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利用锰电子顺磁共振探测MAPbCl杂化钙钛矿的结构和动力学性质。

Probing structural and dynamic properties of MAPbCl hybrid perovskite using Mn EPR.

作者信息

Usevičius Gediminas, Turčak Justinas, Zhang Yuxuan, Eggeling Andrea, Einorytė Žyginta, Hope Michael Allan, Svirskas Šarūnas, Klose Daniel, Kalendra Vidmantas, Aidas Kestutis, Jeschke Gunnar, Banys Jūras, Šimėnas Mantas

机构信息

Faculty of Physics, Vilnius University, Sauletekio 3, 10257 Vilnius, Lithuania.

Laboratory of Magnetic Resonance, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland.

出版信息

Dalton Trans. 2024 Apr 30;53(17):7292-7302. doi: 10.1039/d4dt00116h.

DOI:10.1039/d4dt00116h
PMID:38587489
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11059044/
Abstract

Hybrid methylammonium (MA) lead halide perovskites have emerged as materials exhibiting excellent photovoltaic performance related to their rich structural and dynamic properties. Here, we use multifrequency (X-, Q-, and W-band) electron paramagnetic resonance (EPR) spectroscopy of Mn impurities in MAPbCl to probe the structural and dynamic properties of both the organic and inorganic sublattices of this compound. The temperature dependent continuous-wave (CW) EPR experiments reveal a sudden change of the Mn spin Hamiltonian parameters at the phase transition to the ordered orthorhombic phase indicating its first-order character and significant slowing down of the MA cation reorientation. Pulsed EPR experiments are employed to measure the temperature dependences of the spin-lattice relaxation and decoherence times of the Mn ions in the orthorhombic phase of MAPbCl revealing a coupling between the spin center and vibrations of the inorganic framework. Low-temperature electron spin echo envelope modulation (ESEEM) experiments of the protonated and deuterated MAPbCl analogues show the presence of quantum rotational tunneling of the ammonium groups, allowing to accurately probe their rotational energy landscape.

摘要

混合甲基铵（MA）卤化铅钙钛矿已成为一类材料，因其丰富的结构和动力学性质而展现出优异的光伏性能。在此，我们利用MAPbCl中Mn杂质的多频（X波段、Q波段和W波段）电子顺磁共振（EPR）光谱，来探究该化合物有机和无机亚晶格的结构及动力学性质。温度依赖的连续波（CW）EPR实验表明，在向有序正交相转变时，Mn自旋哈密顿参数发生突然变化，这表明其具有一级相变特征，且MA阳离子重取向显著减慢。采用脉冲EPR实验来测量MAPbCl正交相中Mn离子的自旋-晶格弛豫时间和退相干时间的温度依赖性，揭示了自旋中心与无机骨架振动之间的耦合。对质子化和氘代MAPbCl类似物进行的低温电子自旋回波包络调制（ESEEM）实验表明存在铵基团的量子旋转隧穿，从而能够精确探测其旋转能态。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/6d2968ba0b6b/d4dt00116h-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/d6703f2bbc9d/d4dt00116h-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/b93c2c795b45/d4dt00116h-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/d7a554ce4019/d4dt00116h-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/c15e364d6e35/d4dt00116h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/6d2968ba0b6b/d4dt00116h-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/d6703f2bbc9d/d4dt00116h-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/b93c2c795b45/d4dt00116h-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/d7a554ce4019/d4dt00116h-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/c15e364d6e35/d4dt00116h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/843e/11059044/6d2968ba0b6b/d4dt00116h-f5.jpg

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