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Donor-acceptor discrete optical emission in 2D perovskites

Two-dimensional (2D) van der Waals nanomaterials have attracted considerable attention for potential use in photonic and optoelectronic applications in the nanoscale, due to their outstanding electrical and optical properties, differing from their bulk state. Currently, 2D perovskite belonging to this group of nanomaterials is widely studied for a wide range of optoelectronic applications. Thanks to their excitonic properties, 2D perovskites are also promising materials for photonics and nonlinear devices working at room temperature. Nevertheless, strong excitonic effects can reduce the photocurrent characteristics when using thinner perovskites phases. In this work, we present solid experimental evidence for the presence of single donor-acceptor pair optical transitions in 2D Lead Halide Perovskites, characterized by sub meV linewidths ($\simeq 120 μeV$) and long decay times (5-8 ns). Micro-photoluminescence evidence is supported by detailed Photoemission measurements, and a model simulation. The association of Phenethylammonium with Methylammonium cations, the latter molecule being only present in 2D Halide Perovskites with thicker phases $n \geq 2$, has been identified as the source of the donor-acceptor pair formation, corresponding to the displacement of lead atoms and their replacement by methylamonium. Our seminal study of discrete Donor-Acceptor Pair (DAP) sharp and bright optical transitions in 2D Lead Halide Perovskites opens new routes to implement DAP as the carrier sources for novel designs of optoelectronic devices with 2D perovskites, and will foster the development of future outstanding properties in non-linear quantum technologies.