Mn4+ 激活的 Ca7Mg2Ga6−yAlyO18:Mn4+ 荧光粉中结构限制诱导的高效深红光发射和负热猝灭性能,Inorganic Chemistry Frontiers

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Mn4+ 激活的 Ca7Mg2Ga6−yAlyO18:Mn4+ 荧光粉中结构限制诱导的高效深红光发射和负热猝灭性能
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2023-03-31 , DOI: 10.1039/d3qi00252g
Jinmei Huang ₁ , Pengfei Jiang ₁ , Zien Cheng ₁ , Rong Wang ₂ , Rihong Cong ₁ , Tao Yang ₁

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高量子效率（QE）和热稳定发射对于荧光粉的应用是必不可少的。由于Mn ⁴⁺的晶格和裸d轨道之间的强耦合，Mn ⁴⁺激活氧化物红色荧光粉通常表现出低QE和严重的热猝灭（TQ），这严重限制了它们的应用前景。在此，我们合理设计了一种新型荧光粉系列Ca ₇ Mg ₂ Ga _{6− y} Al _y O ₁₈ :0.02Mn ⁴⁺ (CMGA _y O:Mn ⁴⁺ , 0 ≤ y ≤ 1.5)，它采用了高结构对称性的空间群F432.通过在结构上将 Mn ⁴⁺发射中心限制在孤立的八面体配位点，同时实现了高效和热稳定的深红色发射（λ _{em = 721 nm）。}具体而言，由于 Al ³⁺合金化诱导的局部结构修改和非辐射跃迁的抑制，CMGA _1.5 O:Mn ⁴⁺分别获得了 90.2 和 75.9% 的最高内部和外部量子效率。对于 CMGA _y O:Mn ⁴⁺和y= 0、0.5 和 1.5，分别。CMGA _0.5 O:Mn ⁴⁺在测量温度范围 (298–473 K) 内表现出异常的负 TQ 行为，这归因于通过孤立的 MnO ₆八面体的电子-声子相互作用获得的能量。此外， CMGO:0.02Mn ⁴⁺的原位高压发射光谱显示发射位置对外部压力高度敏感，不同压力区域的红移系数分别为2.8(2)和1.16(4) nm GPa ^{-1 。}_{CMGA y} O:Mn ⁴⁺这些优异的光致发光特性荧光粉在红色 LED 和光学压力传感器方面具有巨大的应用潜力。这项工作的发现为设计高性能 Mn ⁴⁺激活的荧光粉铺平了道路。

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Structural confinement-induced highly efficient deep-red emission and negative thermal quenching performance in Mn4+-activated Ca7Mg2Ga6−yAlyO18:Mn4+ phosphors

High quantum efficiency (QE) and thermally stable emission are indispensable for the application of phosphors. Owing to the strong coupling between the lattice and naked d-orbitals of Mn⁴⁺, Mn⁴⁺-activated oxide red-emitting phosphors usually exhibit a low QE and serious thermal quenching (TQ), which strictly inhibit their prospective application. Herein, we rationally designed a novel phosphor series Ca₇Mg₂Ga_6−yAl_yO₁₈:0.02Mn⁴⁺ (CMGA_yO:Mn⁴⁺, 0 ≤ y ≤ 1.5), which adopts a high structural symmetry of the space group F432. Highly efficient and thermally stable deep-red emissions (λ_em = 721 nm) were achieved simultaneously by structurally confining the Mn⁴⁺-emitting centres at the isolated octahedrally coordinated sites. Specifically, the highest internal and external quantum efficiencies of 90.2 and 75.9%, respectively, were obtained for CMGA_1.5O:Mn⁴⁺ due to Al³⁺-alloying-induced local structure modification and suppression of non-radiative transitions. Excellent thermal stabilities of 99, 102.2, and 87.9% of room-temperature photoluminescence intensities were retained at 423 K for CMGA_yO:Mn⁴⁺ with y = 0, 0.5, and 1.5, respectively. CMGA_0.5O:Mn⁴⁺ exhibits an abnormal negative TQ behaviour over the measured temperature range (298–473 K), which is attributed to the energy gain via the electron–phonon interactions of the isolated MnO₆ octahedra. Moreover, in situ high-pressure emission spectra of CMGO:0.02Mn⁴⁺ showed that the emission position is highly sensitive to the external pressure with redshift coefficients of 2.8(2) and 1.16(4) nm GPa⁻¹ in different pressure regions. These excellent photoluminescence properties of CMGA_yO:Mn⁴⁺ phosphors signify their great application potential in red LEDs and optical pressure sensors. The findings of this work have paved an avenue for the design of high-performance Mn⁴⁺-activated phosphors.

更新日期：2023-03-31

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