Despite
much attention on the photoelectronic device applications
of CuO-based materials, a thorough analysis of optical properties
and electronic band structure of Ni-doped CuO films is still necessary.
Here, the calculation based on the density functional theory revealed
a strong hybridization of O 2p and Cu 3d orbits near the conduction
band minimum (CBM) and valence band maximum (VBM) of CuO films.
The Ni addition is found to enhance the carrier mobility, because
the weaker localization of O 2p states at the VBM is observed in 50
atom % doped CuO. To confirm the theoretical results, the ellipsometric
spectra of solution-processed CuO films doped by Ni ions (from 0 to
50 atom %) were fitted, and the optical constants were uniquely extracted.
The optical conductivity has a linear increase with the Ni doping
concentration, which results from the decreased electron traps. Besides,
the band gap was found to be modulated in a range of 2.22–2.37
eV owing to the quantum confinement effects. The variation trend is
confirmed by the first-principles calculation, where the computational
indirect band gap is 1.27 and 1.79 eV for pure CuO and 50 atom % Ni-doped
CuO. Four electronic transitions are observed at ∼2.75, 3.27,
4.01, and 4.90 eV, and the physical origins have been discussed.