Self-diffusion of polycrystalline ice Ih under confining pressure: Hydrogen isotope analysis using 2-D Raman imaging

Naoki Noguchi, Tomoaki Kubo, William B. Durham, Hiroyuki Kagi, Ichiko Shimizu

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

We have developed a high-resolution technique based on micro Raman spectroscopy to measure hydrogen isotope diffusion profiles in ice Ih. The calibration curve for quantitative analysis of deuterium in ice Ih was constructed using micro Raman spectroscopy. Diffusion experiments using diffusion couples composed of dense polycrystalline H2O and D2O ice were carried out under a gas confining pressure of 100 MPa (to suppress micro-fracturing and pore formation) at temperatures from 235 K to 245 K and diffusion times from 0.2 to 94 hours. Two-dimensional deuterium profiles across the diffusion couples were determined by Raman imaging. The location of small spots of frost from room air could be detected from the shapes of the Raman bands of OH and OD stretching modes, which change because of the effect of the molar ratio of deuterium on the molecular coupling interaction. We emphasize the validity for screening the impurities utilizing the coupling interaction. Some recrystallization and grain boundary migration occurred in recovered diffusion couples, but analysis of two-dimensional diffusion profiles of regions not affected by grain boundary migration allowed us to measure a volume diffusivity for ice at 100 MPa of (2.8±0.4)×10-3exp-57.0±15.4kJ/molRTm2/s (R is the gas constant, T is temperature). Based on ambient pressure diffusivity measurements by others, this value indicates a high (negative) activation volume for volume diffusivity of -29.5 cm3/mol or more. We can also constrain the value of grain boundary diffusivity in ice at 100 MPa to be 4 that of volume diffusivity.

Original languageEnglish
Pages (from-to)40-47
Number of pages8
JournalPhysics of the Earth and Planetary Interiors
Volume257
DOIs
Publication statusPublished - Aug 1 2016
Externally publishedYes

Fingerprint

hydrogen isotopes
hydrogen isotope
confining pressure
confining
ice
diffusivity
deuterium
grain boundary
grain boundaries
Raman spectroscopy
profiles
frost
fracturing
analysis
gases
gas
quantitative analysis
rooms
screening
temperature

Keywords

  • Diffusion
  • Hydrogen isotope analysis
  • Ice
  • Pressure
  • Raman spectroscopy

ASJC Scopus subject areas

  • Geophysics
  • Space and Planetary Science
  • Physics and Astronomy (miscellaneous)
  • Astronomy and Astrophysics

Cite this

Self-diffusion of polycrystalline ice Ih under confining pressure : Hydrogen isotope analysis using 2-D Raman imaging. / Noguchi, Naoki; Kubo, Tomoaki; Durham, William B.; Kagi, Hiroyuki; Shimizu, Ichiko.

In: Physics of the Earth and Planetary Interiors, Vol. 257, 01.08.2016, p. 40-47.

Research output: Contribution to journalArticle

Noguchi, Naoki ; Kubo, Tomoaki ; Durham, William B. ; Kagi, Hiroyuki ; Shimizu, Ichiko. / Self-diffusion of polycrystalline ice Ih under confining pressure : Hydrogen isotope analysis using 2-D Raman imaging. In: Physics of the Earth and Planetary Interiors. 2016 ; Vol. 257. pp. 40-47.
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