184 © 2025 The Author(s). Published by College of Education for Pure Science (Ibn Al-Haitham), University of Baghdad. This is an open-access article distributed under the terms of the Creative Commons Attribution 4.0 International License Fabrication and Study Structure and Optical Properties of Cu0.75Zn0.25S Thin Film Ali J. Soud1 and Bushra K.H. Al-Maiyaly2* 1,2Department of Physics, College of Education for Pure Science (Ibn Al-Haitham), University of Baghdad, Baghdad, Iraq. *Corresponding Author. Received: 30 May 2024 Accepted: 10 September 2024 Published: 20 April 2025 doi.org/10.30526/38.2.4022 Abstract Thin films (CuxZn1-xS) with x = 0.75 nano crystallized were deposited from the alloy on glass substrates in a vacuum ~ 2 × 10− 5 mbar by thermal evaporation technique with 450±20 nm thickness. The effects of annealed temperature (deposits, 423, 523, and 623) K for one hour on the structure, morphology, and optical properties of Copper Zinc Sulfide (CZS) films were investigated. The structural properties of Cu0.75Zn0.25S films were examined using the X-ray diffraction (XRD) technique as a function of annealed temperatures. XRD presented the Cu0.75Zn0.25S films as polycrystalline in the environment by a mixed hexagonal structure of CuS-ZnS, preferred orientation along the (201) plane, and crystallite size varying from 8.41- 23.28 nm with annealing temperature. Atomic force microscopy (AFM) analysis was used to investigate the morphological properties of Cu0.75Zn0.25S films; the grain size of these films varies with annealing temperature in the range of (58.39 to 139.42) nm with uniform distribution. The influences of annealing temperature on the optical characterization of Cu0.75Zn0.25S thin film were examined using UV-Vis absorption spectroscopy. Direct band gap values of Cu0.75Zn0.25S films are gained from optical absorption measurements with a range (2.3-1.8) eV as a function of annealing temperature. From the results obtained above, it appears to us that the temperature is the most suitable for practical applications, which directed that Cu0.75Zn0.25S thin film is suitable for solar cell applications. Keywords: CZS, Annealing temperature, Thin films, X-ray diffraction, AFM, Thermal evaporation. 1. Introduction CuZnS alloys are considered to have common structures of (ZnS) and (CuS), and due to the high absorptivity of these materials, they are used in the application of solar cells and photodetectors (1). The three elements, copper, zinc, and sulfur are non-toxic and easy to obtain due to their abundance in the Earth’s crust and their cheap price. In addition to their electrical and optical advantages, they are among the materials recommended for use in solar cells (2, 3). Chalcogenide semiconductors, including (CuS), have simple hexagonal crystal structures with lattice measurements, a = 3.79 Å and c = 16.36 Å (4) ZnS was an n-type semiconductor with energy gaps of around (~3.65 eV) (5). while CuS was a p-type semiconductor and had an energy gap of (1.63-1.87 eV) (6). CuS and ZnS are a mixed structure of two chalcogenide metal films, and samples with high copper content are used as an absorbent layer in optoelectronics and photovoltaic applications. Samples with low copper content are used as window/insulating https://creativecommons.org/licenses/by/4.0/ https://creativecommons.org/licenses/by/4.0/ https://orcid.org/0000-0002-5670-3966 mailto:ali.saud2104p@ihcoedu.uobaghdad.edu.iq https://orcid.org/0000-0002-1159-1008 mailto:boshra.k.h@ihcoedu.uobaghdad.edu.iq IHJPAS. 2025,38(2) 185 layers for solar cells (7, 8). The ternary compound alloy will be either n- or p-type and will have a wide energy gap (9,10). ZnS semiconductor is known to absorb UV radiation. 4% of practically all sunlight limits (11). For these important reasons, ZnS semiconductors are synthesized by thin band gap energy semiconductors such as CuS. In addition, CuS is more vulnerable to photo corrosion, this suggests protection across large band gap semiconductors (12). PN junctions were created, which are used in the semiconductors CuS (p-type) and ZnS (n-type) and have the advantage of increasing the lifetime of electrons in earlier recombinants. CuS/ZnS samples are utilized for photocatalytic ordering (13, 14). There are different techniques used by researchers to prepare CuZnS films for example chemically immersion deposits (8,15), pulse laser depositions (16), electrochemical deposition (17), photo chemical depositions (18,19), sol-gel technique (20) spray pyrolysis (3,22,23).and Successive ionic layer absorption (SILAR)(24). In this research, crystalline Cu0.75Zn0.25S thin films have been synthesized by thermal evaporated technique, that influences of annealed temperature (423,523, then 623) K on CZS characterization have been investigated for photo voltaic request. 2. Materials and Methods The ternary alloy (CZS) was formed from the elements copper and zinc, besides sulfide. The three elements were then mixed and placed in a quartz tube under pressure (3 * 10-4 mbar). The process was done. The tube was placed in an electric oven (1300 K) for more than six hours, at a temperature higher than the melted temperatures for CuS and ZnS, then cooled progressively. The three elements are of high purity (99.99%) in a ratio of 0.75:0.25:1. The physical method was used to prepare thin films by changing the weight ratio of the elements that make up the alloy (0.75:0.25:1(by thermal evaporation using (E 306). Before the deposition process began, using an ultrasonic bath with acetone, ethanol, and deionized water, the substrates were cleaned sequentially. Then, it was deposited in a glass substrate at room temperature with a thickness of 450±20 nanometers before being vacuum annealed at temperatures (423, 523, and 623) K in 60 minutes, where the morphological, structural, and optical properties were studied. XRD technique was used to characterize the structure of all films prepare used CuKα radiation greatest 2Ө from 20° to 80 °. Bragg’s law is utilized to consider interplanar spacing (d) of the Miller index (hkl) (25, 26). 2dsinθ=nλ (1) The crystalline size (C.S) of films was valued by utilizing Scherer’s Prescription (27,28). C.S= 0.94𝜆 𝛽𝐶𝑂𝑆𝜃 (2) Where λ: XRD wavelength, β: FWHM of the peaks, and θ: Bragg's angle. The dislocations density (δ) and Micro strain (Ԑ) were estimated by using the equations (3 and 4) respectively (29.30): δ = 1 (C.S)2 (3) Ԑ = B𝐶𝑂𝑆θ 4 (4) The morphology of the CZS film surface was examined by using AFM. The transmit and absorb spectrum was recorded to diversity (400-1100) nm to characterize optical properties for all films prepared. The optical energy gap of Cu0.75Zn0.25S thin films before and after annealing was calculated by using Tauc's equation: (31,32). (αhν)=D (hν -Eg) n (5) IHJPAS. 2025,38(2) 186 hν: the incident photons energy, D: is constant, n: is a number related to the type transition, and α: the absorption coefficient was predicted since absorbance (A) using the equation (33, 34) α= 2.303A 𝑡 (6) Where t: is film thickens. Optical constant values like refractive index (n) and extinction coefficient (K) were estimated by using equations (7, 8) respectively (35, 36): n = {[4R / (R-1)]-K2}1/2 – [(R+1) / (R-1)] (7) K= αλ 4π (8) Where (R) is reflectance that is intended through (36): R = 1-T-A (9) The loss tangent was estimated by using the equations (29): tanδ = εi/ εr (10) Where (εr, εi ): the real and imaginary parts of the dielectric constant which are calculated from the equations below (7, 37): εr = n2-K2 (11) εi =2nK (12) 3. Results and Discussion The crystalline structure of the prepared film was studied, and Figure 1 shows the XRD pattern of Cu0.75Zn0.25S with different annealing temperatures. All the films prepared before and after annealing had a polycrystal structure through lower crystallinity, hexagonal structures, and a mixed phase of CuS and ZnS. Comparison with the obtained XRD decorations shows that these shapes match the standard XRD reference patterns ZnS (JCPDS: 65-0309) and CuS (JCPDS: 06-0464). Since we do not have standard reference XRD patterns for the ternary CZS compound, the results are in very reasonable agreement with the JCPDS data. The entire film was diffracted at angle 2 (29.6737 °, 29.9 °, 29.7969 °, and 29.7818 °) earlier and then later annealed to see the corresponding (102) levels. In the figure, no distinct peaks appeared for the Cu, Zn, or S elements. The secondary peaks in the XRD pattern indicate the phase of ZnS and CuS, and the obtained results are consistent with the JCPDS data. After the annealing process, the peak positions change marginally. The intensity of the peaks increases, and the size of the crystals becomes larger after annealing. This suggests that the reduction of defects and regularity strengthens the crystalline films (28). Figure 1. XRD of Cu0.75Zn0.25S thin films at R.T and diverse annealed temperature. IHJPAS. 