From strong to weak correlations in breathing-mode kagome van der Waals materials: Nb$_3$(F,Cl,Br,I)$_8$ as a robust and versatile platform for many-body engineering

Abstract: By combining ab initio downfolding with cluster dynamical mean-field theory, we study the degree of correlations in the low-temperature structures of the breathing-mode kagome van der Waals materials Nb$_3$(F,Cl,Br,I)$_8$. We show that the Coulomb correlation strength steadily increases from I to Br, Cl, and F, allowing us to identify Nb$_3$I$_8$ as a weakly correlated (obstructed atomic) insulator whose gap is only mildly affected by the local Coulomb interaction. Nb$_3$Br$_8$ and Nb$_3$Cl$_8$ are strongly correlated insulators, whose gaps are significantly influenced by Coulomb-induced vertex corrections. Nb$_3$F$_8$ is a prototypical bulk Mott-insulator whose gap is initially opened by strong correlation effects. Angle-resolved photoemission spectroscopy measurements comparing Nb$_3$Br$_8$ and Nb$_3$I$_8$ allow us to experimentally confirm these findings by revealing spectroscopic footprints of the degree of correlation. Our calculations further predict that the entire material family can be tuned into correlated charge-transfer or Mott-insulating phases upon electron or hole doping. Our magnetic property analysis additionally shows that inter-layer magnetic frustrations in the high-temperature phase drive the lattice phase transition to the low-temperature structures. The accompanying bilayer hybridization through inter-layer dimerization yields magnetic singlet ground states in the Cl, Br, and I compounds. Our findings establish Nb$_3$X$_8$ as a robust, versatile, and tunable class for van der Waals-based Coulomb and Mott engineering and allow us to speculate on the symmetry-breaking effects necessary for the recently observed Josephson diode effect in NbSe$_2$/Nb$_3$Br$_8$/NbSe$_2$ heterostructures.