Slowing magnetic relaxation with open-shell diluents
Slowing magnetic relaxation with open-shell diluents
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DOI：
10.1016/j.xcrp.2022.100802
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发表时间：
2022-03
期刊：
影响因子：
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通讯作者：
Ian P. Moseley;Christopher P. Ard;J. DiVerdi;A. Ozarowski;Hua Chen;Joseph M. Zadrozny
中科院分区：
文献类型：
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作者：
Ian P. Moseley;Christopher P. Ard;J. DiVerdi;A. Ozarowski;Hua Chen;Joseph M. Zadrozny
通过局部环境设计减缓磁弛豫的策略对于开发下一代基于自旋的技术(例如量子信息处理)至关重要。在这里，我们演示了一种通过局部磁环境的化学设计来做到这一点的技术。我们发现，将开壳配合物(Ph_4P)_2[Co(Sph)_4]嵌入到等结构开壳物种(Ph_4P)_2[M(Sph)_4](M=Ni~(2+)，S=1；M_2=Fe~(2+)，S=2；M_2=Mn~(2+)，S=5/2)中将使嵌入的[Co(Sph)_4]~(2-)离子的磁弛豫慢三个数量级。磁学、电子顺磁共振(EPR)和计算分析表明，稀释剂的整数自旋和大的正零场分裂(D)值会产生一个安静的局部磁场，从而减缓嵌入的Co分子的驰豫速率。这些结果将使研究严格的抗磁性同系物要么无法合成，要么不是同构体的磁性系统得以研究。
Strategies for slowing magnetic relaxation via local environmental design are vital for developing next-generation spin-based technologies (e.g., quantum information processing). Herein, we demonstrate a technique to do so via chemical design of a local magnetic environment. We show that embedding the open-shell complex (Ph4P)2[Co(SPh)4] in solid-state matrices of the isostructural, open-shell species (Ph4P)2[M(SPh)4] (M = Ni2+,S= 1; M = Fe2+,S= 2; M = Mn2+,S=5/2) will slow magnetic relaxation for the embedded [Co(SPh)4]2–ion by three orders of magnitude. Magnetometry, electron paramagnetic resonance (EPR), and computational analyses reveal that integer spin and large, positive zero-field splitting (D) values for the diluent produce a quiet, local magnetic field that slows relaxation rates for the embedded Co molecules. These results will enable the investigation of magnetic systems for which strictly diamagnetic congeners are either synthetically inaccessible or are not isostructural.