Harnessing Interfacial Phenomena at Self-Assembled Organic Ultrathin Films

拟议的研究旨在利用有组织的有机分子膜组件来开启，驱动和控制固/液界面的物理化学过程，以促进纳米技术的发展。更具体地说，表面限制的电荷转移相互作用和酶反应将被利用的（大）分子和纳米粒子的二维组装，其次，我们将研究纳米粒子表面曲率的自发组织和不混溶的有机吸附物的混合行为的影响。虽然酶催化反应和有机电子供体受体化合物是公认的概念，但它们在表面化学、分子组装或纳米光刻和纳米纤维中的应用相对较新且未开发。酶反应和电荷转移相互作用是潜在的有用工具。这些提供了对分子界面组装和材料加工的化学特定控制，并且可以在与软有机物质相容的温和条件下进行。拟议的研究还解决了知识赤字周围的作用，纳米结构上的组织和自组装单层膜中的化学基团的可折叠性。拟议的研究的预期成果是通过电刺激可逆地操纵分子和纳米颗粒在固/液界面的氧化还原响应相互作用，支持纳米纤维的有机表面的酶定向光刻，以及对分子相分离和受限几何形状的物理化学理解。

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.