A key difference between our calculations and the prior literature is the spin state at high temperatures, >150 K. Only one set of magnetic data has been acquired on this system with an observed χT = 2 at 300 K which was assigned as arising from two non-interacting S = 1 Cr centers. Our results instead suggest a well-isolated S = 2 ground state for the dimer with strongly interacting Cr centers at high temperatures. We note that strong Cr-Cr interactions are predicted with all computational methods, and across all temperatures in our study (see below), and so we sought to rationalize this difference between theory and experiment.