华南理工大学蒋尚达团队报道了电子顺磁共振揭示铁电钙钛矿的电致晶体场畸变。相关研究成果于2024年7月3日发表在《美国化学会杂志》。

在过去的十年里，磁电材料因其适应各种功能的潜力而引起了多学科的兴趣。特别是，外部电场可以通过自旋-电耦合效应驱动这种材料的量子行为，具有高空间分辨率和低能量成本的优点。

该文中，研究人员报道了具有大压电效应的Mn²⁺掺杂铁电有机-无机杂化钙钛矿[(CH₃)₃NCH₂Cl]CdCl₃的自旋电耦合效应。使跃迁的电场操纵效率由脉冲电子顺磁共振决定。通过模拟角度相关电场调制的连续波电子顺磁共振，得到了自旋-电耦合效应的含方位哈密顿量。结果表明，外加电场不仅影响零场分裂张量的主值，而且影响其主轴方向。

该项工作提出并举例说明了一种理解自旋电耦合效应的途径，该效应源于施加在被施加电场修饰的自旋离子上的晶体场，这可能指导合理筛选和设计满足量子信息应用中自旋的电场操纵效率要求的混合钙钛矿铁电体。

附：英文原文

Title: Electrically Induced Crystal Field Distortion in a Ferroelectric Perovskite Revealed by Electron Paramagnetic Resonance

Author: You-Chao Liu, Jia-Xin Chen, Peng-Xiang Fu, Yi-Qiu Liao, Yi-Han Wang, Ye-Xin Wang, Zheng Liu, Song Gao, Shang-Da Jiang

Issue&Volume: July 3, 2024

Abstract: The magnetoelectric material has attracted multidisciplinary interest in the past decade for its potential to accommodate various functions. Especially, the external electric field can drive the quantum behaviors of such materials via the spin-electric coupling effect, with the advantages of high spatial resolution and low energy cost. In this work, the spin-electric coupling effect of Mn2+-doped ferroelectric organic–inorganic hybrid perovskite [(CH3)3NCH2Cl]CdCl3 with a large piezoelectric effect was investigated. The electric field manipulation efficiency for the allowed transitions was determined by the pulsed electron paramagnetic resonance. The orientation-included Hamiltonian of the spin-electric coupling effect was obtained via simulating the angle-dependent electric field modulated continuous-wave electron paramagnetic resonance. The results demonstrate that the applied electric field affects not only the principal values of the zero-field splitting tensor but also its principal axis directions. This work proposes and exemplifies a route to understand the spin-electric coupling effect originating from the crystal field imposed on a spin ion being modified by the applied electric field, which may guide the rational screening and designing of hybrid perovskite ferroelectrics that satisfy the efficiency requirement of electric field manipulation of spins in quantum information applications.

DOI: 10.1021/jacs.4c05655

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c05655