The first example is a small-molecule dissociation potential energy curve, and the second is magnetic coupling of a metal-oxide cluster that consitutes the node of a metal-organic framework, MOF, as discussed in Ref. 19, here investigated in more depth. nitrogen and carbon form π bonds crossing the boundaries between fragments, which is a process that this LASSCF wave function cannot model. Therefore, as Table shows, LASSCF (10,10) is variationally penalized by about 50 mE h compared to the corresponding CASCI (LASSI[∞,∞]) at the dissociation limit (256 vs 205 mE h ). The missing interfragment interaction is recovered by LASSI[r,q] and the CASCI K (∆N ) given by Eq. ( )] and spin-magnitude [w (I) K (S) given by Eq. ( )] quantum number in each fragment of dissociated (R NN = 3.25 Å) and equilbrium-geometry bisdiazene in the LASSI [3,3] However, examining the eigenvectors of the LASSI [3,3] wave function at both dissociation and equilibrium, we find that the majority of model states in LASSI [3,3] do not actually contribute: the 300 most significant model states collectively account for more than 99.99% of the ground state at both geometries. The 300 significant model states do not necessarily belong to any particular r, q tier of LASSI[r,q], and conversely neither do the roughly 4300 "deadwood" model states, because any r < 3 or q < 3 is inadequate to model the dissociation process with qualitative accuracy. Therefore, in order to improve upon the computational efficiency of LASSI [3,3] and LASSI[r,q] in general, we must investigate what distinguishes significant from deadwood model states.