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Metal-insulator transitions (MIT) occurring in non-adiabatic conditions canevolve through high-energy intermediate states that are difficult to observeand control via static methods. By monitoring the out-of-equilibrium structuraldynamics of a magnetite (Fe3O4) crystal via ultrafast electron diffraction, weshow that MITs can evolve through different pathways by properly selecting theelectronic excitation with light. Near-infrared (800 nm) photons inducing d-delectronic transitions is found to favor the destruction of the long-rangezigzag network of the trimerons and to generate a phase separation betweencubic-metallic and monoclinic-insulating regions. Instead, visible light (400nm) further promotes the long-range order of the trimerons by stabilizing thecharge density wave fluctuations through the excitation of the oxygen 2p toiron 3d charge transfer and, thus, fosters a reinforcement of the monoclinicinsulating phase. Our experiments demonstrate that tailored light pulses candrive strongly correlated materials into different hidden phases, influencingthe lifetime and emergent properties of the intermediate states.

Ultrafast generation of hidden phases via energy-tuned electronic photoexcitation in magnetite