Lin Cheng-Chieh, Huang Shing-Jong, Wu Pei-Hao, Chen Tzu-Pei, Huang Chih-Ying, Wang Ying-Chiao, Chen Po-Tuan, Radeva Denitsa, Petrov Ognyan, Gelev Vladimir M, Sankar Raman, Chen Chia-Chun, Chen Chun-Wei, Yu Tsyr-Yan
International Graduate Program of Molecular Science and Technology (NTU-MST), National Taiwan University, 10617, Taipei, Taiwan.
Molecular Science and Technology Program, Taiwan International Graduate Program (TIGP), Academia Sinica, 11529, Taipei, Taiwan.
Nat Commun. 2022 Mar 21;13(1):1513. doi: 10.1038/s41467-022-29207-6.
Limited methods are available for investigating the reorientational dynamics of A-site cations in two-dimensional organic-inorganic hybrid perovskites (2D OIHPs), which play a pivotal role in determining their physical properties. Here, we describe an approach to study the dynamics of A-site cations using solid-state NMR and stable isotope labelling. H NMR of 2D OIHPs incorporating methyl-d-ammonium cations (d-MA) reveals the existence of multiple modes of reorientational motions of MA. Rotational-echo double resonance (REDOR) NMR of 2D OIHPs incorporating N- and ¹³C-labeled methylammonium cations (C,N-MA) reflects the averaged dipolar coupling between the C and N nuclei undergoing different modes of motions. Our study reveals the interplay between the A-site cation dynamics and the structural rigidity of the organic spacers, so providing a molecular-level insight into the design of 2D OIHPs.
用于研究二维有机-无机杂化钙钛矿（2D OIHPs）中A位阳离子重取向动力学的方法有限，而A位阳离子在决定其物理性质方面起着关键作用。在此，我们描述了一种使用固态核磁共振和稳定同位素标记来研究A位阳离子动力学的方法。含有甲基-d-铵阳离子（d-MA）的2D OIHPs的¹H核磁共振揭示了MA存在多种重取向运动模式。含有N和¹³C标记的甲基铵阳离子（C,N-MA）的2D OIHPs的旋转回波双共振（REDOR）核磁共振反映了经历不同运动模式的C和N原子核之间的平均偶极耦合。我们的研究揭示了A位阳离子动力学与有机间隔基结构刚性之间的相互作用，从而为二维有机-无机杂化钙钛矿的设计提供了分子水平的见解。
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