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We present time-resolved high energy x-ray diffraction (tr-HEXRD),time-resolved hard x-ray photoelectron spectroscopy (tr-HAXPES) andtime-resolved grazing incidence small angle x-ray scattering (tr-GISAXS) dataof the reactive molecular beam epitaxy (RMBE) of $\mathrm{Fe_3O_4}$ ultrathinfilms on various substrates. Reciprocal space maps are recorded during thedeposition of $\mathrm{Fe_3O_4}$ on $\mathrm{SrTiO_3(001)}$, MgO(001) andNiO/MgO(001) in order to observe the temporal evolution of Bragg reflectionssensitive to the octahedral and tetrahedral sublattices of the inverse spinelstructure of $\mathrm{Fe_3O_4}$. A time delay between the appearance of rocksalt and spinel-exclusive reflections reveals that first, the iron oxide filmgrows with $\mathrm{Fe_{1-\delta}O}$ rock salt structure with exclusiveoccupation of octahedral lattice sites. When this film is 1.1$\,$nm thick, thefurther growth of the iron oxide film proceeds in the inverse spinel structure,with both octahedral and tetrahedral lattice sites being occupied. In addition,iron oxide on $\mathrm{SrTiO_3(001)}$ initially grows with none of thesestructures. Here, the formation of the rock salt structure starts when the filmis 1.5$\,$nm thick. This is confirmed by tr-HAXPES data obtained during growthof iron oxide on $\mathrm{SrTiO_3(001)}$, which demonstrate an excess of$\mathrm{Fe^{2+}}$ cations in growing films thinner than 3.2$\,$nm. This rocksalt phase only appears during growth and vanishes after the supply of the Femolecular beam is stopped. Thus, it can be concluded the rock salt structure ofthe interlayer is a property of the dynamic growth process. The tr-GISAXS datalink these structural results to an island growth mode of the first 2-3$\,$nmon both MgO(001) and $\mathrm{SrTiO_3(001)}$ substrates.

Time-resolved diffraction and photoelectron spectroscopy investigation of the reactive molecular beam epitaxy of $\mathrm{Fe_3O_4}$ ultrathin films