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Abstract Interactions between light and matter serve as the basis of many technologies, but the quality of these devices is inherently limited by the optical properties of their constituents. Plasmonic nanoparticles are a highly versatile and tunable platform for the enhancement of such optical properties. However, the near‐field nature of these effects has made thorough study and understanding of these mechanisms difficult. In this work, we introduce a fully confocal technique combining photoswitching super‐resolution microscopy with fluorescence lifetime imaging microscopy to study single‐molecule decay rate enhancement. We demonstrate that the technique combines a spatial resolution better than 20 nm, and a 16 ps temporal resolution. Simultaneously, an autocorrelation measurement is also performed to confirm that the data indeed originates from single molecules. This work provides insight into the various mechanisms of plasmon‐enhanced emission, and allows the study of the correlation between emission intensity and lifetime enhancement. This complicated relationship is shown to be dependent upon the relative influence of various radiative and nonradiative decay pathways. Here, we provide a platform for further study of emission mislocalization, the position‐dependent prominence of different decay pathways, and the direct super‐resolved measurement of the local density of states. 

Abstract The ability to reconfigure spin structure and spin‐photon interactions by an external electric field is a prerequisite for seamless integration of opto‐spintronics into modern electronics. In this study, the use of electric field on the tuning of circular photo galvanic effect in a quasi‐2D oxyhalide perovskite Bi₄NbO₈Cl is reported. The electrical transport measurements are applied to study the switching characteristics of the microsheet devices. The electric field is used to tune the nanoscale devices and an optical orientation approach is applied to understand the field‐tuned spin‐polarized band structures. It is found that the circular photogalvanic current can be erased and re‐created by poling, indicating the electric‐field‐based control over spin structure. The study enriches the basic understanding of the symmetry‐regulated optoelectronic response in ferroelectrics with spin‐orbit coupling.