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Configurational Entropy in Ice Nanosystems: Tools for Structure Generation and Screening.

P Parkkinen¹, S Riikonen¹, L Halonen¹

¹Laboratory of Physical Chemistry, Department of Chemistry, University of Helsinki , P.O. Box 55, FI-00014, Helsinki, Finland.

Journal of Chemical Theory and Computation

|November 19, 2015

Summary

This summary is machine-generated.

Researchers developed a program to explore proton disorder in nanoscale ice systems. This led to discovering a lower-energy ice nanodot isomer, suggesting inherent ferroelectricity in these systems.

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Area of Science:

Physical Chemistry
Materials Science
Nanotechnology

Background:

Low-temperature ice and water in nanoscale systems are subjects of recent experimental and theoretical interest.
Theoretical modeling faces the proton-disorder problem, requiring exploration of numerous configurations for accurate low-energy isomers and entropy effects.

Purpose of the Study:

To present an efficient, general-purpose program for searching and enumerating proton-configurational ensembles in hydrogen-bonded molecular systems.
To apply this program to experimentally relevant ice nanosystems, specifically a boron nitride film-supported ice nanodot.

Main Methods:

Development of a versatile computational program for finite, semiperiodic, and periodic hydrogen-bonded systems.
Systematic generation and analysis of the proton-configurational ensemble for an ice nanodot.
Benchmarking the program using ice nanotubes and finite slabs.

Main Results:

Identification of a novel ice nanodot isomer with an energy approximately 1 eV lower than previously studied configurations.
The identified isomer exhibits a significant dipole moment, indicating inherent ferroelectricity in ice nanodots parallel to the surface.
Demonstration of hydrogen-bond connectivity parameters as effective tools for screening low-energy isomers.

Conclusions:

The developed program efficiently addresses the proton-disorder problem in nanoscale ice.
Ice nanodots supported on boron nitride films possess inherent surface-parallel ferroelectricity.
Hydrogen-bond connectivity analysis provides a valuable method for identifying stable low-energy configurations in hydrogen-bonded nanomaterials.