We report the experimental evidence of evolving lattice distortion in high quality epitaxial orthorhombic SrIrO3(001) thin films fully strained on (001) SrTiO3 substrates. Angle-resolved X-ray photoemission spectroscopy studies show that the surface layer of 5 nm SrIrO3 films is Sr–O terminated, and subsequent layers recover the semimetallic state, with the band structure consistent with an orthorhombic SrIrO3(001) having the lattice constant of the substrate. While there is no band folding in the experimental band structure, additional super-periodicity is evident in low energy electron diffraction measurements, suggesting the emergence of a transition layer with crystal symmetry evolving from the SrTiO3 substrate to the SrIrO3(001) surface. Our study sheds light on the misfit relaxation mechanism in epitaxial SrIrO3 thin films in the orthorhombic phase, which is metastable in bulk
