Unveiling subsurface hydrogen-bond structure of hexagonal water ice

Yuji Otsuki, Toshiki Sugimoto, Tatsuya Ishiyama, Akihiro Morita, Kazuya Watanabe, Yoshiyasu Matsumoto

Research output: Contribution to journalArticlepeer-review

26 Citations (Scopus)

Abstract

The phase-resolved sum-frequency-generation (SFG) spectrum for the basal face of hexagonal ice is reported and is interpreted by molecular dynamics simulations combined with ab initio quantum calculations. Here, we demonstrate that the line shape of the SFG spectra of isotope-diluted OH chromophores is a sensitive indicator of structural rumpling uniquely emerging at the subsurface of hexagonal ice. In the outermost subsurface between the first (B1) and second (B2) bilayer, the hydrogen bond of OB1-H"OB2 is weaker than that of OB1"H-OB2. This implies that subsurface O-O distance is laterally altered, depending on the direction of O-H bond along the surface normal: H-up or H-down, which is in stark contrast to bulk hydrogen bonds. This new finding uncovers how water molecules undercoordinated at the topmost surface influence on the subsurface structural rumpling associated with orientational frustration inherent in water ice.

Original languageEnglish
Article number115405
JournalPhysical Review B
Volume96
Issue number11
DOIs
Publication statusPublished - 2017 Sep 5

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Fingerprint Dive into the research topics of 'Unveiling subsurface hydrogen-bond structure of hexagonal water ice'. Together they form a unique fingerprint.

Cite this