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Reversible Changes in Resistance of Perovskite Nickelate NdNiO<sub>3</sub> Thin Films Induced by Fluorine Substitution
Perovskite
nickel oxides are of fundamental as well as technological interest
because they show large resistance modulation associated with phase
transition as a function of the temperature and chemical composition.
Here, the effects of fluorine doping in perovskite nickelate NdNiO<sub>3</sub> epitaxial thin films are investigated through a low-temperature
reaction with polyvinylidene fluoride as the fluorine source. The
fluorine content in the fluorinated NdNiO<sub>3–<i>x</i></sub>F<sub><i>x</i></sub> films is controlled with precision
by varying the reaction time. The fully fluorinated film (<i>x</i> ≈ 1) is highly insulating and has a bandgap of
2.1 eV, in contrast to NdNiO<sub>3</sub>, which exhibits metallic
transport properties. Hard X-ray photoelectron and soft X-ray absorption
spectroscopies reveal the suppression of the density of states at
the Fermi level as well as the reduction of nickel ions (valence state
changes from +3 to +2) after fluorination, suggesting that the strong
Coulombic repulsion in the Ni 3d orbitals associated with the fluorine
substitution drives the metal-to-insulator transition. In addition,
the resistivity of the fluorinated films recovers to the original
value for NdNiO<sub>3</sub> after annealing in an oxygen atmosphere.
By application of the reversible fluorination process to transition-metal
oxides, the search for resistance-switching materials could be accelerated