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Pheerawich Chitnelawong1, Francesco Sciortino2, Peter H Poole1

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The stability-limit conjecture (SLC) is thermodynamically permissible, even with liquid-liquid transitions. This resolves thermodynamic inconsistencies and explains water

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Area of Science:

  • Thermodynamics
  • Physical Chemistry
  • Materials Science

Background:

  • The stability-limit conjecture (SLC) posits a re-entrant spinodal in supercooled water, explaining diverging thermodynamic responses.
  • Previous arguments questioned the SLC's thermodynamic consistency with general principles.
  • The SLC's relation to the proposed liquid-liquid phase transition in water remains a key area of investigation.

Purpose of the Study:

  • To re-evaluate the thermodynamic viability of the stability-limit conjecture (SLC).
  • To clarify the SLC's compatibility with liquid-liquid phase transitions.
  • To explore unusual thermodynamic behaviors in systems with multiple phase transitions.

Main Methods:

  • Analysis of a model equation of state for water.
  • Thermodynamic modeling to demonstrate binodal-spinodal termination points.
  • Investigation of critical-point-free scenarios for liquid-liquid transitions.

Main Results:

  • Demonstrated that a binodal can terminate on a spinodal without a critical point.
  • Established the thermodynamic permissibility of the SLC in systems with both liquid-gas and liquid-liquid transitions.
  • Clarified unusual thermodynamic behaviors, including critical-point-free liquid-liquid transitions.

Conclusions:

  • The stability-limit conjecture is thermodynamically permissible.
  • The SLC can coexist with liquid-liquid phase transitions, resolving prior inconsistencies.
  • Findings have implications for understanding supercooled water and liquid silicon behavior.