Spin-lattice Coupling and the Emergence of the Trimerized Phase in the S=1 Kagome Antiferromagnet Na2Ti3Cl8

Spin-1 antiferromagnets are abundant in nature, but few theories exist to understand their properties and behavior when geometric frustration is present. Here we study the S = 1 kagome compound Na2Ti3Cl8 using a combination of density functional theory, exact diagonalization, and density matrix renormalization group approaches to achieve a first principles supported explanation of its exotic magnetic phases. We find that the effective magnetic Hamiltonian includes essential non-Heisenberg terms that do not stem from spin-orbit coupling, and both trimerized and spin-nematic magnetic phases are relevant. The experimentally observed structural transition to a breathing kagome phase is driven by spin-lattice coupling, which favors the trimerized magnetic phase against the quadrupolar one. We thus show that lattice effects can be necessary to understand the magnetism in frustrated magnetic compounds and surmise that Na2Ti3Cl8 is a compound that cannot be understood from only electronic or only lattice Hamiltonians, very much like VO2.