Role of Surface Factors on Heterogeneous Ice Nucleation.
Degree: PhD, Chemical and Biomolecular Engineering, 2017, Clemson University
Heterogeneous ice nucleation is the primary pathway for ice formation. However, the detailed molecular mechanisms by which surfaces promote or hinder ice nucleation are not well understood. We present results from extensive molecular dynamics and forward flux sampling (FFS) simulations of ice nucleation near modified surfaces. The surfaces are modified to investigate the effects of different surface factors on the rate and mechanism of ice nucleation. We find that the surface charge distribution has significant effects on ice nucleation. We also investigate the interplay of surface lattice and hydrogen bonding properties in affecting ice nucleation. We find that lattice matching and hydrogen bonding are necessary but not sufficient conditions for observing ice nucleation at these surfaces. We correlate this behavior to the orientations sampled by the metastable supercooled water in contact with the surfaces. We find that ice is observed in cases where water molecules not only sample orientations favorable for bilayer formation but also do not sample unfavorable orientations. This distribution depends on both surface-water and water-water interactions and can change with subtle modifications to the surface properties. Our results provide insights into the diverse behavior of ice nucleation observed at different surfaces and highlights the complexity in elucidating heterogeneous ice nucleation. We also find that while the classical reaction coordinate of largest cluster size is a good measure of the transition between liquid water to ice, the addition of the neighboring liquid structure of the ice gives a better picture. We also have discovered that the structure of the second hydration layer gives a good representation of the reaction coordinate also.
Advisors/Committee Members: Dr. Sapna Sarupria, Committee Chair, Dr. David Bruce, Dr. Rachel Getman, Dr. Mark Roberts, Dr. Steve Stuart.
Subjects/Keywords: ice; interface; nucleation; simulation; Chemical Engineering
to Zotero / EndNote / Reference
APA (6th Edition):
Glatz, B. (2017). Role of Surface Factors on Heterogeneous Ice Nucleation. (Doctoral Dissertation). Clemson University. Retrieved from https://tigerprints.clemson.edu/all_dissertations/2400
Chicago Manual of Style (16th Edition):
Glatz, Brittany. “Role of Surface Factors on Heterogeneous Ice Nucleation.” 2017. Doctoral Dissertation, Clemson University. Accessed October 28, 2020.
MLA Handbook (7th Edition):
Glatz, Brittany. “Role of Surface Factors on Heterogeneous Ice Nucleation.” 2017. Web. 28 Oct 2020.
Glatz B. Role of Surface Factors on Heterogeneous Ice Nucleation. [Internet] [Doctoral dissertation]. Clemson University; 2017. [cited 2020 Oct 28].
Available from: https://tigerprints.clemson.edu/all_dissertations/2400.
Council of Science Editors:
Glatz B. Role of Surface Factors on Heterogeneous Ice Nucleation. [Doctoral Dissertation]. Clemson University; 2017. Available from: https://tigerprints.clemson.edu/all_dissertations/2400