Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites
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...
| Main Authors: | , |
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| Format: | Journal article |
| Language: | English |
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American Chemical Society
2023
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| _version_ | 1797111709785128960 |
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| author | Chen, Y Filip, MR |
| author_facet | Chen, Y Filip, MR |
| author_sort | Chen, Y |
| collection | OXFORD |
| description | 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. |
| first_indexed | 2024-03-07T08:12:41Z |
| format | Journal article |
| id | oxford-uuid:706c52f5-c258-4152-a9be-765859add95b |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T08:12:41Z |
| publishDate | 2023 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:706c52f5-c258-4152-a9be-765859add95b2023-12-08T15:25:13ZTunable interlayer delocalization of excitons in layered organic-inorganic halide perovskitesJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:706c52f5-c258-4152-a9be-765859add95bEnglishSymplectic ElementsAmerican Chemical Society2023Chen, YFilip, MRLayered 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. |
| spellingShingle | Chen, Y Filip, MR Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title | Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title_full | Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title_fullStr | Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title_full_unstemmed | Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title_short | Tunable interlayer delocalization of excitons in layered organic-inorganic halide perovskites |
| title_sort | tunable interlayer delocalization of excitons in layered organic inorganic halide perovskites |
| work_keys_str_mv | AT cheny tunableinterlayerdelocalizationofexcitonsinlayeredorganicinorganichalideperovskites AT filipmr tunableinterlayerdelocalizationofexcitonsinlayeredorganicinorganichalideperovskites |