A Directional Entropic Force Approach for Self-Assembly of 3-Dimensional Enantioselective Crystals

Chiral crystalline structures have been increasingly investigated as a way to create metamaterials with extraordinary optical activity. Current strategies allowing for scalable self-assembly of 3-dimensional, bulk chiral structures do not allow for choice of chirality handedness, representing a missing route for the assembly of enantiopure chiral crystals. By using Monte Carlo simulations, we demonstrate how chiral building blocks can be used to assemble: i) a chiral crystal with pre-defined handedness bias; ii) a chiral crystal without pre-defined bias; and iii) an achiral crystal. We also demonstrate how control over the interaction strength between particles, performed here through the control over the depletant concentration in the system, can be used to reconfigure crystal structures between a chiral and an achiral lattice. Our results reveal previously missing assembly and reconfigurability routes which, together with literature results, close the loop towards assembly of 3-dimensional, bulk chiral crystalline structures with optical activity in the optical range.