Isomorph Invariance of Higher-Order Structural Measures in Four Lennard-Jones Systems

• Published in: Molecules (Basel, Switzerland) Vol. 26; no. 6; p. 1746
• Main Authors: Rahman, Mahajabin, Carter, Benjamin M G D, Saw, Shibu, Douglass, Ian M, Costigliola, Lorenzo, Ingebrigtsen, Trond S, Schrøder, Thomas B, Pedersen, Ulf R, Dyre, Jeppe C
• Format: Journal Article
• Language: English
• Published: Switzerland MDPI 20.03.2021; MDPI AG
• Subjects: bond-orientational order; density scaling; Frank-Kasper bonds; icosahedral local order; Lennard-Jones system; Voronoi structures; bond-orientational order; hidden scale invariance; Voronoi structures; density scaling; isomorph invariance; Frank-Kasper bonds; Lennard-Jones system; icosahedral local order; excess entropy
• DOI: 10.3390/molecules26061746
• ISSN: 1420-3049

In the condensed liquid phase, both single- and multicomponent Lennard-Jones (LJ) systems obey the "hidden-scale-invariance" symmetry to a good approximation. Defining an isomorph as a line of constant excess entropy in the thermodynamic phase diagram, the consequent approximate isomorph invariance of structure and dynamics in appropriate units is well documented. However, although all measures of the structure are predicted to be isomorph invariant, with few exceptions only the radial distribution function (RDF) has been investigated. This paper studies the variation along isomorphs of the nearest-neighbor geometry quantified by the occurrence of Voronoi structures, Frank-Kasper bonds, icosahedral local order, and bond-orientational order. Data are presented for the standard LJ system and for three binary LJ mixtures (Kob-Andersen, Wahnström, NiY2). We find that, while the nearest-neighbor geometry generally varies significantly throughout the phase diagram, good invariance is observed along the isomorphs. We conclude that higher-order structural correlations are no less isomorph invariant than is the RDF.