Enhanced optical third-harmonic generation in phase-engineered nanostructured Zn1-x Cd x S thin films for optoelectronic device applications

A polycrystalline nanostructured thin film of zinc cadmium sulfide was meticulously fabricated on a glass substrate using the thermal evaporation method physical vapor deposition within a vacuum chamber. Different doping concentrations were introduced by varying the cadmium (Cd) content, resulting in Zn1-xCdxS films with Cd concentrations ranging from x = 0.00-0.20 wt %. The impact of Cd doping on the third-order nonlinear optical (TONLO) properties of these films was thoroughly studied using the Z-scan method, employing a diode-pumped solid-state continuous-wave laser. To gain insight into the structural characteristics, the Zn1-xCdxS thin films underwent analysis through x-ray diffraction. Optical studies confirmed the tunability of the optical band gap (Eg) in the Zn1-xCdxS films, ranging from 3.88 eV for undoped ZnS to 2.80 eV for the film fabricated with 20 wt. % of Cd-content. This significant reduction in 'Eg' renders the films highly suitable for use as absorbing layers in applications such as solar cells and optoelectronics. Surface morphology analysis, performed via field emission scanning electron microscopy, revealed noticeable alterations with increased Cd doping. Significantly, the doped films exhibited a substantial redshift in the band edge and an increase in transmittance within the visible and near-infrared regions. The investigation of TONLO properties, including the nonlinear absorption coefficient (beta), nonlinear refractive index (n(2)) and susceptibility chi(3), yielded values ranging from 3.15 x 10(-3) to 8.16 x 10(-3) (cm W-1), 1.65 x 10(-8) to 7.45 x 10(-8) (cm(2) W-1), and 3.12 x 10(-5) to 7.86 x 10(-5) (esu), respectively. These results indicate the presence of self-defocusing nonlinearity in the films. Overall, the outcomes underscore the potential of Cd-doped ZnS nanostructures in modifying surface morphology and enhancing NLO characteristics. Zn1-xCdxS thin films exhibit promise for applications in nonlinear optical devices, as evidenced by these encouraging findings.