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Heating a crystalline solid increases the average energy of its atoms, molecules, or ions, and the solid gets hotter. At some point, the added energy becomes large enough to partially overcome the forces holding the molecules or ions of the solid in their fixed positions, and the solid begins the process of transitioning to the liquid state or melting. At this point, the temperature of the solid stops rising, despite the continual input of heat, and it remains constant until all of the solid is...
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Reaction Coordinate for Ice Crystallization on a Soft Surface.

Laura Lupi1, Rebecca Hanscam1, Yuqing Qiu1

  • 1Department of Chemistry, The University of Utah , 315 South 1400 East, Salt Lake City, Utah 84112-0850, United States.

The Journal of Physical Chemistry Letters
|August 22, 2017
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Summary
This summary is machine-generated.

Molecular simulations reveal that while soft surface flexibility hinders ice nucleation, it doesn't affect the transformation pathway. Crystal cluster size, not surface dynamics, drives ice formation, similar to homogeneous crystallization.

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Area of Science:

  • Molecular simulations
  • Materials science
  • Physical chemistry

Background:

  • Molecular assembly and crystallization are critical in chemistry, engineering, and materials science.
  • Natural processes like atmospheric ice formation and biomineralization involve crystallization.
  • Soft surfaces, including organic interfaces and biomolecules, influence crystal nucleation rates due to structural fluctuations.

Purpose of the Study:

  • To investigate the role of soft surface degrees of freedom in the reaction coordinate for crystal nucleation.
  • To understand the mechanism of ice nucleation promoted by an alcohol monolayer.
  • To determine if surface flexibility impacts the transformation pathway from liquid to ice.

Main Methods:

  • Utilized molecular simulations to model ice nucleation on an alcohol monolayer.
  • Analyzed the impact of surface flexibility on nucleation ability and the transformation coordinate.
  • Compared the driving variables for heterogeneous and homogeneous crystallization.

Main Results:

  • Surface flexibility significantly reduces ice nucleation ability.
  • Surface flexibility does not influence the reaction coordinate for the liquid-to-ice transformation.
  • The size of the crystalline cluster is the primary variable driving the transformation, consistent with homogeneous crystallization.

Conclusions:

  • The flexibility of soft surfaces, despite affecting nucleation rates, does not alter the fundamental pathway of crystallization.
  • Crystal cluster size governs the transformation coordinate, a principle applicable to both heterogeneous and homogeneous ice nucleation.
  • A separation of timescales between surface fluctuations and transition state barrier crossing likely explains this general phenomenon.