Discovery of the soft electronic modes of the trimeron order in magnetite

The Verwey transition in magnetite (Fe3O4) is the first metal–insulator transition ever observed1 and involves a concomitant structural rearrangement and charge–orbital ordering. Owing to the complex interplay of these intertwined degrees of freedom, a complete characterization of the low-temperature phase of magnetite and the mechanism driving the transition have long remained elusive. It was demonstrated in recent years that the fundamental building blocks of the charge-ordered structure are three-site small polarons called trimerons2. However, electronic collective modes of this trimeron order have not been detected to date, and thus an understanding of the dynamics of the Verwey transition from an electronic point of view is still lacking. Here, we discover spectroscopic signatures of the low-energy electronic excitations of the trimeron network using terahertz light. By driving these modes coherently with an ultrashort laser pulse, we reveal their critical softening and hence demonstrate their direct involvement in the Verwey transition. These findings shed new light on the cooperative mechanism at the origin of magnetite’s exotic ground state. Spectroscopic study of the low-energy excitations in magnetite Fe3O4 shows the signatures of its charge-ordered structure involved in the metal–insulator transition, whose building blocks are the three-site small polarons, termed trimerons.