Controlled Folding, Motional, and Constitutional Dynamic Processes of Polyheterocyclic Molecular Strands

General design principles have been developed for the control of the structural features of polyheterocyclic strands and their effector‐modulated shape changes. Induced defined molecular motions permit designed enforcement of helical as well as linear molecular shapes. The ability of such molecular strands to bind metal cations allows the generation of coiling/uncoiling processes between helically folded and extended linear states. Large molecular motions are produced on coordination of metal ions, which may be made reversible by competition with an ancillary complexing agent and fueled by sequential acid/base neutralization energy. The introduction of hydrazone units into the strands confers upon them constitutional dynamics, whereby interconversion between different strand compositions is achieved through component exchange. These features have relevance for nanomechanical devices. We present a morphological and functional analysis of such systems developed in our laboratories. This Review discusses the structural and functional features of polyheterocyclic ligand strands that display designed specific shapes, undergo shape changes on binding of metal cations, and perform various types of pH‐responsive motions induced by metal ions.