LAUSR

Light matter interactions are greatly enhanced in two-dimensional (2D) semiconductors because of strong excitonic effects. Many optoelectronic applications would benefit from creating stacks of atomically thin 2D semiconductors separated by insulating barrier layers, forming multiquantum-well structures. However, most 2D transition metal chalcogenide systems require serial stacking to create van der Waals multilayers. Hybrid metal organic chalcogenolates (MOChas) are self-assembling hybrid materials that combine multiquantum-well properties with scalable chemical synthesis and air stability. In this work, we use spatially resolved linear and nonlinear optical spectroscopies over a range of temperatures to study the strongly excitonic optical properties of mithrene, that is, silver benzeneselenolate, and its synthetic isostructures. We experimentally probe s-type bright excitons and p-type excitonic dark states formed in the quantum confined 2D inorganic monolayers of silver selenide with exciton binding energy up to ∼0.4 eV, matching recent theoretical predictions of the material class. We further show that mithrene's highly efficient blue photoluminescence, ultrafast exciton radiative dynamics, as well as flexible tunability of molecular structure and optical properties demonstrate great potential of MOChas for constructing optoelectronic and quantum excitonic devices.