Prediction for the singlet-triplet excitation energy for the spinel MgTi$_2$O$_4$ using first-principles diffusion Monte Carlo

Abstract

The spinel, MgTi$_2$O$_4$, undergoes a transition into a dimerized state at low temperatures that is expected to be a spin singlet. However, no signature of a singlet-triplet transition has been discovered, in part due to the difficulty of predicting the energy of the transition from theory. We find that the dimers of MgTi$_2$O$_4$ can be described by a Heisenberg model with very small interactions between different dimers. Using high-accuracy first-principles quantum Monte Carlo combined with a novel model-fitting approach, we predict the singlet-triplet gap of these dimers to be 350(50) meV, a higher energy than previous experimental observations have considered. The prediction is published in advance of experimental confirmation.