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

Kastl, Christoph; Schwartzberg, Adam M.; Maserati, Lorenzo

doi:10.1021/acsnano.1c07281

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

Journal Article · 14 February 2022 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.1c07281 · OSTI ID:1812348

Kastl, Christoph ^[1]; Schwartzberg, Adam M. ^[2];

^[3]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Technical Univ. of Munich (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Center for Nano Science and Technology, Milan (Italy)

Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. Hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands, are a particular example. The ligands effectively provide an intralayer confinement for charge carriers resulting in a 2D electronic structure, even in multilayered assemblies. Air-stable metal organic chalcogenides hybrid quantum wells 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, inter-exciton relaxation, and self-trapping of excitons within few picoseconds. Finally, the ps-decay provided by the self-trapping mechanism may be leveraged to unlock the material's potential for ultrafast optoelectronic applications.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES), Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1812348

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 3 Vol. 16; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Picoseconds-Limited Exciton Recombination in Metal–Organic Chalcogenides Hybrid Quantum Wells

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