Generic concept to program the time domain of self-assemblies with a self-regulation mechanism.
Nature regulates complex structures in space and time via feedback loops, kinetically controlled transformations, and under energy dissipation to allow non-equilibrium processes. Although man-made static self-assemblies realize excellent control over hierarchical structures via molecular programming, managing their temporal destiny by self-regulation is a largely unsolved challenge. Herein, we introduce a generic concept to control the time domain by programming the lifetimes of switchable self-assemblies in closed systems. We conceive dormant deactivators that, in combination with fast promoters, enable a unique kinetic balance to establish an autonomously self-regulating, transient pH-state, whose duration can be programmed over orders of magnitude-from minutes to days. Coupling this non-equilibrium state to pH-switchable self-assemblies allows predicting their assembly/disassembly fate in time, similar to a precise self-destruction mechanism. We demonstrate a platform approach by programming self-assembly lifetimes of block copolymers, nanoparticles, and peptides, enabling dynamic materials with a self-regulation functionality.
DWI-Leibniz-Institute for Interactive Materials, Forckenbeckstraße 50, 52074 Aachen, Germany.
Thomas
T
Heuser
DWI-Leibniz-Institute for Interactive Materials, Forckenbeckstraße 50, 52074 Aachen, Germany.
Ann-Kathrin
AK
Steppert
DWI-Leibniz-Institute for Interactive Materials, Forckenbeckstraße 50, 52074 Aachen, Germany.
Catalina Molano
CM
Lopez
DWI-Leibniz-Institute for Interactive Materials, Forckenbeckstraße 50, 52074 Aachen, Germany.
Baolei
B
Zhu
DWI-Leibniz-Institute for Interactive Materials, Forckenbeckstraße 50, 52074 Aachen, Germany.
Andreas
A
Walther
Dynamic Properties; Non-Equilibrium Self-Assembly; Programmable Materials; Self-Regulation; Switchable Materials; Time Domain