“Spin Tweaking” of a High‐Spin Molecule: An Mn25 Single‐Molecule Magnet with an S=61/2 Ground State

Spin doctoring: The already high spin of S=51/2 of a Mn25 complex has been pushed even higher, by approximately 20 %, to S=61/2 by targeted substitution of the azide ligands with an N,O-chelating group. This significant adjustment, or tweaking, of the spin suggests the general possibility that a given type of complicated, high-nuclearity, high-spin molecule can exhibit differing ground states by appropriate modification of the peripheral ligation.