The results of room-temperature fluorescence lifetime measurements are reported for the excitation of J aggregates (Js) of pseudoisocyanine chloride (PIC-Cl) prepared in potassium polyvinyl sulfate (PVS) polymer thin films, their aqueous solutions, and NaCl aqueous solutions. Variations of the microscopic morphologies of the aggregates were investigated. The results show that fluorescence decay features correlated to the morphology change. The observed fluorescence lifetime and quantum efficiency of PIC J aggregates (PIC-Js) in a NaCl aqueous solution were 310 ps and 28%, respectively. The lifetime of the fibril-shaped macroaggregates prepared in PVS thin films was below the instrumental time resolution of 5 ps, and the efficiency decreased to below 3%. The results indicate that PIC-Js prepared with PVS polymers have an increased nonradiative contribution to the excitation deactivation process. In particular, macro-Js with isolated fibril-shaped structures revealed nonradiative pathway(s) that are closely associated to the specific packaging morphology of the constituent meso-Js. The possibility of a destructive effect on the formation of cavity-polaritons is also discussed.
Versatile novel implementations in microspectroscopy are developed, which can provide angle-resolved optical spectroscopy at local sample areas almost in diffraction limit. By selecting focus position of light flux incident within the back focal plane of the objective lens radially from the position of the optical axis of the microscope with employing off-centered pinhole, we can obtain parallel beam with oblique incidence and its angle tuning at the sample surface. In this paper, we describe our specific optical setup and its practical working principle in detail. We report, as a demonstration of its performance, our latest studies on optical properties of cavity polariton states in the so-called quantum microcavity structures, which contain molecular J-aggregates of pseudoisocyanine (PIC) dye as active working materials. By using the microscope technique, we obtain a fair amount of improvement in the linewidth observation of cavity polariton spectra.
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