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Layered Perovskite Doping with Eu³⁺ and β-diketonate Eu³⁺ Complex.

ABSTRACT: Metal halide perovskites are attracting great interest for the fabrication of light-emitting devices encompassing light-emitting diodes, lasers, and scintillators. As the field develops, perovskite doping emerges as a promising way to enrich the material functionalities and enhance the luminescence yield and tunability. While Mn⁺² addition has been well explored, doping with lanthanides has received less attention, even though their intense and line-like luminescence is interesting for a wide range of applications. In this work, we study the doping of NMA₂PbBr₄ layered perovskites with Eu³⁺ and Eu³⁺ tetrakis β-diketonate complex. By exploiting the antenna effect of the naphthalene-based functional cation (NMA = 1-naphtylmethylammonium), direct sensitization of Eu³⁺ is obtained; nevertheless, it is not very efficient due to the non-optimal energy level alignment with the resonance acceptor level of the lanthanide. Protection of Eu³⁺ in the form of tetrakis β-diketonate complex grants a more ideal coordination geometry and energetic landscape for the energy transfer to europium in the perovskite matrix, allowing for a nearly 30-fold improvement in luminescence yield. This work sets the basis for new synthetic strategies for the design of functional perovskite/lanthanide host-guest systems with improved luminescence properties.

SUBMITTER: Cortecchia D

PROVIDER: S-EPMC8043125 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Tris{6,6,7,7,8,8,8-heptafluoro-1-[2-(9,9-dimethylfluorenyl)]-1,3-octanedionate} europium(III) (Eu(III)(hfod)3 1) was synthesized, which was designed to have low luminescence and a large absorption coefficient in order to elucidate the coordination effects of phosphine oxide ligands. The quantum yield (ΦTOT) and photoluminescence intensity of complex 1 were dramatically enhanced by coordinating a diphenyl-4-(dibutylphosphinyl)butyl phosphine oxide (DPDB) ligand, thanks to the increased intrinsic photoluminescence quantum yield of the lanthanide (ΦLn) and the increased energy transfer efficiency (ΦET) in the solution and solid states. In the solid state, there was no energy dissipation by solvent molecules. This excluded the steric shielding effects of the DPDB ligand and allowed the effects of the ligand field environment to be extracted. ΦLn and ΦET of complex 2 were much larger in the solid state than those in the solution state, resulting in larger ΦTOT (solution state: ΦLn 0.50, ΦET 0.42, and ΦTOT 0.21 and solid state: ΦLn 0.74, ΦET 0.47, and ΦTOT 0.35). Larger asymmetry ratios (ratio R) of Eu(III)(hfod)3(DPDB) 2 than those of complex 1 in the solution and solid states indicate that the ligand field of the Eu(III) ion becomes more asymmetric by coordination of the DPDB ligand. Density functional theory calculations showed that ΦLn and ΦET increased when the ligand field around the Eu(III) ion became more asymmetric. Based on these results, we propose a hypothesis on the enhancement of the photoluminescence intensity of 6-coordinated Eu(III)-β-diketonate by a DPDB ligand. When a DPDB ligand coordinates to a Eu(III) ion, the positions of the nearest oxygen atoms around the Eu(III) ion are shifted by steric repulsion and the relative positions of the nearest oxygen atoms are distorted. The distorted coordination environment induces asymmetry in the ligand field, increasing ΦLn and ΦET. ΦTOT is enhanced by the DPDB ligand because it is the product of ΦLn and ΦET. Photoluminescence intensity increases because of the enhanced ΦTOT.

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Layered Perovskite Doping with Eu³⁺ and β-diketonate Eu³⁺ Complex.

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