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Optical and Surface Morphology Study of NiO Thin Films for Optoelectronic Applications

 Optical and Surface Morphology Study of NiO Thin Films for Optoelectronic Applications

Anil Rakshe1,2, Satish N. Vaishnav3, and Sudam D. Chavhan1*

1Department of Physics, V. V. M.’s Sitaram Govind Patil Arts, Science and Commerce College, Sakir, Dist.-Dhule. Maharashtra, Pin-424304, India

2Nutan Maharashtra Institute of Engineering & Technology, Pune, Maharashtra-410507, India

3Department of Chemistry, Sardar Vallabhbhai Patel Arts and Science College, Ainpur Tal. Raver, Dist.-Jalgaon, Maharashtra, Pin-425507, India.

Corresponding author:sudam1578@gmail.com

 

Abstract

Nickel oxide (NiO) thin films were deposited on indium tin oxide (ITO) substrates using a low-cost sol–gel spin-coating technique. The annealing treated NiO films  resulted in uniform and optically transparent films. UV–visible absorption studies showed strong ultraviolet absorption and 90 %  transparency in the visible region. The optical band gap, determined from the Tauc plot assuming a direct allowed transition, was estimated to be 3.35 eV, indicating good optical quality. Atomic force microscopy revealed a continuous, crack-free surface with homogeneously distributed nanoscale grains. The films exhibited a root-mean-square surface roughness of 24.28 nm, which is favorable for efficient charge transport and improved interfacial contact. The combined optical transparency and controlled surface morphology highlight the potential of sol–gel-derived NiO thin films for optoelectronic applications, particularly as hole-transport layers in solar cells and organic light-emitting diode.

Key words: NiO Thin Films, Sol-gel method, Optical band gap.

 

 

 

 

 

 

 

1.      Introduction

Nickel oxide (NiO) is p-type semiconductor material that has attracted considerable attention owing to it’s a wide-optical band-gap i.e 3.4-4.0 eV, excellent chemical stability, and environmentally benign nature. It is one of the promising materials for optoelectronic devices, particularly solar cells, Organic Light-emitting diode and transparent transistors [1–3].  Moreover, its low-cost processing feasibility is more technically appealing to compete with existing materials. And therefore, it is vitally important to study the optical and surface morphological features of NiO thin films prepared by low-cost deposition technique such as, sol-gel, chemical bath deposition and electrochemical deposition.

The optical performance of NiO thin films, including transmittance, absorption coefficient, and optical band gap, plays a decisive role in determining their suitability for transparent and optoelectronic applications. High transparency in the visible region combined with a sharp absorption edge is essential for minimizing optical losses in device architectures [5,6]. At the same time, surface morphological characteristics such as grain size, surface roughness, and film uniformity critically influence charge transport, light scattering, interface quality, and surface-related phenomena [7,8]. Therefore, simultaneous investigation of optical and surface morphological properties is essential for understanding structure–property relationships in NiO thin films.

NiO thin films have been fabricated using a variety of physical and chemical deposition techniques, including sputtering, pulsed laser deposition, chemical vapor deposition, spray pyrolysis, chemical bath deposition, and solution-based routes [9–11]. While physical vapor deposition methods are capable of producing dense and highly crystalline films, they generally require high vacuum conditions, elevated processing temperatures, and expensive instrumentation, which limit their applicability for large-area and low-cost production. Consequently, solution-based chemical techniques have gained increasing attention due to their simplicity, scalability, and compatibility with low-temperature processing.

Among solution-based approaches, the sol–gel method has emerged as a particularly attractive route for the preparation of NiO thin films. The sol–gel process enables molecular-level mixing of metal precursors, resulting in excellent compositional homogeneity and precise control over film stoichiometry [12–14]. In addition, sol–gel deposition techniques such as spin coating allow uniform film formation over large substrates using relatively simple experimental setups. The processing parameters such as solvent concentration, spin coating speed and annealing temperature can be easily optimized to make more suitable for solar cell and OLED applications [15, 16].

Despite the growing number of reports on NiO thin films, a comprehensive correlation between optical properties and surface morphological features for sol–gel-deposited NiO films remains limited. Many studies focus either on optical characterization or on structural and sensing behavior, without providing an integrated understanding of how sol–gel processing parameters simultaneously influence optical response and surface topology. Such combined analysis is crucial for optimizing film properties and advancing practical device integration.

Keeping in mind these points, the present manuscript focuses on the preparation of NiO thin films using the sol–gel method and a comprehensive investigation of their optical and surface morphological properties. Particular emphasis is placed on establishing correlations between sol–gel processing parameters and surface morphology with the aim of providing insights for optimizing NiO thin films for applications in solar cells and OLEDs.

 

2.      Experimental Details

Indium tin oxide (ITO)-coated glass substrates were used to deposited NiOₓ thin films. The substrates were thoroughly cleaned by following standard procedure of ITO i.e.  ultrasonication in detergent solution, deionized water, acetone, and isopropyl alcohol for 10 min each. After cleaning, the substrates were dried using a nitrogen stream and subjected to UV–ozone treatment to remove residual organic contaminants and improve hydrophilicity of ITO surface. A 0.2 M solution of nickel formate dihydrate was dissolved in ethylene glycol under continuous magnetic stirring. To this solution, ethylenediamine was added in a stoichiometric amount corresponding to two molar equivalents with respect to nickel ions. The resulting mixture was stirred at temperature > 90 °C for 2 hours. Prior to film deposition, the solution was allowed to cool to room temperature and subsequently filtered through a 0.45 µm nylon syringe filter to remove any undissolved particulates. The filtered solution was dropped onto the ITO substrates and spin-coated with optimized spin coating recipe. The four layers of spin coated nickel precursor films were then annealed at 325oC for 1 hour in muffle furnace to remove organic residue and form the NiO phase. After annealing the films were treated with UV-ozone light to 15 min to improve the electronic properties of the deposited NiO films. Optical properties of the deposited films were measured using UV-Visible spectrophotometer (JASCO v-600). The surface morphology was carried out using atomic force microscopy (AFM) in tapping mode using a Si tip.

