Issue 5, 2021

Tetrazine molecules as an efficient electronic diversion channel in 2D organic–inorganic perovskites

Abstract

Taking advantage of an innovative design concept for layered halide perovskites with active chromophores acting as organic spacers, we present here the synthesis of two novel two-dimensional (2D) hybrid organic–inorganic halide perovskites incorporating for the first time 100% of a photoactive tetrazine derivative as the organic component. Namely, the use of a heterocyclic ring containing a nitrogen proportion imparts a unique electronic structure to the organic component, with the lowest energy optical absorption in the blue region. The present compound, a tetrazine, presents several resonances between the organic and inorganic components, both in terms of single particle electronic levels and exciton states, providing the ideal playground to discuss charge and energy transfer mechanisms at the organic/inorganic interface. Photophysical studies along with hybrid time-dependent DFT simulations demonstrate partial energy transfer and rationalise the suppressed emission from the perovskite frame in terms of different energy-transfer diversion channels, potentially involving both singlet and triplet states of the organic spacer. Periodic DFT simulations also support the feasibility of electron transfer from the conduction band of the inorganic component to the LUMO of the spacer as a potential quenching mechanism, suggesting the coexistence and competition of charge and energy transfer mechanisms in these heterostructures. Our work proves the feasibility of inserting photoactive small rings in a 2D perovskite structure, meanwhile providing a robust frame to rationalize the electronic interactions between the semiconducting inorganic layer and organic chromophores, with the prospects of optimizing the organic moiety according to the envisaged application.

Graphical abstract: Tetrazine molecules as an efficient electronic diversion channel in 2D organic–inorganic perovskites

Supplementary files

Article information

Article type
Communication
Submitted
27 stu 2020
Accepted
08 ožu 2021
First published
09 ožu 2021

Mater. Horiz., 2021,8, 1547-1560

Tetrazine molecules as an efficient electronic diversion channel in 2D organic–inorganic perovskites

F. Lédée, P. Audebert, G. Trippé-Allard, L. Galmiche, D. Garrot, J. Marrot, J. Lauret, E. Deleporte, C. Katan, J. Even and C. Quarti, Mater. Horiz., 2021, 8, 1547 DOI: 10.1039/D0MH01904F

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