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Ultrafast Dopant-Induced Exciton Auger-like Recombination in Mn-Doped Perovskite Nanocrystals
ACS Energy Letters ( IF 22.0 ) Pub Date : 2020-01-03 , DOI: 10.1021/acsenergylett.9b02678
Shiping Wang 1, 2 , Jing Leng 1 , Yanfeng Yin 1 , Junxue Liu 1 , Kaifeng Wu 1 , Shengye Jin 1
Affiliation  

Manganese(II)-doped perovskite nanocrystals (NCs), because of their unique dual-color (from host excitons and Mn-dopants) emission property, are promising materials for various optical applications. Because the excited state at Mn2+ is extremely long-lived, one or more host excitons coexisting with an excited Mn2+ can be generated in the same NC under continuous excitation, and the behavior of exciton in the presence of excited Mn2+ can determine the optical property of Mn-doped NCs. Herein, by using pump–pump–probe transient absorption spectroscopy, we show that, in Mn-doped CsPbCl3 NCs, the host exciton can undergo ultrafast nonradiative Auger-like recombination (τAug ≈ 12 ps) when coexisting with the excited state at Mn2+. Such fast Auger-like process competes with the exciton-to-dopant energy transfer (τIET ≈ 303 ps) and, thus, allows the Mn-dopant emission from only one Mn2+ site per NC at a time. This dopant-induced Auger-like recombination should correspond to the broadly observed excitation-dependent saturation of dopant emission in Mn-doped NCs, and also makes the Mn-doped NC a potential single photon emitter.

中文翻译:

锰掺杂钙钛矿纳米晶体中超快掺杂物诱导的激子似俄格复合。

锰(II)掺杂的钙钛矿纳米晶体(NCs)由于其独特的双色(来自主体激子和Mn掺杂剂)的发射特性,是用于各种光学应用的有前途的材料。由于Mn 2+处的激发态非常长寿,因此在连续激发下的同一NC中可以生成与激发的Mn 2+共存的一种或多种主体激子,并且在激发的Mn 2+存在下激子的行为可以确定Mn掺杂NC的光学性质。在本文中,通过使用泵-泵-探针瞬态吸收光谱,我们表明,在Mn掺杂CsPbCl 3 NCS,主机激子可以经历非辐射超快俄歇状重组(τ八月当与Mn 2+的激发态共存时(≈12 ps)。这种快速的俄歇式过程与激子到掺杂剂的能量转移(τIET≈303 ps)竞争,因此,每个NC一次只能从一个Mn 2+位点发射Mn掺杂剂。这种掺杂剂诱导的俄歇样重组应该对应于在Mn掺杂的NCs中广泛观察到的激发依赖的掺杂剂发射饱和,并且还使Mn掺杂的NC成为潜在的单光子发射体。
更新日期:2020-01-04
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