Interference between the glass, gel, and gas-liquid transitions

Area of Science:

• Physics
• Materials Science
• Chemical Engineering

Background:

• Interference between equilibrium gas-liquid transitions and non-equilibrium glass/gel transitions is experimentally observed.
• Known phenomena include spinodal line intersection with glass transition, multistep relaxation at gel/glass transition, and gel formation latency.

Purpose of the Study:

• To provide a unifying first-principles microscopic theoretical framework for understanding these complex transitions.
• To describe phenomena associated with spinodal decomposition, gelation, glass transition, and their combinations.

Main Methods:

• Utilizing the kinetic perspective of the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory.
• Applying the theory to irreversible processes in liquids.

Main Results:

• Demonstrated NE-SCGLE theory as a unifying framework for diverse liquid transitions.
• Identified the scenario as a competition between two kinetically limiting behaviors.
• Predicted bifurcation of the liquid-glass line at low densities below the spinodal intersection.

Conclusions:

• NE-SCGLE theory successfully describes the interplay between gas-liquid, glass, and gel transitions.
• The theory offers a microscopic understanding of dynamic arrest and its implications.
• The predicted liquid-glass line bifurcation provides new insights into liquid dynamics.