Deposition of Al-doped ZnO films on polyethylene naphthalate substrate with radio frequency magnetron sputtering

100 nm Al-doped ZnO (AZO) thin films were deposited on polyethylene naphthalate (PEN) substrates with radio frequency magnetron sputtering using 2 wt.% Al-doped ZnO target at various deposition conditions including sputtering power, target to substrate distance, working pressure and substrate temperature. When the sputtering power, target to substrate distance and working pressure were decreased, the resistivity was decreased due to the improvement of crystallinity with larger grain size. As the substrate temperature was increased from 25 to 120 °C, AZO films showed lower electrical resistivity and better optical transmittance due to the significant improvement of the crystallinity. 2 wt.% Al-doped ZnO films deposited on glass and PEN substrates at sputtering power of 25 W, target to substrate distance of 6.8 cm, working pressure of 0.4 Pa and substrate temperature of 120 °C showed the lowest resistivity (5.12 × 10^− 3 Ω cm on PEN substrate, 3.85 × 10^− 3 Ω cm on glass substrate) and high average transmittance (> 90% in both substrates). AZO films deposited on PEN substrate showed similar electrical and optical properties like AZO films deposited on glass substrates.     

Properties of indium tin oxide films deposited on unheated polymer substrates by ion beam assisted deposition

The optical, electrical and mechanical properties of indium tin oxide (ITO) films prepared on polyethylene terephthalate (PET) substrates by ion beam assisted deposition at room temperature were investigated. The properties of ITO films can be improved by introducing a buffer layer of silicon dioxide (SiO₂) between the ITO film and the PET substrate. ITO films deposited on SiO₂-coated PET have better crystallinity, lower electrical resistivity, and improved resistance stability under bending than those deposited on bare PET. The average transmittance and the resistivity of ITO films deposited on SiO₂-coated PET are 85% and 0.90 × 10^− 3 Ω cm, respectively, and when the films are bent, the resistance remains almost constant until a bending radius of 1 cm and it increases slowly under a given bending radius with an increase of the bending cycles. The improved resistance stability of ITO films deposited on SiO₂-coated PET is mainly attributed to the perfect adhesion of ITO films induced by the SiO₂ buffer layer.     

Effect of inserting a buffer layer on the characteristics of transparent conducting impurity-doped ZnO thin films prepared by dc magnetron sputtering

In transparent conducting impurity-doped ZnO thin films prepared on glass substrates by a dc magnetron sputtering (dc-MS) deposition, the obtainable lowest resistivity and the spatial resistivity distribution on the substrate surface were improved by a newly developed MS deposition method. The decrease of obtainable lowest resistivity as well as the improvement of spatial resistivity distribution on the substrate surface in Al- or Ga-doped ZnO (AZO or GZO) thin films were successfully achieved by inserting a very thin buffer layer, prepared using the same MS apparatus with the same target, between the thin film and the glass substrate. The deposition of the buffer layer required a more strongly oxidized target surface than possible to attain during a conventional dc-MS deposition. The optimal thickness of the buffer layer was found to be about 10 nm for both GZO and AZO thin films. The resistivity decrease is mainly attributed to an increase of Hall mobility rather than carrier concentration, resulting from an improvement of crystallinity coming from insertion of the buffer layer. Resistivities of 3 × 10^− 4 and 4 × 10^− 4Ω cm were obtained in 100 nm-thick-GZO and AZO thin films, respectively, incorporating a 10 nm-thick-buffer layer prepared at a substrate temperature around 200 °C.     

Effect of deposition parameters and annealing temperature on the structure and properties of Al-doped ZnO thin films

Transparent conductive films of Al-doped ZnO (AZO) were deposited onto inexpensive soda-lime glass substrates by radio frequency (rf) magnetron sputtering using a ZnO target with an Al content of 3 wt%. The Taguchi method with a L₉ orthogonal array, signal-to-noise (S/N) ratio and analysis of variance (ANOVA) were employed to examine the performance characteristics of the coating operations. This study investigated the effect of the deposition parameters (rf power, sputtering pressure, thickness of AZO films, and substrate temperature) on the electrical, structural, morphological and optical properties of AZO films. The grey-based Taguchi method showed the electrical resistivity of AZO films to be about 9.15 × 10⁻³ Ω cm, and the visible range transmittance to be about 89.31%. Additionally, the films were annealed in a vacuum ambient (5.0 × 10⁻⁶ Torr) at temperatures of 400, 450, 500 and 600 °C, for a period of 30 min. It is apparent that the intensity of the X-ray peaks increases with annealing treatment, leading to improved crystallinity of the films. By applying annealing at 500 °C in a vacuum ambient for 30 min, the AZO films show the lowest electrical resistivity of 2.31 × 10⁻³ Ω cm, with about 90% optical transmittance in the visible region and a surface roughness of Ra = 12.25 nm.     

