Tunable Interlayer Delocalization of Excitons in Layered Organic–Inorganic Halide Perovskites

Chen, Yinan; Filip, Marina R.

doi:10.1021/acs.jpclett.3c02339

Title: Tunable Interlayer Delocalization of Excitons in Layered Organic–Inorganic Halide Perovskites

Journal Article · Mon Nov 20 00:00:00 EST 2023 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.3c02339· OSTI ID:2217264

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Department of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, U.K.

Layered organic–inorganic halide perovskites exhibit remarkable structural and chemical diversity and hold great promise for optoelectronic devices. In these materials, excitons are thought to be strongly confined within the inorganic metal halide layers with interlayer coupling generally suppressed by the organic cations. Here, we present an in-depth study of the energy and spatial distribution of the lowest-energy excitons in layered organic–inorganic halide perovskites from first-principles many-body perturbation theory, within the GW approximation and the Bethe–Salpeter equation. We find that the quasiparticle band structures, linear absorption spectra, and exciton binding energies depend strongly on the distance and the alignment of adjacent metal halide perovskite layers. Furthermore, we show that exciton delocalization can be modulated by tuning the interlayer distance and alignment, both parameters determined by the chemical composition and size of the organic cations. Our calculations establish the general intuition needed to engineer excitonic properties in novel halide perovskite nanostructures.

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Research Organization:: Univ. of Oxford (United Kingdom)

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

Grant/Contract Number:: AC02-5CH11231; AC02-05CH11231; AC05-00OR22725

OSTI ID:: 2217264

Alternate ID(s):: OSTI ID: 2228260

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Vol. 14 Journal Issue: 47; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Electrical conductivity
Excitons
Layered materials
Layers
Perovskites

Title: Tunable Interlayer Delocalization of Excitons in Layered Organic–Inorganic Halide Perovskites

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