posted on 2022-01-22, 00:29authored byRui Chen, Krishnendu Das, Maria A. Cardona, Luca Gabrielli, Leonard J. Prins
Cellular functions
are regulated with high spatial control through
the local activation of chemical processes in a complex inhomogeneous
matrix. The development of synthetic macroscopic systems with a similar
capacity allows fundamental studies aimed at understanding the relationship
between local molecular events and the emergence of functional properties
at the macroscopic level. Here, we show that a kinetically stable
inhomogeneous hydrogel matrix is spontaneously formed upon the local
injection of ATP. Locally, ATP templates the self-assembly of amphiphiles
into large nanoreactors with a much lower diffusion rate compared
to unassembled amphiphiles. The local depletion of unassembled amphiphiles
near the injection point installs a concentration gradient along which
unassembled amphiphiles diffuse from the surroundings to the center.
This allows for a progressive local accumulation of self-assembled
nanoreactors in the matrix upon repetitive cycles of ATP injection
separated by time intervals during which diffusion of unassembled
amphiphiles takes place. Contrary to the homogeneous matrix containing
the same components, in the inhomogeneous matrix the local upregulation
of a chemical reaction occurs. Depending on the way the same amount
of injected ATP is administered to the hydrogel matrix different macroscopic
distributions of nanoreactors are obtained, which affect the location
in the matrix where the chemical reaction is upregulated.