Study on inverse spinel zinc stannate, Zn2SnO4, as transparent conductive films deposited by rf magnetron sputtering

Inverse spinel zinc stannate (Zn₂SnO₄, ZTO) films were deposited onto fused quartz glass substrates heated at 800 °C by rf magnetron sputtering using a ceramic ZTO target (Zn:Sn = 2:1). H₂ flow ratios [H₂/(Ar + H₂)] were controlled from 0 to 30% during the depositions. ZTO films deposited at 800 °C possessed a polycrystalline inverse spinel structure. The lowest resistivity of 1.1 × 10^− 2 Ω cm was obtained for a ZTO film deposited at 20% H₂ flow ratio. The transmittance of the ZTO film was approximately 80% in the visible region.     

Effects of sputtering pressure and Al buffer layer thickness on properties of AZO films grown by rf magnetron sputtering

Transparent and conductive Al-doped (2 wt.%) zinc oxide (AZO) films were deposited on inexpensive soda-lime glass substrates by using rf magnetron sputtering at room temperature. This study analyzed the effects of argon sputtering pressure, which varied in the range from 0.46 to 2.0 Pa, on the morphological, electrical and optical properties of AZO films. The only (0 0 2) diffraction peak of the film were observed at 2θ～34.45°, exhibiting that the AZO films had hexagonal ZnO wurtzite structure, and a preferred orientation with the c-axis perpendicular to the substrate. By applying a very thin aluminum buffer layer with the thickness of 2 nm, findings show that the electrical resistivity was 9.46 × 10⁻⁴ Ω-cm, and the average optical transmittance in the visible part of the spectra was approximately 81%. Furthermore, as for 10 nm thick buffer layer, the electrical resistivity was lower, but the transmittance was decreased.     

Deterioration and recovery in the resistivity of Al-doped ZnO films prepared by the plasma sputtering

A hot-cathode plasma sputtering technique was used for fabricating the highly transparent and conducting aluminum-doped zinc oxide (AZO) films on glass substrates from a disk-shaped AZO (Al₂O₃: 2 wt.%) target. Under particular conditions where the target voltage was V_T = −200 V and the plasma excitation pressure was P_S = 1.5 × 10⁻³ Torr, the lowest resistivity of 4.2 × 10⁻⁴ Ω cm was obtained at 400 nm, and this was associated with a carrier density of 8.7 × 10²⁰ cm⁻³ and a Hall mobility of 17 cm²/V s. From the annealing experiment of the AZO films in the oxygen and nitrogen gases of the atmospheric pressure it was revealed that both the oxygen vacancies and the grain boundaries in the polycrystalline AZO film played an important role in the electrical properties of the film.     

Effect of Cu layer thickness on the structural, optical and electrical properties of AZO/Cu/AZO tri-layer films

Highly conducting AZO/Cu/AZO tri-layer films were successfully deposited on glass substrates by RF magnetron sputtering of Al-doped ZnO (AZO) and ion-beam sputtering of Cu at room temperature. The microstructures of the AZO/Cu/AZO multilayer films were studied using X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM) and atomic force microscope (AFM). X-Ray diffraction measurements indicate that the AZO layers in the tri-layer films are polycrystalline with the ZnO hexagonal structure and have a preferred orientation with the c-axis perpendicular to the substrates. With the increase of Cu thickness, the crystallinity of AZO and Cu layers is simultaneously improved. When the Cu thickness increases from 3 to 13 nm, the resistivity decreases initially and then varies little, and the average transmittance shows a first increase and then decreases. The maximum figure of merit achieved is 1.94 × 10⁻² Ω⁻¹ for a Cu thickness of 8 nm with a resistivity of 7.92 × 10⁻⁵ Ω cm and an average transmittance of 84%.     

