Ab initio screening of quantum frustrated materials with kagome and triangular geometries

Abstract

Geometrical frustration is a powerful route to realize exotic phases such as quantum spin liquids. Despite extensive efforts, systematic searches targeting specific frustration motifs and their potential to host unconventional magnetic ground states remain rare, thus highlighting the need for a more focused and predictive materials discovery approach. Here we present a new strategy combining high-throughput first-principles calculations, magnetic force theory, and spin Hamiltonian analysis. Starting from the 150,000 material database, we catalogue candidate materials that may host competing exchange interactions and new types of magnetic states with the focus on kagome or triangular lattices. Our workflow not only reproduces the majority of known frustrated magnetic materials, validating our approach, but also predicts novel candidate compounds with targeted frustration profiles that have not yet been experimentally synthesized. Among these, we identify six promising new materials: one triangular lattice compound, KMgNiIO6, and five kagome lattice compounds; Li4Fe3WO8, Li2V3F8, Li5VP2(O4F)2, and Li2MgCo3O8 (P2/m and C2/m). For each candidate, we identify detailed magnetic properties and further propose their potential magnetic ground states, revealing that some of them may host entirely new magnetic phases driven by their distinct frustration characteristics.