Advancements in material science and microscopy has allowed for the interrogation of single-emitter fluorescence for the better part of two decades, leading to advances in many areas including bio-imaging, super-resolution imaging techniques, and photonics. However, many aspects of SM phenomena are not yet fully understood, for example, fluorescence intermittency or the observation of telegraph-like switches in emission intensities (commonly referred to as “blinking”) is a most ubiquitous phenomena observed in SM measurements. We have been studying organic dye molecules imbedded in crystalline hosts as a exciting and advantageous SM system, quantifying their photophysical kinetic dispersion observed over ten orders of magnitude. My efforts are to develop new methods of SM collection and analysis to illuminate their underlying physical and chemical mechanisms, unraveling the rich photophysical behaviors exhibited by these most unique systems.