-FRM-II / JCNS-1 / MLZ},
      ddc          = {500},
      cid          = {I:(DE-Juel1)JCNS-FRM-II-20110218 /
                      I:(DE-Juel1)JCNS-1-20110106 / I:(DE-588b)4597118-3},
      pnm          = {6G4 - Jülich Centre for Neutron Research (JCNS) (POF3-623)
                      / 6G15 - FRM II / MLZ (POF3-6G15)},
      pid          = {G:(DE-HGF)POF3-6G4 / G:(DE-HGF)POF3-6G15},
      experiment   = {EXP:(DE-MLZ)KWS2-20140101},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {pmid:31792179},
      UT           = {WOS:000503281500031},
      doi          = {10.1073/pnas.1916180116},
      url          = {https://juser.fz-juelich.de/record/867367},
}