Enhancing optical properties and stability of cesium lead halide quantum dots through nickel substitution and ligand change

S. Y. Kim, Ho Won Jang
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Abstract

In this study, we investigated the methods for prolonged lifetime in the CsPbX3 (X: Cl, Br, I) structured perovskite materials. First, the changes in structural and optical properties were compared by doping Ni in the CsPbBr3 quantum dots (QDs). The steady-state photoluminescence (PL) intensity of Ni-doped QDs shows 3.8 times increase comparing with undoped QDs. CsPbBr3 without nickel had a quantum efficiency of only 56.7 %, whereas CsPbBr3 doped with nickel had a quantum efficiency of 82.9 %. It was found that the doped divalent element acts as a defect in the perovskite structure, reducing the recombination rate of electrons and holes. After 48 hours UV-light irradiation, PL intensity of CsPbBr3 decreased about 70 % while that of Ni-substituted CsPbBr3 QDs decreased only 18 %, indicating the prolonged stability against UV-light irradiation. Furthermore, Ni-substituted CsPbBr3 QDs shows higher stability against temperature and moisture. These results confirmed that Ni substitution method is effective to increase the stability of CsPbX3 QDs. Second, we used sulfuroleylamine (S-OLA) complex which was utilized to etch the defect-rich surface of the CsPbI3 QDs and then self-assembly to form a matrix outside the CsPbI3 QDs protected the QDs from environmental moisture and solar irradiation. The PL intensity of the CsPbI3 QDs increased by 21% of its initial value. There was a significant increase in the colloidal stability of the CsPbI3 QDs. The introduction of S-OLA induced the recovery of the lost photoluminescence of the nonluminous aged CsPbI3 QDs with time to 95% of that of the fresh QDs. Furthermore, the PL was maintained for one month. The increase in the stability and PL intensity are critical for realizing high-performance perovskite-QD-based devices. In this study, we investigated the methods for prolonged lifetime in the CsPbX3 (X: Cl, Br, I) structured perovskite materials. First, the changes in structural and optical properties were compared by doping Ni in the CsPbBr3 quantum dots (QDs). It was found that the doped divalent element acts as a defect in the perovskite structure, reducing the recombination rate of electrons and holes. Ni-substituted CsPbBr3 QDs shows higher stability against temperature and moisture. These results confirmed that Ni substitution method is effective to increase the stability of CsPbX3 QDs. Second, we used sulfuroleylamine (S-OLA) complex which was utilized to etch the defect-rich surface of the CsPbI3 QDs and then self-assembly to form a matrix outside the CsPbI3 QDs protected the QDs from environmental moisture and solar irradiation. The introduction of S-OLA induced the recovery of the lost photoluminescence of the nonluminous aged CsPbI3 QDs with time to 95% of that of the fresh QDs.
通过镍取代和配体改变提高卤化铯铅量子点的光学性能和稳定性
在本研究中,我们研究了延长CsPbX3 (X: Cl, Br, I)结构钙钛矿材料寿命的方法。首先,比较了在CsPbBr3量子点(QDs)中掺杂Ni后结构和光学性质的变化。与未掺杂的量子点相比,掺镍量子点的稳态光致发光强度提高了3.8倍。不含镍的CsPbBr3的量子效率仅为56.7%,而掺杂镍的CsPbBr3的量子效率为82.9%。结果发现,掺杂的二价元素在钙钛矿结构中起缺陷作用,降低了电子和空穴的复合速率。在紫外光照射48 h后,CsPbBr3量子点的PL强度下降了约70%,而ni取代的CsPbBr3量子点的PL强度仅下降了18%,表明CsPbBr3量子点在紫外光照射下具有较长的稳定性。此外,ni取代的CsPbBr3量子点具有更高的温度和湿度稳定性。这些结果证实了Ni取代法可以有效地提高CsPbX3量子点的稳定性。其次,我们利用硫-油基胺(S-OLA)配合物在CsPbI3量子点表面蚀刻缺陷丰富的表面,然后自组装形成CsPbI3量子点外的基质,保护量子点免受环境水分和太阳辐射的影响。CsPbI3量子点的发光强度比初始值提高了21%。CsPbI3量子点的胶体稳定性显著提高。引入S-OLA后,未发光老化CsPbI3量子点的光致发光损失随时间恢复到新鲜量子点的95%。此外,PL维持了一个月。稳定性和发光强度的提高是实现高性能钙钛矿量子点器件的关键。在本研究中,我们研究了延长CsPbX3 (X: Cl, Br, I)结构钙钛矿材料寿命的方法。首先,比较了在CsPbBr3量子点(QDs)中掺杂Ni后结构和光学性质的变化。结果发现,掺杂的二价元素在钙钛矿结构中起缺陷作用,降低了电子和空穴的复合速率。ni取代CsPbBr3量子点具有较高的温度和湿度稳定性。这些结果证实了Ni取代法可以有效地提高CsPbX3量子点的稳定性。其次,我们利用硫-油基胺(S-OLA)配合物在CsPbI3量子点表面蚀刻缺陷丰富的表面,然后自组装形成CsPbI3量子点外的基质,保护量子点免受环境水分和太阳辐射的影响。引入S-OLA后,未发光老化CsPbI3量子点的光致发光损失随时间恢复到新鲜量子点的95%。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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