Natural-orbital analysis of our RASSCF(16e,16o) calculations suggests that the two component S = 1 units of this system are best understood not as two S = 1 chromium ions, but as two pairs of electrons occupying two pairs of orbitals distinguished by the magnitude of their angular momentum about the Cr-Cr internuclear axis. The two-step crossover of cation I consists of the reduction from S = 2 to S = 0 of these two electron pairs at two different temperatures. Our analysis supports some aspects of both of the two proposed spin-crossover mechanisms of Goeta, A. et al.: