Intertwined spin-charge stripe order and polar lattice distortion in La${}_3$Ni${}_2$O${}_7$

Abstract

The low-temperature density-wave state of La${}_3$Ni${}_2$O${}_7$ hosts pronounced spin-density-wave (SDW) order, while recent experiments further reveal charge redistribution and a concomitant lattice-symmetry lowering. However, the microscopic relationship among spin, charge, and lattice remains unclear. Using first-principles calculations, we investigate the pressure evolution of the electronic structure and static spin susceptibility of La${}_3$Ni${}_2$O${}_7$, together with the energetics and lattice response of representative magnetic configurations. We trace the SDW instability to strong Fermi-surface nesting and find that the high-pressure spin response closely tracks $T_{\mathrm{C}}$, suggesting spin-fluctuation-mediated pairing. Among the candidate magnetic states considered, the spin-charge-stripe states emerge as energetically favored and dynamically stable, developing pronounced disproportionation of both the local Ni moments and the Ni--O bond lengths. Remarkably, the lowest-energy a-stripe state spontaneously relaxes into the experimentally proposed polar Am2m structure through a polar distortion along the b axis. These results establish a unified picture in which spin, charge, and lattice responses are strongly intertwined in the low-pressure density-wave state, while spin fluctuations remain a plausible ingredient of superconductivity under pressure.