AbstractLead-halide perovskites are highly promising for various optoelectronic applications, including laser devices. However, fundamental photophysics explaining the coherent-light emission from this material system is so intricate and often the subject of debate. Here, we systematically investigate photoluminescence properties of all-inorganic perovskite microcavity at room temperature and discuss the excited state and the light–matter coupling regime depending on excitation density. Angle-resolved photoluminescence clearly exhibits that the microcavity system shows a transition from weak coupling regime to strong coupling regime, revealing the increase in correlated electron–hole pairs. With pumping fluence above the threshold, the photoluminescence signal shows a lasing behavior with bosonic condensation characteristics, accompanied by long-range phase coherence. The excitation density required for the lasing behavior, however, is found to exceed the Mott density, excluding the exciton as the excited state. These results demonstrate that the polaritonic Bardeen–Cooper–Schrieffer state originates the strong coupling formation and the lasing behavior.
Ultrafast carrier interactions in metal-halide perovskites probed with two-dimensional electronic spectroscopy
