Spectroscopic Evidence of a Dimensionality-Induced Metal-to-Insulator Transition in the Ruddlesden–Popper La(n+1)Ni(n)O(3n+1) Series

[Image: see text] Perovskite-based heterostructures have recently gained remarkable interest, thanks to atomic-scale precision engineering. These systems are very susceptible to small variations of control parameters, such as two-dimensionality, strain, lattice polarizability, and doping. Focusing on the rare-earth nickelate diagram, LaNiO(3) (LNO) catches the eye, being the only nickelate that does not undergo a metal-to-insulator transition (MIT). Therefore, the ground state of LNO has been studied in several theoretical and experimental papers. Here, we show by means of infrared spectroscopy that an MIT can be driven by dimensionality control in ultrathin LNO films when the number of unit cells drops to 2. Such a dimensionality tuning can eventually be tailored when a physically implemented monolayer in the ultrathin films is replaced by a digital single layer embedded in the Ruddlesden–Popper La(n+1)Ni(n)O(3n+1) series. We provide spectroscopic evidence that the dimensionality-induced MIT in Ruddlesden–Popper nickelates strongly resembles that of ultrathin LNO films. Our results can pave the way to the employment of Ruddlesden–Popper La(n+1)Ni(n)O(3n+1) to tune the electronic properties of LNO through dimensional transition without the need of physically changing the number of unit cells in thin films.