  relentless is an open-source Python package that enables the optimization of
objective functions computed using molecular dynamics simulations. It has a
high-level, extensible interface for model parametrization; setting up,
running, and analyzing simulations natively in established software packages;
and gradient-based optimization. We describe the design and implementation of
relentless in the context of relative entropy minimization, and we demonstrate
its abilities to design pairwise interactions between particles that form
targeted structures. relentless aims to streamline the development of
computational materials design methodologies and promote the transparency and
reproducibility of complex workflows integrating molecular dynamics
simulations.
