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Surface Characterization of Nanostructured ITO Films of Oxygen Plasma Gas by Magnetron Sputtering for Dye-Sensitized Solar Cells Applications

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31 May 2024

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04 June 2024

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10 October 2024

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Abstract
The surface characterization of indium tin oxide (ITO) films was processed by oxygen (O2) plasma gas using a magnetron sputtering method of varying O2-plasma gas from 20 sccm to 100 sccm for potentially fostering in electronic devices applications on dye-sensitize solar cells (DSSC) in this work. In order to gain an outstanding performance rate with high-quality thin films, the affect of correlation between the electrical, optical, and morphology properties was significantly investigated. Clearly, the content of investigation exhibited that the films properties was changed by variation of the gas composition. These changes have contemporary relevance to the sputtering gas during the deposition process. To conclude, the greatest electrical properties was displayed by O2 -plasma gas flow rate of 20 sccm, which showed the lowest resistivity. In addition to this, the final products were practically fabricated to active layers for dye-sensitize solar cells (DSSC) applications. The highest efficiency of DSSC device was indicated of approximately 0.35% which was located by 40 sccm of the O2-plasma gas. Consequently, the study could be a possibility way of preparing ITO thin films with improved special properties of substantial applications for solar cells devices in the near future.
Keywords: 
Subject: Engineering  -   Energy and Fuel Technology

1. Introduction

Thin films technology has been recently studied in relation to their applications for the production of the electronic devices, for example thin films transistors (TFT), integrated circuit (I.C), and light-emitting diode [1,2,3]. In addition to this, thin films are an essential for the development of unique optical devices with exceptional films properties. Although these thin films were observed as the most interesting materials, the lack of stability noticed in electrical conductive applications was a barrier to practically used. Therefore, the next step in the development of thin films is required to overcome these problems. In replacement, there was found that the transparent conducting oxides (TCOs) has become the effective electrical conductive materials [4,5]. Normally, the TCOs are an expedient with thin films technologies and use in various optoelectrical devices, especially, solar cells [6,7]. However, the technical advanced for producing TCOs materials are constructively considered in nowadays. The TCOs materials could be characterized by introducing metallic elements to adjust the structural such as tin (Sn) [8], aluminum (Al) [9], zinc (Zn) [10] and indium (In) [11]. Of these element replacement types, indium tin oxide (ITO) optimizes a superior substitution for the TCOs materials [12,13]. ITO is typically consisted of indium (III) oxide (In2O3) and tin (IV) oxide (SnO2) which commercially exhibits outstanding conductivity, low sheet resistivity and high transparency [14,15]. General deposition methods of thin films could be prepared by different methods, for instance, electron beam evaporation [16], thermal evaporation [17], pulsed laser deposition (PLD) [18], ion assisted plasma evaporation [19], as well as sputtering [20,21,22]. Among these deposition processes, sputtering is an appropriate method for a preparation of the thin films. Inherently, sputtering is a method of making thin films in a few nanometers on the need substrate which offers more advantages than others. As the advantageous, there are a supportive of creating large areas films for several industrial applications, gaining for high-quality oxide films of complex oxides as well as importantly effective cost than other methods [23,24]. For this, the most resourceful focus for growing thin films by sputtering method is the use of a magnetron source. In which, the generation of plasma with an enhanced glow discharge is importantly applied [25]. Hence, the active gas of plasma generation reacts with the thin films and in the deposition atmosphere. For the deposition atmosphere, oxygen plasma has become interested that is generated by utilizing an oxygen (O2) on plasma system. Due to its effective, oxygen plasmas show a wide application in modifying surface functional for nanoelectronics device fabrication [26,27,28,29]. However, the desired properties of thin films are determined by the technique utilized together with deposition parameters, for example films materials, substrate, and deposition rate that could be provided vital properties like electrical and optical [30].
In this work, the goal is to study the physical and electrical properties of nanostructured on ITO films prepared via the magnetron sputtering method through the sputtering O2 plasma gas. To obtain the optimum growth parameters to applied with DSSC devices, the variation on O2 gas flow rate of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm were compared to find excellent results. Thus, the obtained of films products will be beneficial of new method for producing in solar cell industry.