Physical properties of hydrogenated Al-doped ZnO thin layer treated by atmospheric plasma with oxygen gas

Hydrogenated Al-doped ZnO (H:AZO) thin films were deposited on glass substrates at room temperature by radio-frequency magnetron sputtering at various hydrogen flow rates. The addition of hydrogen improved the resistivity of the H:AZO films significantly. A thin insulating layer was produced on H:AZO films by atmospheric pressure plasma with Ar/O₂ reactive gas. The resistivity degenerated and the optical band gap of the oxygen plasma-treated H:AZO films decreased from 3.7 eV to 3.4 eV. This was attributed to a decrease in the hydrogen concentration at the film surface according to elemental depth analysis.     

Room temperature deposition of Al-doped ZnO films on quartz substrates by radio-frequency magnetron sputtering and effects of thermal annealing

High-quality Al-doped zinc oxide (AZO) thin films have been deposited on quartz substrates by radio-frequency magnetron sputtering at room temperature for thin film solar cell applications as transparent conductive oxide (TCO) electrode layers. Effects of post-deposition annealing treatment in pure nitrogen and nitrogen/hydrogen atmosphere have been investigated. Annealing treatments were carried out from 300 °C to 600 °C for compatibility with typical optoelectronic device fabrication processes. A series of characterization techniques, including X-ray diffraction, scanning electron microscopy, Hall, optical transmission, and X-ray photoelectron spectroscopy has been employed to study these AZO materials. It was found that there were significant changes in crystallinity of the films, resistivity increased from 4.60 × 10^− 4 to 4.66 × 10^− 3 Ω cm and carrier concentration decreased from 8.68 × 10²⁰ to 2.77 × 10²⁰ cm^− 3 when annealing in 400 °C pure nitrogen. Whereas there were no significant changes in electrical and optical properties of the AZO films when annealing in 300-500 °C nitrogen/hydrogen atmosphere, the electrical stability of the AZO films during the hydrogen treatment is attributed to both desorption of adsorbed oxygen from the grain boundaries and production of additional oxygen vacancies that act as donor centers in the films by removal of oxygen from the ZnO matrix. These results demonstrated that the AZO films are stably suited for TCO electrodes in display devices and solar cells.     

Electrical mechanism analysis of Al2O3 doped zinc oxide thin films deposited by rotating cylindrical DC magnetron sputtering

Cost efficient and large area deposition of superior quality Al₂O₃ doped zinc oxide (AZO) films is instrumental in many of its applications, including solar cell fabrication due to its numerous advantages over indium tin oxide (ITO) films. In this study, AZO films were prepared by a highly efficient rotating cylindrical direct current (DC) magnetron sputtering system using an AZO target, which has a target material utilization above 80%, on glass substrates in argon (Ar) ambient. A detailed analysis on the electrical, optical, and structural characteristics of AZO thin films was performed for the solar cell, as well as display applications. The properties of films were found to critically depend on deposition parameters, such as sputtering power, substrate temperature, working pressure, and film thickness. A low resistivity of ~ 5.5 × 10^− 4 Ω cm was obtained for films deposited at 2 kW, keeping the pressure, substrate temperature and thickness constant at 3 mTorr, 230 °C and ~ 1000 nm respectively. This was due to an increase in carrier mobility and large grain size. Mobility is found to be controlled by ionized impurity scattering within the grains, since the mean free path of carriers is much smaller than the grain size of the films. The AZO films showed a high transparency of ~ 90% in the long wavelength region. Our results offer a cost-efficient AZO film deposition method that can fabricate films with significant low resistivity and high transmittance that can be applied in thin-film solar cells, as well as thin film transistor (TFT) and non-volatile memory (NVM).     

Characteristics of sputtered Al-doped ZnO films for transparent electrodes of organic thin-film transistor

Aluminum-doped ZnO (AZO) thin-films were deposited with various RF powers at room temperature by radio frequency (RF) magnetron sputtering method. The electrical properties of the AZO film were improved with the increasing RF power. These results can be explained by the improvement of the crystallinity in the AZO film. We fabricated the organic thin-film transistor (OTFT) of the bottom gate structure using pentacene active and poly-4-vinyl phenol gate dielectric layers on the indium tin oxide gate electrode, and estimated the device properties of the OTFTs including drain current-drain voltage (I_D-V_D), drain current-gate voltage (I_D-V_G), threshold voltage (V_T), on/off ratio and field effect mobility. The AZO film that grown at 160 W RF power exhibited low resistivity (1.54 × 10^− 3 Ω·cm), high crystallinity and uniform surface morphology. The pentacene thin-film transistor using the AZO film that's fabricated at 160 W RF power exhibited good device performance such as the mobility of 0.94 cm²/V s and the on/off ratio of ~ 10⁵. Consequently, the performance of the OTFT such as larger field-effect carrier mobility was determined the conductivity of the AZO source/drain (S/D) electrode. AZO films prepared at room temperature by the sputtering method are suitable for the S/D electrodes in the OTFTs.     

