Journal
ACS NANO
Volume 16, Issue 3, Pages 3715-3722Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c07281
Keywords
hybrid semiconductors; metal-organic chalcogenides; transient absorption; two-dimensional excitons; self-trapping
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Funding
- Center for Novel Pathways to Quantum Coherence in Materials, Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]
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Metal-organic species can self-assemble into large-scale, atomically defined supramolecular architectures. In this study, the excited carrier dynamics in a prototypical metal-organic chalcogenide were investigated, revealing a complex relaxation cascade.
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](infinity), 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 psdecay provided by the self-trapping mechanism may be leveraged to unlock the material's potential for ultrafast optoelectronic applications.
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