Femtosecond-laser induced two-photon absorption of GaN and AlxGa1-xN thin films: Tuning the nonlinear optical response by alloying and doping

Abstract Semiconductors thin films are the foundation of modern technology. While the nonlinear optical (NLO) properties of bulk semiconductors have been systematically studied in the last three decades, it is still a great challenge to obtain them for semiconductors thin films, as the high laser irradiance in NLO experiments tends to irreversibly damage the thin films. In addition, tuning the NLO response of semiconductor thin films by alloying and doping has not been explored yet. Here, we study the influence of the Aluminum content in AlxGa1-xN thin films and the n-type doping concentration in GaN thin films on their two-photon absorption (2 PA) coefficients. For this, we investigate five different GaN-based thin films: an unintentionally doped one with no Al as a reference, two n-type doped GaN films with distinct concentrations of silicon impurities, and two AlxGa1-xN alloys with an aluminum content of 5.5% and 9.0%, respectively. The femtosecond 2 PA spectra reveal that doping impurities reduce the non-linear coefficients (∼10%), while alloying with Al enhances the 2 PA coefficient up to 30%. We use the model of Brandi and Araujo to determine Kane's energy parameter related to the transition matrix element for each sample and compare them with recent theoretical studies based on the k·p theory where an excellent agreement is found.