Ultrathin Al-doped transparent conducting zinc oxide films fabricated by pulsed laser deposition

Al-doped transparent conducting zinc oxide (AZO) films, approximately 20-110 nm-thick, were deposited on glass substrates at substrate temperatures between 200 and 300 °C by pulsed laser deposition (PLD) using an ArF excimer laser (λ = 193 nm). When fabricated at a substrate temperature of 260 °C, a 40-nm-thick AZO film showed a low resistivity of 2.61 × 10^− 4 Ω·cm, carrier concentration of 8.64 × 10²⁰ cm^− 3, and Hall mobility of 27.7 cm²/V·s. Furthermore, for an ultrathin 20-nm-thick film, a resistivity of 3.91 × 10^− 4 Ω·cm, carrier concentration of 7.14 × 10²⁰ cm^− 3, and Hall mobility of 22.4 cm²/V·s were obtained. X-ray diffraction (XRD) spectra, obtained by the θ-2θ method, of the AZO films grown at a substrate temperature of 260 °C showed that the diffraction peak of the ZnO (0002) plane increased as the film thickness increased from 20 to 110 nm. The full-width-at-half-maximum (FWHM) values were 0.5500°, 0.3845°, and 0.2979° for film thicknesses of 20, 40, and 110 nm, respectively. For these films, the values of the average transmittance in visible light wavelengths (400-700 nm) were 95.1%, 94.2%, and 96.6%, respectively. Field emission scanning electron microscopy (FE-SEM) and atomic force microscopy (AFM) observations showed that even the 20-nm-thick films did not show island structures. In addition, exfoliated areas or vacant and void spaces were not observed for any of the films.     

Rapid thermal-plasma annealing of ZnO:Al films for silicon thin-film solar cells

Rapid thermal annealing of sputter-deposited ZnO and Al-doped ZnO (AZO) films with and without an amorphous silicon (a-Si) capping layer was investigated using a radio-frequency (rf) argon thermal plasma jet at atmospheric pressure. The resistivity of bare ZnO films on glass decreased drastically from 10⁶ to 10³ Ω·cm at maximum surface temperatures T_max above 650 °C, whereas the resistivity increased from 10^− 4 to 10^− 3-10^− 2 Ω·cm for bare AZO films. On the other hand, the resistivity of AZO films with a 30-nm-thick a-Si capping layer remained below 10^− 4 Ω·cm, even after TPJ annealing at a T_max of 825 °C. X-ray diffraction and X-ray photoemission electron studies revealed that the film crystallization of both AZO and a-Si layers was promoted without the formation of an intermixing layer. Additionally, the crystallization of phosphorous- and boron-doped a-Si layers at the sample surface was promoted, compared to that of intrinsic a-Si under identical plasma annealing conditions. The role of the a-Si capping layer on sputter-deposited AZO and ZnO films during TPJ annealing is demonstrated. The effects of the mixing of phosphorous and boron impurities in a-Si:H during TPJ annealing of flat and textured AZOs are also discussed.     

Electrical and optical properties of Al-doped ZnO films deposited by hollow cathode gas flow sputtering

Al-doped ZnO (AZO) films were deposited on glass by hollow cathode gas flow sputtering using Zn-Al alloy targets. Sputtering power for all the depositions was fixed at 1500 W. Resistivities of 0.81-1.1 × 10^− 3 Ω cm were obtained for AZO films deposited at room temperature with an O₂ flow from 38 to 50 standard cubic centimetre/minute (SCCM), while static deposition rates were almost constant at 270-300 nm/min. On the other hand, lower resistivities of 5.2-6.4 × 10^− 4 Ω cm were obtained for AZO films deposited at 200 °C with an O₂ flow from 25 to 50 SCCM, while the static deposition rates were almost constant at 200-220 nm/min. Average transmittances in the visible light region were above 80% for both sets of films.     