2025,38(2) 187 From Table 1 the calculation values show the density of dislocations (δ), microstrain (Ԑ), and crystallite size (C.S.) for Cu 0.75 Zn 0.25 S films. It appears that the value of the size of the nanocrystals increases with increasing annealing temperatures and the values of dislocation density and micro strain decrease after the annealing process. The reason is due to the improvement of the crystalline structure of the films in addition to the decrease in defects. It is also clear from the values in the table of the films (Cu 0.75 Zn 0.25 S) annealed at 623 K for one hour have a lower dislocation density, microstrain, and a higher crystalline size compared to other films. This can be attributed to the decrease in the full width at half maximum (FWHM) of the main peak, which ultimately leads to an increase in crystallinity. The size of these films (37). In addition to the observation of the dissimilarity in dislocated density, partial stress is inversely correlated with crystal size, a result that aligns with (21). Table 1. Structural limitations aimed at Cu 0.75 Zn 0.25 S thin film. Ta (K) dexp (Å) 2θexp (deg.) (hkl) FWHM (deg.) C.S (nm) δ*1016 (lines/m2) ε*10-3 R.T 423 3.00819 29.6737 102 1.02 0.7667 8.419517 11.20702 1.4106707 7.961957 8.419517 11.20702 2.97783 29.9 102 523 2.99603 29.7969 102 0.706 12.16765 6.7544 12.16765 623 3.0001 29.7818 102 0.3689 23.2856 1.844273 23.2856 Through AFM analysis, the effect of annealing temperature on the surface appearance of Cu 0.75 Zn 0.25 S thin films with a thickness of (450 nm) was studied at room temperature and next annealed by (423,523,623) K. The AFM images clearly illustrate the gradual dispersion of grains in CZS thin films at varying annealing temperatures. Figure 2 displays uniform grain surface morphology. As you can see in Table 2, the surface roughness values go up with the annealing temperature. They go from 0.953 nm for CZS thin films made at room temperature to 5.05 nm for CZS thin films annealed at 673 K. The surface morphology results presented in Table 2 indicate an increase in the average grain size from 58.39 nm to 139.42 nm after annealing, which aligns with the X-ray results. The root mean square (RMS) of roughness increases with increasing annealing temperature. All parameters were increased and then annealed, and then the samples annealed at 623 K had higher values. The performance was attributable to the enhancement of the films structurally and the increased movement of atoms. All parameters were increased and then annealed, and then the samples annealed at 623 K had higher values. The performance was attributed to the structural enhancement of the films and the increased movement of atoms, which led to the rearrangement and accumulation of molecules. And increases in the surface roughness of the film, which may play a good role in the performance of thin films for the photovoltaic cells. XRD results showed that the explanations were mostly correct, and there was also an increase in the film's surface roughness, which may be a good thing for the performance of thin films in photovoltaic cells. The explanations were in decent agreement with the XRD consequences, besides reference (37). IHJPAS. 2025,38(2) 188 Table 2. Roughness average, grain size, and Root mean square of Cu 0.75 Zn 0.25 S thin film. Ta (K) Grain size (nm) Roughness average (nm) Root mean square R.T 58.39 0.953 1.31 423 81.14 1.67 2.1 523 623 88.52 139.42 2.4 5.05 2.74 7.07 IHJPAS. 2025,38(2) 189 Figure 2. AFM descriptions of Cu0.75Zn0.25S films for diverse annealed temperature. It is clear to us from Figure 3 that the optical absorption spectra of Cu 0.75 Zn 0.25 S thin film were on wavelength variety (400-1000) nm at room temperature, besides once annealed by (423,523,623) K for 60 minutes. The absorbance values decrease with increasing wavelength, while they increase with cumulative annealing temperature. After annealing, this behavior shows that the optical transmittance values have gone down. These values depend a lot on the crystal structure, chemical composite, surface morphology, and film thickness. Increasing the annealing temperature may result in the size growth of crystallites, leading to reduced optical scattering, which is consistent with the AFM and XRD data. From this figure, the sample annealed at 623 K will have a high absorption value of approximately 80%, and all samples show high absorption in the visible region, which makes these films preferred materials for photovoltaic requests, and the behavior is consistent per studied (40, 7). The absorption coefficient of all films prepared evaluated from equation (6) was found to be (α > 104 cm-1) which means the allowed direct transition is promising to occur. Also notice that after annealing the absorption coefficient values increase, as publicized on Figure 3 on behalf of similar details indication earlier. Figure 3. Absorbance and absorption coefficients of Cu0.75Zn0.25S thin films versus wavelength before and after annealing. The optical energy gap of Cu0.75Zn0.25S thin films was calculated from the plot of (αhν)2 compared to hν using Tauc's equation as shown in Figure 4. This figure shows the optical energy gap reductions from (2.3 to 1.8) eV through cumulative annealed temperature shifted to lower photon energy. The variant in the optical band gap values may be correlated to the IHJPAS. 