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Despite its use as a constituent layer for realization of a polar metal and interfacial conductivity, the microscopic study of electronic structure of CaTiO is still very limited. Here, we epitaxially stabilized CaTiO films on NdGaO (110) substrates in a layer-by-layer way by pulsed laser deposition. The structural and electronic properties of the films were characterized by reflection-high-energy-electron-diffraction, X-ray diffraction, and element-specific resonant X-ray absorption spectroscopy. To reveal the orbital polarization and the crystal field splitting of the titanium 3 state, X-ray linear dichroism was carried out on CaTiO films, demonstrating the orbital configuration of / <  <  < . To further explore the origin of this configuration, we performed the first-principles density function theory calculations, which linked the orbital occupation to the on-site energy of Ti 3 orbitals. These findings can be important for understanding and designing exotic quantum states in heterostructures based on CaTiO.


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