Experimental and theoretical evidence for bilayer-bybilayer surface melting of crystalline ice

M. Alejandra Sánchez, Tanja Kling, Tatsuya Ishiyama, Marc Jan Van Zadel, Patrick J. Bisson, Markus Mezger, Mara N. Jochum, Jenée D. Cyran, Wilbert J. Smit, Huib J. Bakker, Mary Jane Shultz, Akihiro Morita, Davide Donadio, Yuki Nagata, Mischa Bonn, Ellen H.G. Backus

Research output: Contribution to journalArticlepeer-review

79 Citations (Scopus)

Abstract

On the surface of water ice, a quasi-liquid layer (QLL) has been extensively reported at temperatures below its bulk melting point at 273 K. Approaching the bulk melting temperature from below, the thickness of the QLL is known to increase. To elucidate the precise temperature variation of the QLL, and its nature, we investigate the surface melting of hexagonal ice by combining noncontact, surfacespecific vibrational sum frequency generation (SFG) spectroscopy and spectra calculated from molecular dynamics simulations. Using SFG, we probe the outermost water layers of distinct single crystalline ice faces at different temperatures. For the basal face, a stepwise, sudden weakening of the hydrogen-bonded structure of the outermost water layers occurs at 257 K. The spectral calculations from the molecular dynamics simulations reproduce the experimental findings; this allows us to interpret our experimental findings in terms of a stepwise change from one to two molten bilayers at the transition temperature.

Original languageEnglish
Pages (from-to)227-232
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume114
Issue number2
DOIs
Publication statusPublished - 2017 Jan 10

Keywords

  • Crystalline ice
  • Stepwise
  • Sum frequency generation
  • Surface melting
  • Water

ASJC Scopus subject areas

  • General

Fingerprint

Dive into the research topics of 'Experimental and theoretical evidence for bilayer-bybilayer surface melting of crystalline ice'. Together they form a unique fingerprint.

Cite this