Layer Dependence of Excitonic Properties in 2D Hybrid Metal Organic Chalcogenolates

Rapidly expanding integration of semiconductors in consumer electronics up through large-scale supercomputers necessitates substantial quantum and production efficiency improvements to reduce global electricity consumption. 2D semiconductors, like transition metal dichalcogenides (TMDs) and 2D lead halide perovskites (LHPs), have emerged in recent years as strong contenders over silicon and other bulk semiconductors due to their strong exciton binding energies and highly tunable properties.<br/>We investigate metal organic chalcogenolates (MOCs) as 2D semiconductors that can improve upon these existing structures—for example, the layer dependence of TMDs and instability of metal halide perovskites. MOCs are a novel class of van der Waals stacked hybrid organic-inorganic semiconductors with extreme 1D quantum confinement, in-plane anisotropy, and strong exciton-lattice interaction. Moreover, unlike TMDs and 2D LHPs, MOCs feature covalent bonding between organic and inorganic components, providing strong environmental stability while also allowing for bandgap tunability through organic functionalization. These properties are promising for applications as light emitting diodes (LEDs), excitonic switches, and a variety of other optoelectronic devices. Silver phenylselenolate, AgSePh, is a MOC of particular interest due to its narrow, natively blue emission (~467 nm). However, its excited state dynamics are still dominated by unknown nonradiative recombination mechanisms, limiting its potential to revolutionize future semiconductor frameworks. This work details layer dependence studies that determine the susceptibility of individual MOC layers to one another and their environment to elucidate the intrinsic light-matter interaction of this hybrid material class.