“Precise determination of pair interactions from pair statistics of many-body systems in and out of equilibrium” is Published in Physical Review E

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The determination of the pair potential \(v(\mathbf{r})\) that accurately yields an equilibrium state at positive temperature \(T\) with a prescribed pair correlation function \(g_2(\mathbf{r})\) or corresponding structure factor \(S(\mathbf{k})\) in \(d\)-dimensional Euclidean space \(\mathbb{R}^d\) is an outstanding inverse statistical mechanics problem with far-reaching implications. Recently, Zhang and Torquato [Phys. Rev. E 101, 032124 (2020)] conjectured that any realizable \(g_2(\mathbf{r})\) or \(S(\mathbf{k})\) corresponding to a translationally invariant nonequilibrium system can be attained by a classical equilibrium ensemble involving only (up to) effective pair interactions. Testing this conjecture for nonequilibrium systems as well as for nontrivial equilibrium states requires improved inverse methodologies. We have devised an optimization algorithm to precisely determine effective pair potentials that correspond to pair statistics of general translationally invariant disordered many-body equilibrium or nonequilibrium systems at positive temperatures. This methodology utilizes a parameterized family of pointwise basis functions for the potential function whose initial form is informed by small-, intermediate- and large-distance behaviors dictated by statistical-mechanical theory. Subsequently, a nonlinear optimization technique is utilized to minimize an objective function that incorporates both the target pair correlation function \(g_2(\mathbf{r})\) and structure factor \(S(\mathbf{k})\) so that the small intermediate- and large-distance correlations are very accurately captured. To illustrate the versatility and power of our methodology, we accurately determine the effective pair interactions of the following four diverse target systems: (1) Lennard-Jones system in the vicinity of its critical point, (2) liquid under the Dzugutov potential, (3) nonequilibrium random sequential addition packing, and (4) a nonequilibrium hyperuniform “cloaked” uniformly randomized lattice. We found that the optimized pair potentials generate corresponding pair statistics that accurately match their corresponding targets with total \(L_2\)-norm errors that are an order of magnitude smaller than that of previous methods. The results of our investigation lend further support to the Zhang-Torquato conjecture. Furthermore, our algorithm will enable one to probe systems with identical pair statistics but different higher-body statistics, which will shed light on the well-known degeneracy problem of statistical mechanics.