Resilient cluster Mott states in layered Nb₃Cl₈ against pressure-induced symmetry breaking

In this work, by combining density-functional theory (DFT) with dynamical mean-field calculations (DMFT), we compare the crystal and electronic structures of the prototype cluster Mott insulator Nb$_{3}$Cl$_8$ at ambient and high-pressure. We explain the finite but significantly reduced charge gap experimentally observed at $P=9.7$ GPa. We reveal a local symmetry breaking of the Nb$_{3}$ trimer under pressure, reducing its symmetry from $C_{3v}$ to $C_{s}$. This leads to a strong bandwidth enhancement and a lift of band degeneracy. Crucially, despite the significant change of band details, the cluster Mott insulating state is robust against local symmetry breaking. We show that the experimental observed gap under pressure is still a cluster Mott gap and its reduced value stems from both increased bandwidth and reduced Coulomb interactions under pressure. Our study provides the first systematic theoretical elucidation of how pressure-induced symmetry breaking dictates the cluster Mott state, establishing a robust foundation for understanding the intricate relationship between symmetry, local/non-local correlations, and emergent quantum states in correlated cluster compounds.