2. Experimental Set Up

The ITO coated glass substrates with a thickness of 0.7 mm (Lumtec., Taiwan) and sheet resistance of 9 to 15 Ω/sq were experimentally used in this study. The first stage in the sputtering process of ITO films was to wiped using pro-wipe paper (Elleair., Japan), which then was dipped into acetone for 3 minutes using ultrasonic cleaner machine (Tullker Co., Ltd.) to remove any contamination and surface oils before the sputtering process. After that, the ITO substrates were faithfully placed in the vacuum chamber (SUS304) to drive the sputtering process by magnetron sputtering machine. Figure 1 illustrates the equipment employed to O2 plasma gas sputtered on ITO substrates. Looking in more detail in Figure 1, the distance between target and ITO substrate was set by 8 cm, and the room temperature was maintained by cooling system. The ITO surface was sputtered by O2-plasma gas under the gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively. The power used for sputtering process was set at 50 W, along with the chamber was pumped down to 8.6x10-6 Torr or lower exhausted of the sputtering chamber.
The structural, optical, and electrical properties of ITO thin films were precisely investigated. The structural properties of the ITO thin films sputtered by oxygen plasma gas was studied by X-ray diffraction (XRD) (Rigaku D/max 2100H) that was scanned in a 2 θ range of 10°–70° along with a monochromatized Cu Kα radiation indicating λ = 1.5418 Å. The UV-VIS spectrophotometer (Hitachi, U-3000) in the range of 200-2000 nm was used to measure the optical transmittance spectra of ITO thin films. And the field emission scanning electron microscope (FE-SEM) (JEOl, JSM-7610F) was applied to quantify the morphological of the films. In addition to this, the four-point probe method (DASOL ENG FPP-HS-8) and Hall effect measurement (ECOPIA HMS-2000) were used to analyze the electrical properties.

3. Results and Discussion

Transparent conducting oxides (TCOs) have been designed to improve the films properties, including high transparency and low resistivity. Therefore, to provide nanostructured ITO films with the desired of properties, the ITO films was sputtered through O2-plasma gas by magnetron sputtering method to enhance the efficiency of light transmittance and electrical conductivity. Note that the arrangements of less crystallized or amorphous in a crystalline structure have an effect to the electrical properties causing high resistivity of the films [31]. Therefore, the improvement of ITO films is an absolutely necessary. In this study, the analysis of nanostructured ITO films sputtered by O2-plasma gas using sputtering technique was presented.

3.1. Effects of O2 Plasma Gas Flow Rate on Properties of Nanostructured ITO Films

According to the previous studied, Zhong Zhi You et al. [31] reported the etching of ITO thin films by oxygen plasma. The results showed that the O2 plasma gas has an oblivious effect to the nanostructured ITO films which could be change the stoichiometry of ITO surface that boosts the surface free energy (SFE) and improving wetting condition. Therefore, the effect of the gas flow rate in O2 plasma gas at 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm were studied by sputtering technique following to the experimental parameters in Table 1. As can be seen in the table, the sputter deposition parameters for O2 plasma gas were illustrated that affects to the properties of structure, physical, transmittance, electrical of ITO films as following.

3.2. Crystal Structure

The x-ray diffraction pattern of nanostructured ITO films with the As-deposited (ASD) and after sputtered by O2-plasma gas flow rate of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively as shown in Figure 2. The result showed that the x-ray diffraction pattern of nanostructured ITO films presented the (222) and (440) plane in 2θ which showed the angle by 30.7° and 51.3°, respectively. By considerable the intensity of peaks on (222) and (440) plane, there have been found that when the gas flow rate increased, the XRD peak intensity did not change. This mean that the orientation of ITO nanostructured films was constant which corresponded to the previous study of Chen et al. [32]. In this researcher group, they studied the effect of time treatment by oxygen plasma on ITO thin films which found that there was not change in the crystal structure of thin films.

