Isotropic pairwise interactions that promote the self assembly of complex
particle morphologies have been discovered by inverse design strategies derived
from the molecular coarse-graining literature. While such approaches provide an
avenue to reproduce structural correlations, thermodynamic quantities such as
the pressure have typically not been considered in self-assembly applications.
In this work, we demonstrate that relative entropy optimization can be used to
discover potentials that self-assemble into targeted cluster morphologies with
a prescribed pressure when the iterative simulations are performed in the
isothermal-isobaric ensemble. By tuning the pressure in the optimization, we
generate a family of simple pair potentials that all self-assemble the same
structure. Selecting an appropriate simulation ensemble to control the
thermodynamic properties of interest is a general design strategy that could
also be used to discover interaction potentials that self-assemble structures
having, for example, a specified chemical potential.Comment: 29 pages, 8 figure