Scanning exciton microscopy and single-molecule resolution and detection

摘要

Abstract: Subwavelength light sources have been constructed with the aid of luminescent and exciton transporting materials. These EXCITOR (exciton transmitted optical radiation) sources produce evanescent luminescence and can be used as scanning, light emitting tips of nanometer dimensions. They can also be used as scanning exciton donor tips. The theoretical resolution limit of this kind of near-field optical microscopy is on the atomic or molecular scale. The detection limit is a single molecule, but in contrast to other single molecule detection methods, this single molecule could be identified spatially as well as spectrally. Experimental examples of such an EXCITOR tip consist of gold or aluminum coated glass micropipettes with active crystal tips (anthracene, tetracene, perylene, etc.). Design considerations involve optical, excitonic, photochemical and mechanical properties of the luminescent point source. As it is scanned over a sample, it senses a variety of perturbations such as quenching or external heavy atom effects. It can also actively excite a luminescent probe. The latter process can be non-radiative (e.g., Forster) or may involve absorption and re-emission of evanescent luminescence. Spatially coupled emission and absorption processes are of both theoretical and practical interest. They open a way for reducing by many orders of magnitude the number of photons required to excite a single, isolated chromophore. Molecular exiton microscopy allows extention of near-field microscopy beyond the 50 nm limit already achieved and, thus, permits a new frontier of resolution with light based on the limits of energy transfer measurements. In essence, then, the goal of this research is a spectrally sensitive light microscope that will have the capability to zoom non-destructively and in air from the limits of resolution of lens-based confocal light microscopy (200 nm) to molecular dimensions of 1 nm.!