Enhancement of Nonlinear Absorption in Defect Controlled ZnO Polycrystalline Thin Films by Means of Co‐Doping

The structural, optical, and nonlinear optical absorption properties of ZnO polycrystalline thin films are investigated. Energy bandgap values are obtained with linear absorption spectrum and depending on either sole doping of Al or co‐doping, bandgap energies shift toward higher or lower energies. With Al‐only doping, bandgap of the ZnO thin film shifts toward higher energies which can be attributed to Moss–Burstein effect, and with co‐doping (Al–Cu or Al–Co) bandgap energies shift toward lower energies due to defect states residing within the bandgap. Urbach energies and grain sizes are calculated to study the effect of defect states on the nonlinear absorption, and these calculations indicate that co‐doping drastically reduces the grain size thereby increasing the contribution to the defect density by means of boundary defects. To analyze the transmission in open aperture Z‐scan data, a theoretical model incorporating one‐photon, two‐photon, and free‐carrier absorptions as well as their saturations is used. By this modeling, saturation intensity thresholds and effective nonlinear absorption coefficients are extracted from fitting of the experimental data. Highest saturation intensity threshold and effective nonlinear absorption coefficient are found for ZnO:(Al, Co) and ascribed to having the smallest bandgap energy and highest Urbach energy.