Investigation of nanoscale spatial heterogeneity in polymeric materials by using 3D single-molecule tracking techniques

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In this project, we have focused on constructing single-molecule imaging apparatuses with three-dimensional (3D) resolution for the investigation of spatial heterogeneity at the molecular level in polymeric materials. To achieve 3D localization, two approaches were employed. The first one is so-called the astigmatism imaging method, in which a cylindrical lens was inserted into the imaging system to modify the shape of the fluorescent image of a single molecule depending on Z-position. The second approach is a structured illumination with a periodic intensity modulation along the Z-axis due to the interference of two laser beams. These imaging apparatuses provided the 3D resolution of several tens of nanometers. By using the 3D super-resolution techniques, we have clarified the mechanism of anomalous diffusion of guest molecules in polymer films. In addition, we have also succeeded in the visualization of spatial heterogeneity in polymeric materials.