Pressure-Engineered Optical and Charge Transport Properties of Mn2+/Cu2+ Codoped CsPbCl3 Perovskite Nanocrystals via Structural Progression
Pressure-Engineered Optical and Charge Transport Properties of Mn2+/Cu2+ Codoped CsPbCl3 Perovskite Nanocrystals via Structural Progression
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通过结构进展压力工程设计 Mn2/Cu2 共掺杂 CsPbCl3 钙钛矿纳米晶体的光学和电荷传输性能
DOI：
10.1021/acsami.0c15068
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发表时间：
2020
影响因子：
9.5
通讯作者：
Yang Jinghai
中科院分区：
文献类型：
--
作者：
Zhang Junkai;Zheng Yuzhu;Liu Guangtao;Ma Yanzhang;Gong Lei;Guan Renquan;Cui Xiaoyan;Yan Jiejuan;Zhao Jialong;Yang Jinghai
在这项工作中，与相应的纯cspbcl3纳米晶体（nc）和Mn2+掺杂cspbcl3nc相比，Mn2+/Cu2+共掺杂cspbcl3nc具有更好的光致发光（PL）和光致发光量子产率（PL QYs）（57.6%），延长了PL寿命（1.78 ms），提高了热耐受性（523 K），这是由于添加CuCl2诱导的高效Mn2+掺杂（3.66%）。此外，我们对Mn2+/Cu2+共掺杂的cspbcl3nc施加压力，发现光致发光的红移后蓝移是由带隙演化引起的，与结构相从立方向正交相转变有关。此外，我们还发现在523 K的预热条件下，这种相变表现出明显的形态不变性，并伴随着电导率的显著提高。对经过高温处理的产品施加的压力增大了电学差异，并且由于包装更紧密，容易使界面加强。有趣的是，当施加的压力为2.9 GPa时，在退火的nc中观察到缺陷引发的离子和电子混合导电（MIEC）。压力相关的离子传导与局部纳米晶体非晶化和偏应力的增加密切相关，这在阻抗谱中得到了清晰的描述。最后，与未施加压力的产品相比，回收的产品具有更好的电导率（提高了5-6倍）和更强的光电响应。我们的发现不仅揭示了cspbx3在结构上的压力调谐光学和电学性质，而且为更多非晶全无机cspbx3的光电应用开辟了有前途的探索。
In this work, compared with the corresponding pure CsPbCl3nanocrystals (NCs) and Mn2+-doped CsPbCl3NCs, Mn2+/Cu2+-codoped CsPbCl3NCs exhibited improved photoluminescence (PL) and photoluminescence quantum yields (PL QYs) (57.6%), prolonged PL lifetimes (1.78 ms), and enhanced thermal endurance (523 K) as a result of efficient Mn2+doping (3.66%) induced by the addition of CuCl2. Furthermore, we applied pressure on Mn2+/Cu2+-codoped CsPbCl3NCs to reveal that a red shift of photoluminescence followed by a blue shift was caused by band gap evolution and related to the structural phase transition from cubic to orthorhombic. Moreover, we also found that under the preheating condition of 523 K, such phase transition exhibited obvious morphological invariance, accompanied by significantly enhanced conductivity. The pressure applied to the products treated with high temperature enlarged the electrical difference and easily intensified the interface by closer packaging. Interestingly, defect-triggered mixed ionic and electronic conducting (MIEC) was observed in annealed NCs when the applied pressure was 2.9 GPa. The pressure-dependent ionic conduction was closely related to local nanocrystal amorphization and increased deviatoric stress, as clearly described byin situimpedance spectra. Finally, retrieved products exhibited better conductivity (improved by 5–6 times) and enhanced photoelectric response than those when pressure was not applied. Our findings not only reveal the pressure-tuned optical and electrical propertiesviastructural progression but also open up the promising exploration of more amorphous all-inorganic CsPbX3-based photoelectric applications.