3.3. Surface Morphology

In this section, the FE-SEM technique was exploited to characterize separately the surface structure of nanostructured ITO films sputtering by the difference O2-plasma gas flow of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm. The cross-sectional area of nanostructured ITO films was shown by Figure 5. The detailed reveals the growths of ITO nanorod films at different O2 -plasma flows. Figure 5a presents the area– selective deposition (ASD) films, along with Figure 5b–f showing sputtered films of O2-plasma gas flow from 20 sccm to 100 sccm. For additional information, FE-SEM images of the top surface nanostructured ITO films were displayed in Figure 6. Simultaneously, the ITO samples were provided by magnetron sputtering technique under O2-plasma gas flow of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, individually. As observed by FE-SEM technique, the grain size was invariable with the sputtering by O2-plasma gas which can be seen in Figure 6a–f.
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Figure 3. Physical ITO substrates before processing by variation of sputtering gas flow from 20 sccm O2-plasma gas to 100 sccm O2-plasma gas.
Figure 3. Physical ITO substrates before processing by variation of sputtering gas flow from 20 sccm O2-plasma gas to 100 sccm O2-plasma gas.
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Figure 4. Magnetron sputtering system preparing nanostructured ITO films using by variation of sputtering gas flow from 20 sccm O2-plasma gas to 100 sccm O2-plasma gas.
Figure 4. Magnetron sputtering system preparing nanostructured ITO films using by variation of sputtering gas flow from 20 sccm O2-plasma gas to 100 sccm O2-plasma gas.
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Figure 5. Cross-sectional FE-SEM images of the O2-plasma gas sputtered/nanorods to ITO films by magnetron sputtering technique at various plasma gas flow: (a)ADS films ; (b) 20 sccm O2-Plasma gas; (c) 40 sccm O2-Plasma gas; (d) 60 sccm O2-Plasma gas; (e) 80 sccm O2-Plasma gas; (f) 100 sccm O2-Plasma gas.
Figure 5. Cross-sectional FE-SEM images of the O2-plasma gas sputtered/nanorods to ITO films by magnetron sputtering technique at various plasma gas flow: (a)ADS films ; (b) 20 sccm O2-Plasma gas; (c) 40 sccm O2-Plasma gas; (d) 60 sccm O2-Plasma gas; (e) 80 sccm O2-Plasma gas; (f) 100 sccm O2-Plasma gas.
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Figure 6. Top surface FE-SEM images of the O2-plasma gas sputtered/nanorods to ITO films by magnetron sputtering technique at various plasma gas flow: (a) ASD films ; (b) 20 sccm O2-Plasma gas; (c) 40 sccm O2-Plasma gas; (d) 60 sccm O2-Plasma gas; (e) 80 sccm O2-Plasma gas; (f) 100 sccm O2-Plasma gas.
Figure 6. Top surface FE-SEM images of the O2-plasma gas sputtered/nanorods to ITO films by magnetron sputtering technique at various plasma gas flow: (a) ASD films ; (b) 20 sccm O2-Plasma gas; (c) 40 sccm O2-Plasma gas; (d) 60 sccm O2-Plasma gas; (e) 80 sccm O2-Plasma gas; (f) 100 sccm O2-Plasma gas.
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Based on the FE-SEM images, the average values of length and diameter of the nanorods were analyzed and measured summarizing in Figure 7. Once the O2 plasma gas was enhanced, Gaussian distribution [––] was applied to calculate the average values under the difference conditions of O2 plasma gas. In this, the calculation results were shown in Figure 7. To consider a vital change on the ITO nanorods films quality, the ASD films and sputtered films were essentially compared by focusing on the effect of films surfaces. The performance illustrates that has a small effect on ITO nanorods films as the O2-plasma gas of sputtering process varied. Remarkably, the nanorods size distribution was ranged by around 199-211 nm in length with O2 plasma gas variation. However, the size of ITO nanorods films slightly decreased with changing the O2-plasma gas flow rates, while O2-plasma gas did not affect the crystallinity of ITO nanorods films. As well as this, the average diameter of nanorods was in the range of about 50-63 nm. Hence, this is possible to verify the exceptional change in the sputtering rates of O2-plasma gas due to the obtained results of ITO nanorods films investigation.

3.4. Optical Transmittance

In order to demonstrate the trait of studied optical transmittance, the transmittance values in the visible region were accurately measured through the spectrophotometer devices in the wavelength range 250-2000 nm. In this process, the study take advantage of the ITO films that coated on glass substrates, receiving ITO-TF/Glass to extensively investigate the average transmittance of substrates. Accordingly, experimental results of the ITO glass, ASD films and O2 sputtered films used the comparison in O2 flow conditions such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm which showed the graph trend in Figure 8. The results appeared that the ITO-TF/Glass films with surface sputtering presented the high optical transmittance and similar in each condition of O2 flows. The measurement explored the surface properties of an average transmittance values of all samples was above 85% in the wavelength of visible light ranges from 380 to 750 nm. In terms of wavelength, the overall visible light wavelength was throughout range of 400-700 nm. This effect was corresponded to the variations of O2-plasma gas 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm on substrates by magnetron sputtering technique.
Furthermore, the study proposed the enhancement of the characteristic discussion of the difference substrates comparing to O2 plasma sputtered, including glass, ASD films, and ITO commercial which can be seen in Figure 9. The characterization was found that the optical transmittance quality tended to decline from 88.5% to 87% and continuously dropped to 85.5% under the O2-plasma gas flow rates of 20 cm3/min, 40 cm3/min, respectively. According to this, the process involved that the light transmittance values was obtained when a surface was bombarded with positive ions of oxygen. Note that the energy ion bombarded of the surface caused the decreased to the light transmittance values, resulting in occurring of oxygen vacancy gap. On the other hand, at O2-plasma gas flow rates of 60 sccm, 80 sccm, and 100 sccm did not impact to the values of light transmittance in visible region. This may be caused by more collisions of oxygen positive ions, leading to the decreasing of energy of oxygen ions.
In particular, the performance capabilities of ITO-TF/Glass, ASD films, and O2-plasma sputtered films at different experimental conditions of O2-plasma gas flow rates such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm was analyzed in terms of the omnidirectional characteristic that was maintained over a wide range of angles of incidence between 0 and 80 degrees. For this, Figure 10 displayed a transmission spectrum with different wavelengths, including 500 nm (Figure 10a, 600 nm (Figure 10b), and 700 nm (Figure 10c) in the graph form. Looking the graph in more detail, the optical transmission spectra at the various angles of incidence obviously indicated the similar results for overall samples. To compare the optimal experimental state, the outcome clearly identified that the samples with O2-plasma sputtered had higher optical transmission than the ITO-TF/Glass. For that reason, the performance could be summarized that nanostructured ITO films with O2-plasma sputtered offered a suitable alternative to use for active layer fabrication on TCO materials in DSSC application.