Result and Discussion

Figure 1 (a) shows the atomic force microscopy (AFM) image of annealed NiO thin film prepared by sol-gel method. It indicate that formation of nanocrystalline NiO thin films. The films surface is continuous and without any cracks, confirming good coverage of the substrate.  The AFM topographical images reveal the presence of uniformly distributed nanoscale grains across the film surface. These grain-like features are typical of sol–gel-derived metal oxide thin films and originate from the nucleation and growth of NiO nanocrystallites during the thermal annealing process.

 

 

 

 

 

 

 

 

 

 

 

 

 

 


Figure 1:  Atomic force microscopic image of NiO thin films (a) surface topography and (b) surface roughness analysis.

The films exhibit a relatively smooth surface with low root-mean-square (RMS) roughness, reflecting the effectiveness of the sol–gel deposition combined with optimized spin-coating and annealing conditions. Quantitative roughness analysis, such as average roughness (Rₐ) equals to 17.74 nm and RMS roughness (Rq) equals to 24.28 nm further confirms the smooth surface morphology of the NiO thin films as shown in figure 1(b). The low surface roughness and uniformly deposited NiO films are potentially useful to fabricate highly efficient organic solar cell and organic light-emitting diodes. The smooth morphology reduces the density of surface defects and grain-boundary-related trap states, thereby facilitating efficient hole transport through the NiO layer. In addition, the uniform surface improves interfacial contact with adjacent functional layers, which is critical for minimizing contact resistance and enhancing charge extraction in optoelectronic devices. These morphological characteristics suggest that the prepared NiO thin films are well suited for application as hole-transporting layers in solar cells and organic light-emitting diodes. Therefore, atomic force microscopy study confirm that the sol-gel method is a reliable and low-cost approach for fabricating highly uniform NiO thin films.

Figure 2 (a) shows the optical absorption of NiO thin films grown on ITO substrate by using sol-gel method. The optical absorption spectra of the NiO thin films annealed at 325 °C for 1h were recorded in the ultraviolet–visible (UV–Vis) wavelength range to evaluate their optical behavior. The films exhibit strong absorption in the ultraviolet region, while maintaining low absorption in the visible range, indicating around 90% optical transparency in the visible region. This absorption characteristic is typical of wide band gap p-type NiO thin films. A sharp absorption edge is observed below 350nm wavelength, suggesting good film quality and improved crystallinity after thermal annealing. The annealing treatment at 325 °C promotes the decomposition of organic residues and enhances the formation of the NiO phase, which results in reduced defect density and improved optical uniformity. The weak absorption in the visible region confirms that the sol-gel prepared NiO thin films are one of the alternatives for p-type organic hole transporting materials and will be more promising candidate to play the efficient role of hole-transporting material in third generation solar cells and solution processed organic light-emitting diodes.

The optical band gap of the NiO thin films annealed at 325°C for 1h was determined using the Tauc relation as shown in figure 2(b). The absorption coefficient (α) was calculated from the measured absorbance, and the optical band gap energy (Eg) was estimated by plotting

(𝛼𝜈)2 as a function of photon energy (hν), assuming a direct allowed electronic transition for NiO. The linear region of the Tauc plot was extrapolated to intersect the photon energy axis, where (𝛼𝜈)2 = 0. The Tauc plot exhibits a well-defined linear region, indicating a direct band gap transition and good optical quality of the NiO thin films. The calculated optical band gap value was found to around 3.30 eV which is within the range of reported NiO thin films. The sharpness of the absorption edge and the linearity of the Tauc plot suggest reduced structural disorder and a lower density of localized states within the band gap because of the thermal annealing of NiO films at 325 °C for 1 hour. The annealing process facilitates the removal of residual organic components and enhances the formation of the NiO phase, leading to improved crystallinity and electronic structure. As a result, the observed band gap value is consistent with improved film quality.

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

Figure 2: (a) Optical absorption, and  (b) Tauc plot  of ITO/NiO thin filims  annealed at  325oC for 1 hour.

Conclusions

In the present study, pin-hole free and highly uniform NiO thin films were successfully fabricated by a spin-coating methods. The annealed NiO films exhibit strong ultraviolet absorption around 350nm wavelength and 90 % transparency in the visible region. The wide optical band of 3.35 eV obtained from Tauc plots corroborates its special feature of transparent metal oxide semiconductor properties. Analysis of surface morphology of NiO thin films via AFM analysis revealed a smooth, uniform surface with homogeneously distributed nanoscale grains having surface roughness of around 24.28 nm, which is excellent for efficient charge transport and enhanced interfacial contact. These results demonstrate that sol–gel-processed NiO thin films possess the essential optical transparency and surface uniformity required for hole-transport layers, making them promising for application in solar cells and organic light-emitting diodes.

 

Acknowledgment

This paper is respectfully dedicated to the Hon. Principal Dr. R. R. Ahire of Vidya Vikas Mandal’s Sitaram Govind Patil Arts, Science and Commerce College, Sakri, on the occasion of his superannuation, in recognition of his visionary leadership, unwavering commitment to academic excellence, and lifelong service to education. The authors express their heartfelt gratitude to Prof. Ellen Moons, Department of Physics and Engineering, Karlstad University, Karlstad, Sweden, for her invaluable guidance, constant encouragement, and generous experimental support, which greatly enriched the present work.

 

 

 

 

 

 

 

 

 

 

 

 

 

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