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Thin film synthesis methods developed over the past decades have unlockedemergent interface properties ranging from conductivity to ferroelectricity.However, our attempts to exercise precise control over interfaces areconstrained by a limited understanding of growth pathways and kinetics. Here wedemonstrate that shuttered molecular beam epitaxy induces rearrangements ofatomic planes at a polar / non-polar junction of LaFeO$_3$ (LFO) /$n$-SrTiO$_3$ (STO) depending on the substrate termination. Surfacecharacterization confirms that substrates with two different (TiO$_2$ and SrO)terminations were prepared prior to LFO deposition; however, local electronenergy loss spectroscopy measurements of the final heterojunctions show apredominantly LaO / TiO$_2$ interfacial junction in both cases. Ab initiosimulations suggest that the interfaces can be stabilized by trapping extraoxygen (in LaO / TiO$_2$) and forming oxygen vacancies (in FeO$_2$ / SrO),which points to different growth kinetics in each case and may explain theapparent disappearance of the FeO$_2$ / SrO interface. We conclude thatjudicious control of deposition timescales can be used to modify growthpathways, opening new avenues to control the structure and properties ofinterfacial systems.

Dynamic Interface Rearrangement in LaFeO$_3$ / $n$-SrTiO$_3$ Heterojunctions