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Title: Dynamics and unsteady morphologies at ice interfaces driven by D 2O–H 2O exchange

Abstract

The growth dynamics of D 2O ice in liquid H 2O in a microfluidic device were investigated between the melting points of D 2O ice (3.8 °C) and H 2O ice (0 °C). As the temperature was decreased at rates between 0.002 °C/s and 0.1 °C/s, the ice front advanced but retreated immediately upon cessation of cooling, regardless of the temperature. This is a consequence of the competition between diffusion of H 2O into the D 2O ice, which favors melting of the interface, and the driving force for growth supplied by cooling. Raman microscopy tracked H/D exchange across the solid H 2O–solid D 2O interface, with diffusion coefficients consistent with transport of intact H 2O molecules at the D 2O ice interface. At fixed temperatures below 3 °C, the D 2O ice front melted continuously, but at temperatures near 0 °C a scalloped interface morphology appeared with convex and concave sections that cycled between growth and retreat. Finally, this behavior, not observed for D 2O ice in contact with D 2O liquid or H 2O ice in contact with H 2O liquid, reflects a complex set of cooperative phenomena, including H/D exchange across the solid–liquid interface, latent heat exchange,more » local thermal gradients, and the Gibbs–Thomson effect on the melting points of the convex and concave features.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [2]; ORCiD logo [3]
  1. New York Univ. (NYU), New York, NY (United States). Dept. of Chemistry, and Molecular Design Inst.; Yeshiva Univ., New York, NY (United States). Dept. of Chemistry and Biochemistry
  2. New York Univ. (NYU), New York, NY (United States). Courant Inst. of Mathematical Sciences
  3. New York Univ. (NYU), New York, NY (United States). Dept. of Chemistry, and Molecular Design Inst.
Publication Date:
Research Org.:
New York Univ. (NYU), New York, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1540260
Grant/Contract Number:  
SC0012296
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 44; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; science & technology; ice growth; microfluids; hydrogen-deuterium exchange; Raman microscopy; ice morphology

Citation Formats

Drori, Ran, Holmes-Cerfon, Miranda, Kahr, Bart, Kohn, Robert V., and Ward, Michael D. Dynamics and unsteady morphologies at ice interfaces driven by D2O–H2O exchange. United States: N. p., 2017. Web. doi:10.1073/pnas.1621058114.
Drori, Ran, Holmes-Cerfon, Miranda, Kahr, Bart, Kohn, Robert V., & Ward, Michael D. Dynamics and unsteady morphologies at ice interfaces driven by D2O–H2O exchange. United States. doi:10.1073/pnas.1621058114.
Drori, Ran, Holmes-Cerfon, Miranda, Kahr, Bart, Kohn, Robert V., and Ward, Michael D. Mon . "Dynamics and unsteady morphologies at ice interfaces driven by D2O–H2O exchange". United States. doi:10.1073/pnas.1621058114. https://www.osti.gov/servlets/purl/1540260.
@article{osti_1540260,
title = {Dynamics and unsteady morphologies at ice interfaces driven by D2O–H2O exchange},
author = {Drori, Ran and Holmes-Cerfon, Miranda and Kahr, Bart and Kohn, Robert V. and Ward, Michael D.},
abstractNote = {The growth dynamics of D2O ice in liquid H2O in a microfluidic device were investigated between the melting points of D2O ice (3.8 °C) and H2O ice (0 °C). As the temperature was decreased at rates between 0.002 °C/s and 0.1 °C/s, the ice front advanced but retreated immediately upon cessation of cooling, regardless of the temperature. This is a consequence of the competition between diffusion of H2O into the D2O ice, which favors melting of the interface, and the driving force for growth supplied by cooling. Raman microscopy tracked H/D exchange across the solid H2O–solid D2O interface, with diffusion coefficients consistent with transport of intact H2O molecules at the D2O ice interface. At fixed temperatures below 3 °C, the D2O ice front melted continuously, but at temperatures near 0 °C a scalloped interface morphology appeared with convex and concave sections that cycled between growth and retreat. Finally, this behavior, not observed for D2O ice in contact with D2O liquid or H2O ice in contact with H2O liquid, reflects a complex set of cooperative phenomena, including H/D exchange across the solid–liquid interface, latent heat exchange, local thermal gradients, and the Gibbs–Thomson effect on the melting points of the convex and concave features.},
doi = {10.1073/pnas.1621058114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 44,
volume = 114,
place = {United States},
year = {2017},
month = {10}
}

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