Nonlinear Optical Properties of Aluminum Doped Zinc Oxide
Abstract
Nonlinear optical (NLO) materials are crucial to future progress in industrial and technological applications that involve intense light-matter interaction. While ZnO-related materials are known to possess good NLO properties, existing results on ZnO and AZO (Al-doped ZnO) are mostly available at a single wavelength or limited ranges. Therefore, NLO dispersions (wavelength dependences) are not entirely studied, especially at longer wavelengths far below the bandgap. It is important to explore wavelength dependences since doping can induce a drastic change in the NLO responses at varied spectral ranges via doping-induced subgap-state contributions. We present results of our studies on nonlinear harmonic generation from our samples, which include 1) second harmonic generation and 2) third harmonic generation precisely characterized by Maker fringes as a function of both Al doping and wavelength. We exhaustively discuss the possible cause for the modified optical nonlinearities observed in our AZO thin films and give detailed comparisons of our observations with the previous studies. We also present the results of open- and close-aperture Z-scans to characterize the two-photon absorption coefficient (TPA) and the nonlinear refractive index (NLR), respectively, of the AZO films. There was no clearcut evidence of monotonic dependence of TPA and NLR on doping. This presumably indicates that the overall effect is nontrivial and should be understood in terms of combined effects of bandgap shift and crystallinity upon varying the doping level. Most intriguingly, we found that NLR values from the closed-aperture Z-scan are very large by orders of magnitude when compared with the bulk counterparts. Similar observation was made for TPA values from the open-aperture Z-scan. To countercheck very large NLO absorption, we conducted simple intensity scan by varying the incident photon number on each sample but fixing the beam area to eliminate any possible errors related to optical damage at the Z-scan focus. However, we confirmed that the TPA values are also very large and comparable to those obtained by the open-aperture Z-scan. We try to explain this very large nonlinearity by seriously considering the previously proposed models.
- Publication:
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Ph.D. Thesis
- Pub Date:
- 2017
- Bibcode:
- 2017PhDT........20O
- Keywords:
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- Physics