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Avoiding the Kauzmann Paradox via Interface-Driven Divergence in States.

Andrew Martin1,2, Jason R Green3,4, Martin Thuo1,2

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The Kauzmann paradox (KP) is challenged by surface chemical speciation in core-shell particles (CSPs). This phenomenon prevents equilibrium phase transitions, offering new insights into deep undercooling and glass formation.

Keywords:
Entropy catastropheGlassy systemsMetastabilityPhase transitionSupercooling

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Non-equilibrium Thermodynamics

Background:

  • The Kauzmann paradox (KP) posits that deeply supercooled liquids may possess lower entropy than crystalline solids.
  • While equilibrium thermodynamics extensively studies this entropy catastrophe, solidification is a far-from-equilibrium process.

Purpose of the Study:

  • To investigate how far-from-equilibrium processes, specifically surface chemical speciation in core-shell particles (CSPs), impact the Kauzmann paradox.
  • To explore the possibility of avoiding the entropy catastrophe during deep undercooling.

Main Methods:

  • Experimental and theoretical analysis of solidification in CSPs.
  • Modeling of nonequilibrium processes, including surface tensor asymmetry and thermodynamic speed limits.
  • Analysis of entropy production and configurational entropy in glass formation.

Main Results:

  • Surface chemical speciation in CSPs perturbs entropy production, hindering continuum equilibrium phase transitions.
  • Speciation-induced surface stress divergence generates nonequilibrium fluxes, frustrating homogeneous nucleation and enabling deep undercooling.
  • A modified form of the Kauzmann paradox emerges under thermodynamic speed limits, which can be averted by incorporating an interfacial state.

Conclusions:

  • Surface chemical speciation in CSPs offers a novel mechanism to avoid the Kauzmann paradox's entropy catastrophe.
  • Deep undercooling and glass formation can be achieved without violating fundamental thermodynamic principles by considering interfacial states.