3.5. Electrical Properties

According to measured samples from ITO glass, ASD films, ITO-TF/Glass as well as O2 plasma sputtered films at O2-plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm preparing by magnetron sputtering technique, the greatest electrical conductivity was shown by ITO-TF/Glass substrate. In Figure 11, the data illustrated that the sheet resistance of ITO-TF/Glass was found to be decreased dramatically with the O2-plasma gas flow rate of 20 sccm. Conversely, at O2-plasma gas flow rates 40 sccm, the sheet resistance on ITO-TF/Glass substrate was sharp increased. Another, the sheet resistance at O2-plasma gas flow rates from 60 sccm to 100 sccm was quite constant. Nonetheless, the samples of O2 plasma sputtered films at O2-plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm exhibited more higher sheet resistance values than the ASD films. Based on the above mentioned, at 20 sccm O2-plasma gas flow was the most effective in changing properties of ITO-TF/Glass, which showed the lowest sheet resistance. In this case, the effective electrical properties resulted from ion oxygen bombardment on the surface. This was a beneficial to the removal of contaminants on the surface of the films.
Moreover, finial ITO films products were obtained through successive applications for DSSC devices. Next section, the efficiency of DSSC was discussed by focusing on ASD films and O2 plasma sputtered films at O2-plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm preparing by magnetron sputtering technique.

3.6. The Applicatins of Nanostructured ITO Thin Films on O2 Plasma Gas Sputteres to TCO Materials for DSSC Devices

The TCO layers in DSSCs act as a layer that permit incident light to enter the photoanode and counter electrode. The application of nanostructured ITO films was constructed by using O2 plasma gas sputtered at the gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm for applying as an active layer of DSSC devices. In order to explore the DSSC properties, voltage drop, and current were investigated to determine the efficiency (%Eff) of DSSCs which could be explained as following.

3.7. The Improvent of DSSC Devices with Nanostructured ITO Thin Films on O2 Plasma Gas Sputtered at Flow Rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm to TCO Materials for DSSC Devices

The efficiency of DSSC applied with nanostructured ITO films of O2 plasma gas sputtered films at the flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, showing in Figure 12. There have been found that when increasing the gas flow rate, the efficiency of DSSCs was increased. However, when investigating the O2 plasma treated films at the gas flow rate of 60 sccm, 80 sccm, and 100 sccm, the efficiency of DSSCs was declined gradually. Especially, the DSSCs applied with nanostructured ITO films of O2 plasma gas sputtered films at 40 sccm gas flow rate exhibited the highest efficiency of 0.35%.

4. Conclusions

The surface characterization of nanostructured ITO films with O2-plasma gas was entirely reviewed in the study. The effects of O2-plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm influenced on the structural, morphological, optical, and electrical properties was mainly studied. According to the obtained results, the using of O2 -plasma gas did not effect to the surface structural of ITO nanorods films (size and diameter) growth on ITO thin films. In this case, the sheet resistance was increased when oxygen gas flow rate rising, however, transmittance properties in the visible region was slightly plummeted. In addition to this, the usable of nanostructured ITO films with O2 plasma sputtered in various O2 plasma gas flow rates from 20 sccm to 100 sccm for DSSC applications was feasibility contributed. The results showed that the O2-plasma sputtered was ability to improve the efficiency of DSSC by varying plasma gas flows. Thoroughly, the highest percentage of DSSC efficiency was given by 40 sccm O2 gas flow rate. On the contrary, at 60 sccm, 80 sccm, and 100 sccm O2 plasma gas was constantly declined. Eventually, the result of this work grants the capability of satisfactory fabrication on thin films technology for active layers designs in solar cells industry in the future.

