1. The study uses a minimal four-orbital, four-electron model to describe spimmerism and SOC. How might the inclusion of additional d-orbitals or ligand-field asymmetry (e.g., tetragonal vs. octahedral distortions) affect the predicted spin-state mixing? The authors neglect charge-transfer states (LMCT/MLCT) and vibronic coupling. Could these effects destabilize spimmerism in real systems, particularly in strongly correlated transition metal complexes?
2. The authors claim that spimmerism persists even for Lambda≫1.0. Does this hold for experimentally relevant SOC strengths, or would strong SOC quench spimmerism in favor of spin-orbit-dominated states? The model assumes frozen ligand spins. How would dynamic spin fluctuations (e.g., due to temperature or exchange modulation) influence the coexistence of spimmerism and SOC?
3. The study proposes spimmeric states for quantum error correction. What are the expected coherence times (T2) of such states, given SOC-induced relaxation pathways?The results focus on a d2 ion (e.g., Ni(II)). Would d4−d7 systems (more common in spin-crossover chemistry) exhibit similar behavior, or would Jahn-Teller effects dominate? Would be great to hear the authors’ thoughts on these points!
