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We combine ultrafast electron diffraction and time-resolved terahertzspectroscopy measurements to unravel the connection between structure andelectronic transport properties during the photoinduced insulator-metaltransitions in vanadium dioxide. We determine the structure of the metastablemonoclinic metal phase, which exhibits anti-ferroelectric charge order arisingfrom a thermally activated, orbital-selective phase transition in the electronsystem. The relative contribution of this photoinduced monoclinic metal (whichhas no equilibrium analog) and the photoinduced rutile metal (known from theequilibrium phase diagram) to the time and pump-fluence dependent multi-phasecharacter of the film is established, as is the respective impact of these twodistinct phase transitions on the observed changes in terahertz conductivity.Our results represent an important new example of how light can control theproperties of strongly correlated materials and elucidate that multi-modalexperiements are essential when seeking a detailed connection between ultrafastchanges in optical-electronic properties and lattice structure in complexmaterials.

How optical excitation controls the structure and properties of vanadium dioxide