Ab initio screening of quantum frustrated materials with kagome geometries

The kagome lattice offers a fertile ground for exploring complex magnetic orders driven by geometric frustration and competing exchange interactions. Building on our multi-step ab initio screening framework, we identified several unsynthesized kagome-lattice compounds—Li₄Fe₃WO₈, Li₂V₃F₈, Li₅VP₂(O₄F)₂, and Li₂MgCo₃O₈ (P2/m and C2/m)—whose extracted exchange parameters fall into distinct regimes of the J₁-J₂-J_3a(3d) Heisenberg model. By combining Luttinger–Tisza analysis with Landau–Lifshitz–Gilbert simulations, we map the full classical phase diagram and uncover multiple nontrivial spin ordering, including the well-known q=0, √3 × √3, and cuboctahedral (cuboc-1 and cuboc-2) orders. Crucially, when J_3a and J₂ compete, we identify a previously unreported cuboctahedral-3 (cuboc-3) phase characterized by an enlarged 4×4 magnetic unit cell and twofold chiral degeneracy. Our results position Li₂MgCo₃O₈ near the cuboc-3 region, Li₄Fe₃WO₈ within cuboc-1, and Li₂V₃F₈ and Li₅VP₂(O₄F)₂ in the highly-frustrated J₁-dominated sector hosting classical Coulomb-liquid-like behavior. These findings demonstrate how first-principles-derived exchange interaction can bridge materials design and model phase diagrams, guiding future experimental searches for chiral and quantum spin-liquid states in kagome magnets.