Mn2+ 激活的零维金属（Cd、Zn）卤化物杂化物，具有近乎统一的 PLQY 和零热淬火,The Journal of Physical Chemistry C

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Mn2+ 激活的零维金属（Cd、Zn）卤化物杂化物，具有近乎统一的 PLQY 和零热淬火
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-04-30 , DOI: 10.1021/acs.jpcc.2c08264
Jumana Hasin Marayathungal ₁ , Deep Kumar Das ₁ , Rangarajan Bakthavatsalam ₁ , Jisvin Sam ₁ , Venkatesha R. Hathwar ₂ , Raghavaiah Pallepogu ₃ , Sudipta Dutta ₁ , Janardan Kundu ₁

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低维卤化锑杂化物中基于高发光自陷激子 (STE) 的发射通常会遭受严重的热猝灭，这限制了它们在照明应用中的使用。有趣的是，Mn ²⁺激活的低维金属卤化物杂化物具有其特有的 d-d 跃迁，不易受热淬火的影响。因此，开发具有高 PLQY 和零热淬灭的 Mn ²⁺活化金属卤化物杂化物已受到越来越多的研究努力。在此，我们合成了Mn ²⁺掺杂的零维金属(Cd ²⁺ , Zn ²⁺) 溴化物杂化物利用 DABCO（1,4-二氮杂双环 [2.2.2] 辛烷）作为有机阳离子。结构分析证实了主体金属 (Cd, Zn) 卤化物杂化物中存在替代掺杂剂 (Mn ^{2+ )。}光学上，Mn ²⁺掺杂的 Cd 系统 (C ₆ H ₁₄ N ₂ Cd _0.94 Mn _0.06 Br ₄ H ₂ O) 显示 (i) 双发射带（由于四面体 Mn 中心的绿色发射和由于主体 STE 的橙色发射），(ii) 能量从掺杂剂转移到主体 (Mn → Cd) 的有力证据，以及 (iii) 零热淬灭行为，尽管 PLQY 较低。另一方面，Mn ²⁺掺杂的Zn杂化物（C ₆H ₁₄ N ₂ Zn _0.81 Mn _0.19 Br ₄ ) 展示了具有高发光 (PLQY ∼ 94%) 绿光发射（四面体 Mn 中心）和零热猝灭行为的稳健光学特性。^{Mn 2+}激活的金属卤化物杂化物的这种强发光零热猝灭行为可以为寻找用于高温照明应用的新功能材料铺平道路。

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Mn2+-Activated Zero-Dimensional Metal (Cd, Zn) Halide Hybrids with Near-Unity PLQY and Zero Thermal Quenching

Highly luminescent self-trapped exciton (STE)-based emission in low-dimensional antimony halide hybrids typically suffers from severe thermal quenching that limits their use in lighting applications. Interestingly, Mn²⁺-activated low-dimensional metal halide hybrids, with their characteristic d–d transitions, are less susceptible to thermal quenching. Consequently, developing Mn²⁺-activated metal halide hybrids with high PLQY and zero thermal quenching has received increasing research efforts. Herein, we synthesized Mn²⁺-doped zero-dimensional metal (Cd²⁺, Zn²⁺) bromide hybrids utilizing DABCO (1,4-diazabicyclo[2.2.2]octane) as the organic cation. Structural analysis confirms the presence of substitutional dopants (Mn²⁺) in the host metal (Cd, Zn) halide hybrids. Optically, the Mn²⁺-doped Cd system (C₆H₁₄N₂Cd_0.94Mn_0.06Br₄H₂O) shows (i) dual emission bands (green emission due to tetrahedral Mn center and orange emission due to host STEs), (ii) strong evidence of energy transfer from dopants to host (Mn → Cd), and (iii) zero thermal quenching behavior albeit with low PLQY. On the other hand, Mn²⁺-doped Zn hybrids (C₆H₁₄N₂Zn_0.81Mn_0.19Br₄) demonstrate robust optical properties with highly luminescent (PLQY ∼ 94%) green emission (tetrahedral Mn center) and zero thermal quenching behavior. Such strongly luminescent zero thermal quenching behavior of Mn²⁺-activated metal halide hybrids could pave the way for the search for new functional materials for their use in high-temperature lighting applications.

更新日期：2023-04-30

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