Title: Dynamics and unsteady morphologies at ice interfaces driven by D₂O–H₂O exchange

Abstract

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 andmore » concave features.« less

Authors:

Drori, Ran  ^[1];

• Search DOE PAGES for author "Drori, Ran"
• Search DOE PAGES for ORCID "0000-0002-6436-5602"

Holmes-Cerfon, Miranda ^[2]; Kahr, Bart  ^[3];

• Search DOE PAGES for author "Kahr, Bart"
• Search DOE PAGES for ORCID "0000-0002-7005-4464"

Kohn, Robert V. ^[2]; Ward, Michael D.  ^[3]

• Search DOE PAGES for author "Ward, Michael D."
• Search DOE PAGES for ORCID "0000-0002-2090-781X"

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+ Show Author Affiliations

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:

Mon Oct 30 00:00:00 EDT 2017

Research Org.:

New York Univ. (NYU), 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