Exciton dissociation in 2D layered metal-halide perovskites

Angelica Simbula (), Luyan Wu, Federico Pitzalis, Riccardo Pau, Stefano Lai, Fang Liu, Selene Matta, Daniela Marongiu, Francesco Quochi, Michele Saba (), Andrea Mura and Giovanni Bongiovanni
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Angelica Simbula: Università degli Studi di Cagliari
Luyan Wu: Università degli Studi di Cagliari
Federico Pitzalis: Università degli Studi di Cagliari
Riccardo Pau: Università degli Studi di Cagliari
Stefano Lai: Università degli Studi di Cagliari
Fang Liu: Shanghai Jiao Tong University
Selene Matta: Università degli Studi di Cagliari
Daniela Marongiu: Università degli Studi di Cagliari
Francesco Quochi: Università degli Studi di Cagliari
Michele Saba: Università degli Studi di Cagliari
Andrea Mura: Università degli Studi di Cagliari
Giovanni Bongiovanni: Università degli Studi di Cagliari

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Layered 2D perovskites are making inroads as materials for photovoltaics and light emitting diodes, but their photophysics is still lively debated. Although their large exciton binding energies should hinder charge separation, significant evidence has been uncovered for an abundance of free carriers among optical excitations. Several explanations have been proposed, like exciton dissociation at grain boundaries or polaron formation, without clarifying yet if excitons form and then dissociate, or if the formation is prevented by competing relaxation processes. Here we address exciton stability in layered Ruddlesden-Popper PEA2PbI4 (PEA stands for phenethylammonium) both in form of thin film and single crystal, by resonant injection of cold excitons, whose dissociation is then probed with femtosecond differential transmission. We show the intrinsic nature of exciton dissociation in 2D layered perovskites, demonstrating that both 2D and 3D perovskites are free carrier semiconductors and their photophysics is described by a unique and universal framework.

Date: 2023
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DOI: 10.1038/s41467-023-39831-5

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