title: Negative thermal expansion in single-component systems with isotropic interactions.
abstract: We have devised an isotropic interaction potential that gives rise to negative thermal expansion (NTE) behavior in equilibrium many-particle systems in both two and three dimensions over a wide temperature and pressure range (including zero pressure). An optimization procedure is used in order to find a potential that yields a strong NTE effect. A key feature of the potential that gives rise to this behavior is the softened interior of its basin of attraction. Although such anomalous behavior is well-known in material systems with directional interactions (e.g., zirconium tungstate), to our knowledge, this is the first time that NTE behavior has been established to occur in single-component many-particle systems for isotropic interactions. Using constant-pressure Monte Carlo simulations, we show that as the temperature is increased, the system exhibits negative, zero, and then positive thermal expansion before melting (for both two- and three-dimensional systems). The behavior is explicitly compared to that of a Lennard-Jones system, which exhibits typical expansion upon heating for all temperatures and pressures.
authors.affiliation: Department of Physics, Princeton University, Princeton, New Jersey 08544, USA.
authors.forename: Mikael C
authors.initials: MC
authors.lastname: Rechtsman
authors.forename: Frank H
authors.initials: FH
authors.lastname: Stillinger
authors.forename: Salvatore
authors.initials: S
authors.lastname: Torquato