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Devitrification and melting in vapor deposited ice.
Fabio Leoni1, Fausto Martelli1,2,3, John Russo1
1Dipartimento di Fisica, Università degli Studi di Roma La Sapienza, Piazzale Aldo Moro 5, Rome 00185, Italy.
The Journal of Chemical Physics
|September 8, 2025
Summary
This study reveals how different amorphous ices melt and devitrify when heated. Vapor-deposited ices, unlike quenched ices, melt from the surface and show unique structural changes, indicating enhanced stability.
Area of Science:
- Materials Science
- Condensed Matter Physics
- Physical Chemistry
Background:
- Ultrastable glasses, particularly amorphous ices, exhibit complex equilibration dynamics under thermal stress.
- Understanding devitrification and melting is crucial for materials science and predicting glass behavior.
- Recent experimental and theoretical interest focuses on heating protocols for these materials.
Purpose of the Study:
- To investigate the devitrification and melting dynamics of conventional quenched (QG) and vapor-deposited (DG) amorphous ices.
- To correlate hydrogen-bond network statistics with structural stability during thermal processes.
- To differentiate melting behaviors between QG and DG amorphous ices.
Main Methods:
- Simulations using the mW water model.
- Controlled heating ramp protocols.
- Development of an algorithm to reconstruct hydrogen-bond networks and analyze bond ring statistics.
- Tracking crystalline and liquid clusters during devitrification and melting.
Main Results:
- Hydrogen bond ring statistics correlate with glass structural stability and track phase changes.
- QG melts in the bulk, while DG preferentially melts from the free surface.
- DG exhibits an excess of 5-membered rings near the surface, promoting crystal nucleation.
- DG shows an anomalous Avrami exponent, suggesting higher kinetic stability.
Conclusions:
- Melting behavior and devitrification pathways differ significantly between QG and DG amorphous ices.
- Hydrogen bond network analysis provides insights into the structural stability and phase transitions of amorphous solids.
- DG's surface-initiated melting and anomalous kinetics are linked to its enhanced kinetic stability.
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