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The axial ligation by the –P[double bond, length as m-dash]O group of a phosphonic diamide in an air-stable Nd(III) complex ensures a pseudo-D5h symmetry leading to the stabilization of the mJ = |±9/2〉 state; this in turn is responsible for the observed SIM behaviour at zero field and the slow relaxation of magnetization up to 8.0 K.

Graphical abstract: An unprecedented zero field neodymium(iii) single-ion magnet based on a phosphonic diamide

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