Systematic exploration of accessible topologies of cage molecules via minimalistic models

Abstract

Cages are macrocyclic structures with an intrinsic internal cavity that support applications in separations, sensing and catalysis. These materials can be synthesised via self-assembly of organic or metal-organic building blocks....

De Novo Atomistic Discovery of Disordered Mechanical Metamaterials by Machine Learning

“…Despite the structural stability present herein, we must pay attention to different molecular design rules that may significantly affect the stability of their final structures, such as a molecular design strategy proposed recently to explore the energy‐stable molecular topology by tuning bond angles of building blocks and assembling the building blocks into different types of topological cages. [ 21 ] Theoretically, it is true that some configurations are more unstable than others and occupy higher energy state in their potential energy landscape (PEL). [ 26,31 ] From the PEL viewpoint, the structural stability of our melt‐quenched structures is likely originated from the fact that, by tuning forcefield parameters, the topography of PEL varies accordingly but our melt‐quenching rule enables each structure to fully relax in its own PEL with no confinement, so as to reach a deep local minimum.…”

“…[ 18–20 ] Impressively, recent study inspires us with automatic design of topology‐accessible molecular assembly by devising its constitutive building blocks. [ 21 ] However, built upon spatial arrangement of particle‐level blocks, such particle systems such as glasses are traditionally stereotyped as the pristine bulk elements of architected materials—rather than the architected material itself. [ 22,23 ] rendering it elusive whether mechanical metamaterials can be feasible at atomistic or microparticle level, [ 6,24 ] let alone the atomistic lesson of structural disorder in devising metamaterials.…”

Dynamic covalent synthesis

“…Looking ahead, one can foresee major developments coming from molecular modelling approaches where simple tools can enable screening in silico the formation of cage-type structures which will be particularly informative for flexible systems. 158 Combining such computational tools with robotic screening will significantly speed up the discovery process and expand the range of complex structures that can be produced. 159 With the escalating impact of artificial intelligence, 160,161 this growing body of data will improve the predictability of complex synthesis of discrete assemblies.…”