Controlling Electron Spin Decoherence in Nd-based Complexes via Symmetry Selection

Jing Li; Lei Yin; Shi-Jie Xiong; Xing-Long Wu; Fei Yu; Zhong-Wen Ouyang; Zheng-Cai Xia; Yi-Quan Zhang; Johan van Tol; You Song; Zhenxing Wang

doi:10.1016/j.isci.2020.100926

Controlling Electron Spin Decoherence in Nd-based Complexes via Symmetry Selection

iScience. 2020 Mar 27;23(3):100926. doi: 10.1016/j.isci.2020.100926. Epub 2020 Feb 20.

Authors

Jing Li¹, Lei Yin², Shi-Jie Xiong³, Xing-Long Wu³, Fei Yu¹, Zhong-Wen Ouyang², Zheng-Cai Xia², Yi-Quan Zhang⁴, Johan van Tol⁵, You Song⁶, Zhenxing Wang⁷

Affiliations

¹ State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.
² Wuhan National High Magnetic Field Center & School of Physics, Huazhong University of Science and Technology, Wuhan 430074, P. R. China.
³ National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093, P. R. China.
⁴ Jiangsu Key Laboratory for NSLSCS, School of Physical Science and Technology, Nanjing Normal University, Nanjing 210023, P. R. China. Electronic address: zhangyiquan@njnu.edu.cn.
⁵ National High Magnetic Field Laboratory, Florida State University, Tallahassee, FL 32310, USA. Electronic address: vantol@magnet.fsu.edu.
⁶ State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China. Electronic address: yousong@nju.edu.cn.
⁷ Wuhan National High Magnetic Field Center & School of Physics, Huazhong University of Science and Technology, Wuhan 430074, P. R. China. Electronic address: zxwang@hust.edu.cn.

Abstract

Long decoherence time is a key consideration for molecular magnets in the application of the quantum computation. Although previous studies have shown that the local symmetry of spin carriers plays a crucial part in the spin-lattice relaxation process, its role in the spin decoherence is still unclear. Herein, two nine-coordinated capped square antiprism neodymium moieties [Nd(CO₃)₄H₂O]^5- with slightly different local symmetries, C₁ versus C₄ (1 and 2), are reported, which feature in the easy-plane magnetic anisotropy as shown by the high-frequency electron paramagnetic resonance (HF-EPR) studies. Detailed analysis of the relaxation time suggests that the phonon bottleneck effect is essential to the magnetic relaxation in the crystalline samples of 1 and 2. The 240 GHz Pulsed EPR studies show that the higher symmetry results in longer decoherence times, which is supported by the first principle calculations.

Keywords: Materials Property; Molecules; Quantum Chemical Calculations.