2025,38(2) 190 variation in crystallite size and grain boundaries; these values correspond to solar cell application and are in good agreement with (3, 7). Figure 4. Disparity (αhv)2 through photon energy besides optical energy gap for Cu0.75Zn0.25S thin films before and after annealing. Figure 5 demonstrates that the refractive index (n) values for Cu0.75Zn0.25S thin films varied with wavelength, indicating annealed temperatures, which can be attributed to differences in the film's structural features. Figure 5 demonstrates how variations in the film's structural features cause the refractive index (n) values to fluctuate with the wavelength of the Cu0.75Zn0.25S thin films, especially during annealed temperatures. Changes in preparation conditions and technology lead to behavioral changes in the refractive index, and several factors, including the type of material and the crystal structure, influence its value. Additionally, the roughness coefficient of the surface of the prepared film influences the refractive index values. It also demonstrates that all films exhibit peak-to-length movement. Figure 6 illustrates the less wave variation of extinction coefficient (k) values for the Cu0.75Zn0.25S thin film on R.T., which was then annealed at different temperatures. This figure illustrates a similar behavior of the absorption coefficient, with values increasing after annealing, as the extinction coefficient values primarily depend on the arrangement of the absorption coefficient values. Figure Figure 5. Refractive index contrasted with length for Figure 6. Extinction coefficient versus wave CZS C CZS thin films divers annealed temperature. For CZS thin films divers annealed temperature. IHJPAS. 2025,38(2) 191 The loss tangent (tanδ) for Cu0.75Zn0.25S thin films by way of purpose for annealed temperatures Figure 7 is evaluated from equation (10) which mainly depends on real (εr) and imaginary εi parts of the dielectric constant and denotes the characteristic debauchery of electromagnetic energy in the material into heat. This figure shows the loss factor (tanδ) values differ through wavelength from (0.01) to (0.35) contingent on grain size, structural defects, and lattice strain in the films. Figure 7. Variation loss tangent with wavelength for Cu0.75Zn0.25S thin films before and after annealing. 4. Conclusions In this work, the possibility of preparing Cu0.75Zn0.25S Nanocrystalline thin films with 450 nm thickness using the thermal evaporation method is deposited on a glass substrate before and after annealing at (423,523,623) K for one hour. The crystal structure of Cu0.75Zn0.25S films from the XRD study confirms that these films have mixed phases of CuS and ZnS and are polycrystalline hexagonal with preferential orientation along the (102) plane, and when increasing annealing temperatures caused enhanced film structures, the crystallite size increased and there was a small displacement in the spectrum curve towards high values of angle diffraction. The atomic force microscope (AFM) results show uniform distribution, and the annealing temperatures played an essential role in the grain size, which increased after annealing. Optical measurement results confirm the nature of electronic transitions for Cu0.75Zn0.25S films was allowed direct transition electronic, the absorbance values increased after annealing, the CZS thin films have high values of absorption coefficient, and the direct energy gap (Eg) decreased from 2.3 eV to 1.8 eV with increase annealing temperatures, which decreased towards the mid of the visible region, which makes Cu0.75Zn0.25S films suitable for photovoltaic application. Acknowledgment We thank the Thin Film Lab., Department of Physics, College of Education for Pure Science/ Ibn Al-Haitham, University of Baghdad. Conflict of Interests The authors declare that they have no conflicts of interest. IHJPAS. 2025,38(2) 192 Funding None. 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