Highly Degenerate Ground States in a Frustrated Antiferromagnetic Kagome Lattice in a Two-Dimensional Metal–Organic Framework

Realization of the Kagome antiferromagnetic (KAF) lattice is of high interest because the geometric frustration in the Kagome lattice is expected to give rise to highly degenerated ground states that may host exotic phases such as quantum spin liquid. Here we demonstrate the design and synthesis of a single-layer two-dimensional metal-organic framework (2D-MOF) containing a Kagome lattice of Fe(II) ions assembled on a Au(111) surface. First-principles calculations reveal that the Fe(II) ions are at a high spin state of S = 2 and are coupled antiferromagnetically with nearest-neighboring exchange J1 = 5.8 meV. The ground state comprises various degenerated spin configurations including the well-known q = 0 and q = √3 × √3 phases. Remarkably, we observe a spin excitation at 6 meV using tunneling spectroscopy. This work points out a feasible route toward realizing spin 1/2 KAF, a candidate quantum spin liquid system, by replacing Fe(II) by Cu(II) in the same structure.