Inverse Design Method with Enhanced Sampling for Complex Open Crystals: Application to Novel Zeolite Self-assembly

Optimizing the design and synthesis of complex crystal
structures
presents pivotal opportunities and challenges in materials design.
While recent computational advances in inverse design have proven
effective for simpler crystals, their extension to intricate structures
such as zeolites remains challenging. In this work, we introduce an
efficient and robust inverse design workflow specifically tailored
for the predictive design of a broad range of complex phases. By integrating
an evolutionary parameter optimization strategy with enhanced sampling
molecular dynamics simulations, this approach effectively surmounts
the high energy barriers that typically hinder self-assembly in these
complex structures. We apply this inverse design workflow to facilitate
the efficient self-assembly of target zeolite frameworks in an efficient
coarse-grained model of a tetrahedral network-forming component and
a structure-directing agent. Using this method, we not only successfully
reproduce the self-assembly of known structures like the Z1 and SGT
zeolites and Type-I clathrates but also uncover previously unknown
optimal design parameters for SOD and CFI zeolites. Remarkably, our
approach also leads to the discovery of an uncatalogued framework,
which we designate as Z5. Our methodology not only enables the screening
and optimization of self-assembly protocols but also expands the possibilities
for discovering hypothetical structures, driving innovation in materials
design and offering a robust tool for advancing crystal engineering
in complex systems.