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Self-Sustained Freeze-Sublime Oscillations at a Micrometer Liquid-Vacuum Interface
Alexander K Lemmens1, Nureshan Dias1, Musahid Ahmed1
1Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
The Journal of Physical Chemistry Letters
|June 26, 2026
Summary
Oscillating freeze-sublime cycles occur when liquids like acetone flow through tiny openings into a vacuum. This phenomenon involves rapid cooling, freezing, and sublimation, impacting microfluidics and space chemistry.
Area of Science:
- Physical Chemistry
- Materials Science
- Fluid Dynamics
Background:
- Liquids escaping into a vacuum through micro-apertures exhibit complex, rapid phase changes.
- Flash evaporation, cooling, and solidification are key processes at these micro-scale liquid-vacuum interfaces.
Purpose of the Study:
- Investigate the freeze-sublime oscillatory behavior of pure acetone and acetone-water mixtures.
- Analyze the dynamics of vapor emission and phase transitions in microchannels under vacuum.
Main Methods:
- Utilized single-photon ionization time-of-flight mass spectrometry to study effusing liquids.
- Employed Hertz-Knudsen evaporation framework for temporal decay analysis.
- Conducted heat-transfer simulations to model cooling zones and solidification.
Main Results:
- Observed self-sustained freeze-sublime oscillations with periodic vapor emission (tens of seconds).
- Identified transient solidification within the microchannel as the cause of suppressed flow.
- Demonstrated that water addition alters oscillation frequency and causes compositional segregation.
Conclusions:
- Micron-scale liquid-vacuum interfaces are nonequilibrium systems driven by evaporation and phase transitions.
- The freeze-sublime cycle has implications for microfluidics, vacuum chemistry, and astrophysical outgassing.
- Evaporative cooling can induce localized solidification, controlling liquid flow through micro-apertures.
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