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Metal-organic species can be designed to self-assemble in large-scale,atomically defined, supramolecular architectures. Hybrid quantum wells, whereinorganic two-dimensional (2D) planes are separated by organic ligands, are aparticular example. The ligands effectively provide an intralayer confinementfor charge carriers resulting in a 2D electronic structure, even inmultilayered assemblies. Air-stable metal organic chalcogenides hybrid quantumwells have recently been found to host tightly bound 2D excitons with strongoptical anisotropy in a bulk matrix. Here, we investigate the excited carrierdynamics in the prototypical metal organic chalcogenide [AgSePh], disentanglingthree excitonic resonances by low temperature transient absorptionspectroscopy. Our analysis suggests a complex relaxation cascade comprisingultrafast screening and renormalization, inter-exciton relaxation, andself-trapping of excitons within few picoseconds. The ps-decay provided by theself-trapping mechanism may be leveraged to unlock the material's potential forultrafast optoelectronic applications.

Exciton self-trapping causes picoseconds recombination in metal-organic chalcogenides hybrid quantum wells