Harnessing Interfacial Phenomena at Self-Assembled Organic Ultrathin Films

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The proposed research is aimed at harnessing organized, organic, molecular film assemblies to switch on, drive, and control physicochemical processes at solid/liquid interfaces in ways that will facilitate the development of nanotechnologies. More specifically, surface-confined charge-transfer interactions and enzyme reactions will be exploited for the two-dimensional assembly of (macro-)molecules and nanoparticles, and secondly, we will examine the effect of nanoparticle surface curvature on the spontaneous organization and mixing behavior of immiscible organic adsorbates. While enzyme-catalyzed reactions and organic electron-donor-acceptor compounds are well-established concepts, their application in surface chemistry, molecular assembly or nanolithography and nanofabrication is relatively new and undeveloped. Enzyme reactions and charge-transfer interactions are potentially useful tools. These offer chemically specific control over the interfacial assembly of molecules and processing of materials and can be carried out under mild conditions that are compatible with soft organic matter. The proposed research also addresses the knowledge deficit surrounding the role that nanostructure plays on the organization and miscibility of chemical groups in self-assembled monolayer films. The expected outcomes of the proposed research are redox-responsive interactions for reversibly manipulating molecules and nanoparticles at solid/liquid interfaces via electrical stimuli, enzyme-directed lithography of organic surfaces in support of nanofabrication, as well as a physicochemical understanding of molecular phase separation and miscibility in confined geometries.