Toward Engineering Intrinsic Line Widths and Line Broadening in Perovskite Nanoplatelets

Perovskite nanoplatelets possess extremely narrow absorption and emission line widths, which are crucial characteristics for many optical applications. However, their underlying intrinsic and extrinsic line-broadening mechanisms are poorly understood. Here, we apply multidimensional coherent spectroscopy to determine the homogeneous line broadening of colloidal perovskite nanoplatelet ensembles. We demonstrate a dependence of not only their intrinsic line widths but also of various broadening mechanisms on platelet geometry. We find that decreasing nanoplatelet thickness by a single monolayer results in a 2-fold reduction of the inhomogeneous line width and a 3-fold reduction of the intrinsic homogeneous line width to the sub-millielectronvolts regime. In addition, our measurements suggest homogeneously broadened exciton resonances in two-layer (but not necessarily three-layer) nanoplatelets at room-temperature.