Hysteresis and Stochastic Fluorescence by Aggregated Ensembles of Graphene Quantum Dots.

"Blinking" behavior of fluorophores, being harmful for the majority of super-resolved techniques, turns into a key property for stochastic optical fluctuation imaging and its modifications, allowing one to look at the fluorophores already used in conventional microscopy, such as graphene quantum dots, from a completely new perspective. Here we discuss fluorescence of aggregated ensembles of graphene quantum dots structured at submicron scale. We study temperature dependence and stochastic character of emission. We show that considered quantum dots ensembles demonstrate rather complicated temperature-dependent intermittent emission, that is, "blinking" with a tendency to shorten "blinking" times with the increase of temperature. We verify "blinking" mechanism demonstrating hysteresis of the optical response under pulsed excitation timed to expected rates of dots transition to "dark" nonemitting states. Experimental results are well fitted by a simple qualitative model of transitions to the "dark" states. The obtained results suggest that this type of standardized quantum dots and even their submicron-size agglomerations can be useful as controlled fluorophores for super-resolution microscopy and, particularly, for SOFI-like microscopy.