Author Contributions

Conceptualization, W.P. and N.M.; methodology, S.A.; software, T.T.; validation, X.X., Y.Y. and W.P. and N.K.; formal analysis, S.A and T.T..; investigation, A.S.; resources, N.K.; data curation, W.P.; writing—original draft preparation, N.M. and A.S.; writing—review and editing, S.A.; visualization, T.M.; supervision, N.K. and N.K.; project administration, N.M.; funding acquisition, All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by the Royal Golden Jubilee (RGJ) Ph.D scholarship from the National Research Council of Thailand under the Ministry of Higher Education, Science, Research, and Innovation, grant number N41A650091.

Acknowledgments

The authors would like to thank School of Energy Environment and Materials under Energy Technology program, King Mongkut’s University of Technology Thonburi (KMUTT), Bangkok, Thailand.

Conflicts of Interest

The authors declare no conflicts of interest.

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Figure 1. Schematic diagram showing magnetron sputtering system applied to provide nanostructured ITO films of varying O2-plasma gas such 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively at 50 W of power supply.
Figure 1. Schematic diagram showing magnetron sputtering system applied to provide nanostructured ITO films of varying O2-plasma gas such 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively at 50 W of power supply.
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Figure 2. The X-ray pattern diffraction of nanostructured ITO films between ASD films and sputtered films of varying O2 plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm.
Figure 2. The X-ray pattern diffraction of nanostructured ITO films between ASD films and sputtered films of varying O2 plasma gas flow rates of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm.
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Figure 7. Information of the average length and diameter of ITO nanorods films proving by magnetron sputtering technique at different the O2-plasma gas flow rates from 20 sccm–100 sccm.
Figure 7. Information of the average length and diameter of ITO nanorods films proving by magnetron sputtering technique at different the O2-plasma gas flow rates from 20 sccm–100 sccm.
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Figure 8. Optical transmission spectra of the ITO glass, ASD films, and O2 sputtered films at different experimental conditions of O2-plasma gas flow rates such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm preparing by magnetron sputtering technique.
Figure 8. Optical transmission spectra of the ITO glass, ASD films, and O2 sputtered films at different experimental conditions of O2-plasma gas flow rates such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm preparing by magnetron sputtering technique.
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Figure 9. Average value of light transmittance values in the visible region of glass, ASD films and ITO commercial proving by magnetron sputtering technique of varying O2-plasma gas flow rates, 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm.
Figure 9. Average value of light transmittance values in the visible region of glass, ASD films and ITO commercial proving by magnetron sputtering technique of varying O2-plasma gas flow rates, 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm.
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Figure 10. Transmittance spectrum curves of the omnidirectional characteristics at 500 nm, 600 nm and 700 nm comparing to ITO-TF/Glass, ASD films, and O2 sputtered films at different experimental conditions of O2-plasma gas flow rates such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm: (a) 500 nm wavelength; (b) 600 nm wavelength; (c) 700 nm wavelength.
Figure 10. Transmittance spectrum curves of the omnidirectional characteristics at 500 nm, 600 nm and 700 nm comparing to ITO-TF/Glass, ASD films, and O2 sputtered films at different experimental conditions of O2-plasma gas flow rates such as 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm: (a) 500 nm wavelength; (b) 600 nm wavelength; (c) 700 nm wavelength.
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Figure 11. Sheet resistance of ITO-TF/Glass for various O2-plasma gas flow rates, 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm by magnetron sputtering technique.
Figure 11. Sheet resistance of ITO-TF/Glass for various O2-plasma gas flow rates, 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm by magnetron sputtering technique.
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Figure 12. The efficiency of DSSC devices applied to nanostructured ITO thin films at oxygen gas flow rate of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively.
Figure 12. The efficiency of DSSC devices applied to nanostructured ITO thin films at oxygen gas flow rate of 20 sccm, 40 sccm, 60 sccm, 80 sccm, and 100 sccm, respectively.
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Table 1. Sputter parameters for O2-plasma gas sputtered on nanostructured ITO films.
Table 1. Sputter parameters for O2-plasma gas sputtered on nanostructured ITO films.
Parameter Determine
Pressure (before deposition) 8.6×10−6 Torr
Pressure (during deposition) 2.6×10−2. Torr
Time 5 minutes
Power 50 Watt
Oxygen gas flow rate 20, 40, 60, 80 and 100 sccm
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Copyright: This open access article is published under a Creative Commons CC BY 4.0 license, which permit the free download, distribution, and reuse, provided that the author and preprint are cited in any reuse.
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