Reznik Carmen, Berg Rosalie, Foster Ed, Advincula Rigoberto, Landes Christy F
Rice University, Houston, Texas 77005.
University of Houston, Houston, Texas 77204.
J Phys Chem Lett. 2011 Mar 17;2(6). doi: 10.1021/jz200065f.
Single-molecule fluorescence spectroscopy is employed to reveal 3-dimensional details of the mechanisms underpinning ion transport in a polyelectrolyte thin film possessing polymer-brush nanoscale order. The ability to resolve fluorescence emission over three discrete polarization angles reveals that these ordered materials impart 3-dimensional orientation to charged, diffusing molecules. The experiments, supported by simulations, report global orientation parameters for molecular transport, track dipole angle progressions over time, and identify a unique transport mechanism: translational diffusion with restricted rotation. Generally, realization of this experimental method for translational diffusion in systems exhibiting basic orientation should lend itself to evaluation of transport in a variety of important, ordered, functional materials.
单分子荧光光谱法用于揭示具有聚合物刷纳米级有序结构的聚电解质薄膜中离子传输机制的三维细节。通过在三个离散偏振角上解析荧光发射的能力表明,这些有序材料赋予带电扩散分子三维取向。在模拟的支持下,实验报告了分子传输的全局取向参数,追踪了偶极角随时间的变化,并确定了一种独特的传输机制:受限旋转的平移扩散。一般来说,在具有基本取向的系统中实现这种平移扩散的实验方法,应有助于评估各种重要的、有序的、功能性材料中的传输。