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通过钾阳离子掺杂实现缺陷钝化和晶格畸变来揭示胶体钙钛矿量子点的光致发光调控:并非越多越好。

Unveiling the photoluminescence regulation of colloidal perovskite quantum dots via defect passivation and lattice distortion by potassium cations doping: Not the more the better.

作者信息

Chu Ya, Wang Chao, Ma Linlin, Feng Xia, Wang Beibei, Wu Yanqing, Jia Yan, Zhang Mingshui, Sun Yan, Zhang Haoyue, Zhao Guangjiu

机构信息

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin 300354, China.

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China.

出版信息

J Colloid Interface Sci. 2021 Aug 15;596:199-205. doi: 10.1016/j.jcis.2021.03.128. Epub 2021 Mar 24.

Abstract

In this work, we have first demonstrated that the potassium cation doping effect on photoluminescence (PL) regulation of CHNHPbBr (CHNH=MA) colloidal perovskite quantum dots (QDs) is significantly different from the other alkali cation doping effects. The PL intensity will be generally enhanced with the increase doping amounts of other alkali cations. Herein, we have unveiled that the PL of the potassium-doped perovskite QDs is initially prompted by the potassium ions doping and then inhibited with further growing doping amount of the potassium ions. Furthermore, we have also demonstrated that the PL inhibition phenomenon is ascribed as quick trapping of redundant photogenerated electrons by the trap states after huge amount doping besides defect passivation and octahedral structure distortion induced by the initial doping. At the same time, the specific excited state transient absorption and the lifetime of MAKPbBr also confirm that the radiation recombination process is enhanced via defect passivation and lattice distortion, which is induced by moderate potassium cations doping. In addition, the PL of colloidal perovskite quantum dots can be adjusted from orange to cyan within the wavelength range of 300 nm - 600 nm and exhibit better stability.

摘要

在这项工作中,我们首先证明了钾阳离子掺杂对CHNHPbBr(CHNH = MA)胶体钙钛矿量子点(QDs)光致发光(PL)调控的影响与其他碱金属阳离子掺杂效应显著不同。随着其他碱金属阳离子掺杂量的增加,PL强度通常会增强。在此,我们揭示了钾掺杂钙钛矿量子点的PL最初因钾离子掺杂而增强,随后随着钾离子掺杂量的进一步增加而受到抑制。此外,我们还证明了PL抑制现象归因于大量掺杂后陷阱态对多余光生电子的快速俘获,以及初始掺杂引起的缺陷钝化和八面体结构畸变。同时,MAKPbBr的特定激发态瞬态吸收和寿命也证实,适度的钾阳离子掺杂引起的缺陷钝化和晶格畸变增强了辐射复合过程。此外,胶体钙钛矿量子点的PL在300 nm - 600 nm波长范围内可从橙色调节至青色,并表现出更好的稳定性。

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