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Ferroelectric order driven Eu³⁺ photoluminescence in BaZr_xTi_1-xO₃ perovskite.

ABSTRACT: The ability to tune and enhance the properties of luminescent materials is essential for enlarging their application potential. Recently, the modulation of the photoluminescence emission of lanthanide-doped ferroelectric perovskites by applying an electric field has been reported. Herein, we show that the ferroelectric order and, more generally the polar order, has a direct effect on the photoluminescence of Eu³⁺ in the model BaZr_xTi_1-xO₃ perovskite even in the absence of an external field. The dipole arrangement evolves with increasing x from long-range ferroelectric order to short-range order typical of relaxors until the non-polar paraelectric BaZrO₃ is achieved. The cooperative polar interactions existing in the lattice (x < 1) promote the off-center displacement of the Eu³⁺ ion determining a change of the lanthanide site symmetry and, consequently, an abrupt variation of the photoluminescence emission with temperature. Each type of polar order is characterized by a distinct photoluminescence behaviour.

SUBMITTER: Canu G

PROVIDER: S-EPMC6478923 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Materials with optical multifunctionality such as photoluminescence (PL), radioluminescence, and thermoluminescence (TL) are a boon for a sustainable society. BaHfO3 (barium hafnium oxide [BHO]) under UV irradiation demonstrated visible PL endowed by oxygen vacancies (OVs). Eu3+ doping in BHO (BHOE) introduces f-state impurity levels just below the conduction band for both Eu@Ba and Eu@Hf sites, causing efficient host-to-dopant energy transfer, generating intense 5D0 → 7F1 magnetic dipole transitions (MDT) with internal quantum yield of ∼70%. X-ray photoelectron spectroscopy and electron paramagnetic resonance showed the formation of OVs in both BHO and BHOE samples with more vacancies in the doped sample. The positron lifetime measurements suggested that Eu3+ ions are distributed at both Ba2+ and Hf4+ sites. The association of OVs with Hf4+ and Eu3+ ions due to high charge/radius ratio is considered to be responsible for lowering the symmetry around Eu3+ ions to C 4v in BHOE. Density functional theory studies of defect formation energy justified the same. Time-resolved emission spectroscopy showed distinct spectra for Eu@Ba and Eu@Hf sites corresponding to symmetric and asymmetric environments, respectively. This could be highly relevant in designing color tunable phosphor by forcing dopant ions at one specific site because Eu@Ba displayed orange emission whereas Eu@Hf displayed red emission. We could further harness BHOE for X-ray scintillator application by designing a thin film, which showed efficient conversion of high-energy X-ray into visible light. Under beta irradiation; both BHO and BHOE showed distinct TL glow curves as shallow traps were formed in the former and deep traps in the latter, which could have long-term implications in harnessing this material for persistent luminescence. We believe that BHO/BHOE demonstrated an extraordinary credential as a perovskite for multifunctional applications in the area of defect-induced light emission, UV phosphor, X-ray scintillator, and TL crystals.

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Ferroelectric order driven Eu³⁺ photoluminescence in BaZr_xTi_1-xO₃ perovskite.

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Ferroelectric order driven Eu³⁺ photoluminescence in BaZr_xTi_1-xO₃ perovskite.