Chemical Information Processing by a Responsive Chemical System

Abstract

Nature has an extraordinary capacity to precisely regulate the chemical reactivity in a highly complex mixture of molecules that is present in the cell. External stimuli lead to transient up-and downregulation of chemical reactions and provide a means for a cell to process information arriving from the environment. The development of synthetic chemical systems with life-like properties requires strategies that allow likewise control over chemical reactivity in a complex environment. Here, we show a synthetic system that mimics the initial steps that take place when a natural signal transduction pathway is activated. Monophosphate nucleosides act as chemical triggers for the self-assembly of nanoreactors that upregulate chemical reactions between reagents present at low micromolar concentrations. Different nucleotides template different assemblies and hence activate different pathways, thus establishing a distinct connection between input and output molecules. Trigger-induced upregulation of chemical reactivity occurs for only a limited amount of time because the chemical triggers are gradually removed from the system by enzymes. It is shown that the same system transiently produces different output molecules depending on the chemical input that is provided.

Chemically fueled dynamic switching between assembly-encoded emissions

“…Only in a few instances has this regulatory mechanism been applied to control the functional outcome of the transiently stable assembled structure. 22–28 Most importantly, applying a similar mechanism towards an aggregate-to-aggregate transformation, and thereby dynamic switching between the associated physical properties, has not been paid much attention. 29–32 Aggregate-to-aggregate transformation is of interest as it can potentially expand the horizon of chemically fueled self-assembled systems beyond the ON–OFF functional outcome associated with the monomer-to-aggregate transition.…”