Room Temperature Single-Photon Emission from Individual Perovskite Quantum Dots

Abstract

Lead-halide-based perovskites have been the subject of numerous recent studies largely motivated by their exceptional performance in solar cells. Electronic and optical properties of these materials have been commonly controlled by varying the composition (<i>e.g.</i>, the halide component) and/or crystal structure. Use of nanostructured forms of perovskites can provide additional means for tailoring their functionalities <i>via</i> effects of quantum confinement and wave function engineering. Furthermore, it may enable applications that explicitly rely on the quantum nature of electronic excitations. Here, we demonstrate that CsPbX₃ quantum dots (X = I, Br) can serve as room-temperature sources of quantum light, as indicated by strong photon antibunching detected in single-dot photoluminescence measurements. We explain this observation by the presence of fast nonradiative Auger recombination, which renders multiexciton states virtually nonemissive and limits the fraction of photon coincidence events to ∼6% on average. We analyze limitations of these quantum dots associated with irreversible photodegradation and fluctuations (“blinking”) of the photoluminescence intensity. On the basis of emission intensity-lifetime correlations, we assign the “blinking” behavior to random charging/discharging of the quantum dot driven by photoassisted ionization. This study suggests that perovskite quantum dots hold significant promise for applications such as quantum emitters; however, to realize this goal, one must resolve the problems of photochemical stability and photocharging. These problems are largely similar to those of more traditional quantum dots and, hopefully, can be successfully resolved using advanced methodologies developed over the years in the field of colloidal nanostructures.