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Upon reduction of the film thickness we observe a metal-insulator transition in epitaxially stabilized, spin-orbit coupled SrIrO ultrathin films. By comparison of the experimental electronic dispersions with density functional theory at various levels of complexity we identify the leading microscopic mechanisms, i.e., a dimensionality-induced re-adjustment of octahedral rotations, magnetism, and electronic correlations. The astonishing resemblance of the band structure in the two-dimensional limit to that of bulk SrIrO opens new avenues to unconventional superconductivity by “clean” electron doping through electric field gating.

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