Strategies for slowing magnetic relaxation are vital for developing next-generation spin-based technologies (e.g. quantum information processing). For single molecule magnets, slow relaxation is most often observed for complexes diluted in a diamagnetic substrate; however, applications of these molecules will require slow magnetic relaxation to be maintained in magnetically noisy environments.This work details a new technique for extending magnetic relaxation via chemical design of a local magnetic environment. Specifically, it has been found 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 up to three orders of magnitude. Magnetometry, EPR, and computational analyses reveal that integer spin diluents with large, positive zero field splitting (D) values produce a quiet local magnetic field and enable slower relaxation rates despite the presence of unparied electrons in the environment.

Slowing magnetic relaxation with open-shell diluents

ACS Spring 2022

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