(C16H28N)2SbCl5：一种新型无铅零维金属卤化物杂化物，具有亮橙色发射,Science China Materials

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(C16H28N)2SbCl5：一种新型无铅零维金属卤化物杂化物，具有亮橙色发射
Science China Materials ( IF 6.8 ) Pub Date : 2022-01-29 , DOI: 10.1007/s40843-021-1937-y
Hui Peng , Ye Tian , Zongmian Yu , Xinxin Wang , Bao Ke , Yueting Zhao , Tiantian Dong , Jianping Wang , Bingsuo Zou

零维 (0D) 金属卤化物因其迷人的光电特性而处于蓬勃发展的状态。在此，合成并研究了 (C16H28N)2SbCl5 的锑基金属卤化物（C16H28N+ = 苄基三丙基铵阳离子），其中分离的 [SbCl5]2- 簇被 C16H28N+ 包围以形成 0D 方形锥体结构。(C16H28N)2SbCl5 在低能辐照（400 nm）下在 633 nm 处显示出宽带橙色发射，具有接近统一的光致发光量子效率（97.8%）。有趣的是，(C16H28N)2SbCl5 在高能辐照（300 nm）后在 477 nm 处显示了一个额外的发射峰，这归因于自旋轨道耦合的双峰转变为两个独立的自陷激子（STE）。与温度相关的拉曼光谱清楚地揭示了多声子耦合的特征，表明 (C16H28N)2SbCl5 中存在强烈的非谐电子-声子相互作用。与温度相关的发射光谱和密度泛函理论结果表明，观察到的双波段发射源自 [SbCl5]2- 单元中的单重态和三重态 STE。结合(C16H28N)2SbCl5的高效发射和优异的稳定性，制备了具有96.6超高显色指数的稳定白光发光二极管。

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(C16H28N)2SbCl5: A new lead-free zero-dimensional metal-halide hybrid with bright orange emission

Zero-dimensional (0D) metal halides are in a blossoming status for their fascinating optoelectronic properties. Herein, an antimony-based metal halide of (C16H28N)2SbCl5 (C16H28N+ = benzyltripropylammonium cations), where the isolated [SbCl5]2− clusters are surrounded by C16H28N+ to form a 0D square-pyramidal structure, was synthesized and investigated. The (C16H28N)2SbCl5 exhibited a broadband orange emission at 633 nm upon the low-energy irradiation (400 nm) with a near-unity photoluminescence quantum efficiency (97.8%). Interestingly, (C16H28N)2SbCl5 showed an additional emission peak at 477 nm upon the higher-energy irradiation (300 nm), which is attributed to the transformation of the doublet of spin-orbit couplings into two independent self-trapped excitons (STEs). Temperature-dependent Raman spectra clearly revealed the characteristics of multi-phonon coupling, demonstrating a strong anharmonic electron-phonon interaction in (C16H28N)2SbCl5. Temperature-dependent emission spectra and density functional theory results illustrated that the observed dual-band emission originated from singlet and triplet STEs in [SbCl5]2− units. Combined with the efficient emission and excellent stability of (C16H28N)2SbCl5, a stable white-light-emitting diode with an ultra-high color rendering index of 96.6 was fabricated.

更新日期：2022-01-29

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