Picoseconds-Limited Exciton Recombination in Metal–Organic Chalcogenides Hybrid Quantum Wells

Metal–organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. A particular example is hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands. The ligands effectively form an intralayer confinement...

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Bibliographic Details
Published in:ACS nano 2022-03, Vol.16 (3), p.3715-3722
Main Authors: Kastl, Christoph, Schwartzberg, Adam M, Maserati, Lorenzo
Format: Article
Language:English
Subjects:
2D excitons
absorption
absorption spectroscopy
electrical conductivity
excitons
hybrid quantum wells
hybrid semiconductors
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
light absorption
metal-organic chalcogenides
metal−organic chalcogenides
nanomaterials
self-trapping
transient absorption
two-dimensional excitons
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Summary:Metal–organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. A particular example is hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands. The ligands effectively form an intralayer confinement for charge carriers resulting in a 2D electronic structure, even in multilayered assemblies. Air-stable layered transition metal organic chalcogenides have recently been found to host tightly bound 2D excitons with strong optical anisotropy in a bulk matrix. Here, we investigate the excited carrier dynamics in the prototypical metal–organic chalcogenide [AgSePh]∞, disentangling three excitonic resonances by low temperature transient absorption spectroscopy. Our analysis suggests a complex relaxation cascade comprising ultrafast screening and renormalization, interexciton relaxation, and self-trapping of excitons within a few picoseconds (ps). The ps-decay provided by the self-trapping mechanism may be leveraged to unlock the material’s potential for ultrafast optoelectronic applications.
ISSN:1936-0851
1936-086X
DOI:10.1021/acsnano.1c07281