The phase behavior of liquids confined in a slit geometry does not reveal a crossover from a three- to a two-dimensional behavior as the gap size decreases. Indeed, the prototypical two-dimensional hexatic phase only occurs in liquids confined to a monolayer. Here, we demonstrate that the dimensionality crossover is apparent in the lateral size dependence of the relaxation dynamics of confined liquids, developing a Debye model for the density of vibrational states of confined systems and performing extensive numerical simulations. In confined systems, Mermin-Wagner fluctuations enhance the amplitude of vibrational motion—or the Debye-Waller factor—by a quantity scaling as the inverse gap width and proportional to the logarithm of the aspect ratio, as a clear signature of a two-dimensional behavior. As the temperature or lateral system size increases, the crossover to a size-independent relaxation dynamics occurs when structural relaxation takes place before the vibrational modes with the longest wavelength develop.

• Received 15 December 2020
• Accepted 13 July 2021

DOI:https://doi.org/10.1103/PhysRevResearch.3.033172

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society