Cooperative metal–photoswitch
interfaces comprise an application-driven
field which is based on strategic coupling of metal cations and organic
photochromic molecules to advance the behavior of both components,
resulting in dynamic molecular and material properties controlled
through external stimuli. In this Perspective, we highlight the ways
in which metal–photoswitch interplay can be utilized as a tool
to modulate a system’s physicochemical properties and performance
in a variety of structural motifs, including discrete molecular complexes
or cages, as well as periodic structures such as metal–organic
frameworks. This Perspective starts with photochromic molecular complexes
as the smallest subunit in which metal–photoswitch interactions
can occur, and progresses toward functional materials. In particular,
we explore the role of the metal–photoswitch relationship for
gaining fundamental knowledge of switchable electronic and magnetic
properties, as well as in the design of stimuli-responsive sensors,
optically gated memory devices, catalysts, and photodynamic therapeutic
agents. The abundance of stimuli-responsive systems in the natural
world only foreshadows the creative directions that will uncover the
full potential of metal–photoswitch interactions in the coming
years.