title: Basis function sampling: a new paradigm for material property computation.
abstract: Wang-Landau sampling, and the associated class of flat histogram simulation methods have been remarkably helpful for calculations of the free energy in a wide variety of physical systems. Practically, convergence of these calculations to a target free energy surface is hampered by reliance on parameters which are unknown a priori. Here, we derive and implement a method built upon orthogonal functions which is fast, parameter-free, and (importantly) geometrically robust. The method is shown to be highly effective in achieving convergence. An important feature of this method is its ability to attain arbitrary levels of description for the free energy. It is thus ideally suited to in silico measurement of elastic moduli and other material properties related to free energy perturbations. We demonstrate the utility of such applications by applying our method to calculate the Frank elastic constants of the Lebwohl-Lasher model of liquid crystals.
authors.affiliation: Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, USA and Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA.
authors.forename: Jonathan K
authors.initials: JK
authors.lastname: Whitmer
authors.affiliation: Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, USA and Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA.
authors.forename: Chi-cheng
authors.initials: CC
authors.lastname: Chiu
authors.affiliation: Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706-1691, USA.
authors.forename: Abhijeet A
authors.initials: AA
authors.lastname: Joshi
authors.affiliation: Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, USA and Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA.
authors.forename: Juan J
authors.initials: JJ
authors.lastname: de Pablo
mesh_terms: D003198:Computer Simulation; D004548:Elasticity; D050866:Liquid Crystals / Q000737:chemistry; D008962:Models, Theoretical; D009010:Monte Carlo Method; D013816:Thermodynamics