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We report the existence of a two-dimensional electron system (2DES) at the(001) surface of CaTiO3. Using angle-resolved photoemission spectroscopy, wefind a hybridization between the d_xz and d_yz orbitals, not observed in the2DESs at the surfaces of other ATiO3 perovskites, e.g. SrTiO3 or BaTiO3. Basedon a comparison of the 2DES properties in these three materials, we show howthe electronic structure of the 2DES (bandwidth, orbital order and electrondensity) is coupled to different typical lattice distortions in perovskites.The orbital hybridization in orthorhombic CaTiO3 results from the rotation ofthe oxygen octahedra, which can also occur at the interface of oxideheterostructures to compensate strain. More generally, the control of theorbital order in 2DES by choosing different A-site cations in perovskitesoffers a new gateway towards 2DESs in oxide heterostructures beyond SrTiO3.

Two-dimensional electron systems in ATiO3 perovskites (A = Ca, Ba, Sr): control of orbital hybridization and order