Chemical Sciences: Transient Nanopatterns by Biocatalytic Self-Assembly
Abstract:
Major Goals: It was the overall aim of this research program to develop transient nanoscale patterns that change their chemical information content and functionality over time with nanoscale resolution. To achieve this, we combined pioneering work from Riedo's Lab (thermochemical nanolithography TCNL) , and Ulijn's Lab (biocatalytic self-assembly). A major goal was to provide fundamental understanding and take concrete steps towards laboratory-based mimicry of fabrication approaches used by living systems. We achieved this by exploiting similar mechanisms used by living systems (catalytic amplification, self-assembly, structural confinement) but harness them as new tools for nanoscale fabrication, in non-biological contexts. Accomplishments: The objective of this collaborative grant between the labs of Rein Ulijn (CUNY) and Elisa Riedo (NYU) was to combine revolutionary nanoscale patterning with catalytic self-assembly to obtain spatiotemporal control of nanostructure formation and breakdown and consequent dynamic control of functionality. By using thermochemical scanning probe lithography (tSPL) we were able to precisely tune the film 3D topographical landscape simultaneously with surface chemistry. This provided control over positioning and concentration of surface-immobilized enzymes [1,2]. Furthermore, by making use of competing enzyme-catalyzed assembly and disassembly reactions, we could demonstrate the transient formation of nanoscale fibers that have programmable chemical content and (electronic) functionality, as well as time programmable assembly - disassembly behavior. We studied fundamental aspects of biocatalytic assembly at solid-liquid interfaces by using both synthetic and biological surfaces and particles.