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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.

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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.