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Comment on the characterization of local structure in an inhomogeneous liquid

The search for local structures within a disordered medium has led to proposals of several methods for probing transient short-range symmetry in a homogeneous mono-atomic liquid. We offer a comparison of different characterizations of such local structure in an in-homogeneous liquid. We simulate the interfaces between a Lennard-Jones liquid and (i) a flat Lennard-Jones wall, (ii) a wall of face-centered cubic-packed Lennard-Jones particles, and (iii) a Lennard-Jones vapor. The interface density distributions in cases (i) and (ii) have oscillations extending several particle diameters into the bulk liquid, while that in case (iii) the interface density distribution monotonically decays from the bulk liquid to the vapor. We search for transient ordered fluctuations, which we identify with local ordered structures, using the Aperture Cross Correlation Function of the system. We find that only particles in the FCC-liquid interface that are in the two layers closest to the FCC surface exhibit preferred four-fold symmetry. Furthermore, the absence of three- or five-fold symmetry peaks in the Aperture Cross Correlation Function of the liquid-vapor interface yields a different picture of that interface than derived from the high density of bi-pyramidal clusters found in the Topological Cluster Classification study (Molecular Physics, 109 (7-10), 1393-1402 (2011)). While the Aperture Cross Correlation Function results need not be viewed as contradictory with the Topological Cluster Classification results, we argue the advantages of using the former to characterize transient ordered fluctuations as being both experimentally accessible in favorable cases and not reliant on a list of structures.