Fabrication of TiO2-based transparent conducting oxide on glass and polyimide substrates

We report on preparation and properties of anatase Nb-doped TiO₂ transparent conducting oxide films on glass and polyimide substrates. Amorphous Ti_0.96Nb_0.04O₂ films were deposited at room temperature by using sputtering, and were then crystallized through annealing under reducing atmosphere. Use of a seed layer substantially improved the crystallinity and resistivity (ρ) of the films. We attained ρ = 9.2 × 10^− 4 Ω cm and transmittance of ~ 70% in the visible region on glass by annealing at 300 °C in vacuum. The minimum ρ of 7.0 × 10^− 4 Ω cm was obtained by 400 °C annealing in pure H₂.     

Structural, electrical and optical properties of ITO films with a thin TiO2 seed layer prepared by RF magnetron sputtering

Tin-doped indium oxide (ITO) films were deposited by RF magnetron sputtering on TiO₂-coated glass substrates (the TiO₂ layer is usually called seed layer). The properties of ITO films prepared at a substrate temperature of 300 °C on bare and TiO₂-coated glass substrates have been analyzed by using X-ray diffraction, atomic force microscope, optical and electrical measurements. Comparing with single layer ITO film, the ITO film with a TiO₂ seed layer of 2 nm has a remarkable 41.2% decrease in resistivity and similar optical transmittance. The glass/TiO₂ (2 nm)/ITO film achieved shows a resistivity of 3.37 × 10⁻⁴ Ω cm and an average transmittance of 93.1% in the visible range. The glass/TiO₂ may be a better substrate compared with bare glass for depositing high quality ITO films.     

Highly conductive alumina-added ZnO ceramic target prepared by reduction sintering and its effects on the properties of deposited thin films by direct current magnetron sputtering

To obtain a suitable sputtering target for depositing transparent conducting Al-doped ZnO (AZO) films by using direct current (DC) magnetron sputtering, this study investigates the possibility of using atmosphere controlled sintering of Al₂O₃ mixed ZnO powders to prepare highly conductive ceramic AZO targets. Experimental results show that a gas mixture of Ar and CO could produce a sintered target with resistivity in the range of 2.23 × 10^− 4 Ω cm. The fairly low resistivity was mainly achieved by the formation of both aluminum substitution (Al_Zn) and oxygen vacancy (V_O), thus greatly increasing the carrier concentration. Compared to usual air sintered target, the thin film deposited by the Ar + CO sintered target exhibited lower film resistivity and more uniform spatial distribution of resistivity. A film resistivity as low as 6.8 × 10^− 4 Ω cm was obtained under the sputtering conditions of this study.     

Structural, optical and electrical properties of AZO/Cu/AZO tri-layer films prepared by radio frequency magnetron sputtering and ion-beam sputtering

Highly conducting tri-layer films consisting of a Cu layer sandwiched between Al-doped ZnO (AZO) layers (AZO/Cu/AZO) were prepared on glass substrates at room temperature by radio frequency (RF) magnetron sputtering of AZO and ion-beam sputtering of Cu. The tri-layer films have superior photoelectric properties compared with the bi-layer films (Cu/AZO, AZO/Cu) and single AZO films. The effect of AZO thickness on the properties of the tri-layer films was discussed. The X-ray diffraction spectra show that all films are polycrystalline consisting of a Cu layer with the cubic structure and two AZO layers with the ZnO hexagonal structure having a preferred orientation of (0 0 2) along the c-axis, and the crystallite size and the surface roughness increase simultaneously with the increase of AZO thickness. When the AZO thickness increases from 20 to 100 nm, the average transmittance increases initially and then decreases. When the fixed Cu thickness is 8 nm and the optimum AZO thickness of 40 nm was found, a resistivity of 7.92 × 10⁻⁵ Ω cm and an average transmittance of 84% in the wavelength range of visible spectrum of tri-layer films have been obtained. The merit figure (F_TC) for revaluing transparent electrodes can reach to 1.94 × 10⁻² Ω⁻¹.     

Synthesis of c-axis preferred orientation ZnO:Al transparent conductive thin films using a novel solvent method

Transparent aluminum doped zinc oxide (ZnO:Al, AZO) conducting thin films with a high-preferential c-axis orientation were synthesized using a new sol-gel formula. The films were deposited using a spin-coating route onto borosilicate glass substrates. We used propylene glycol methyl ether (PGME) as the solvent in place of ethylene glycol monomethyl ether (EGME), which is commonly used because it is easier to deposit onto the substrates. PGME is also superior in terms of health and safety. PGME solvent does not need to settle for several days before use and can be spin-coated as soon as the raw material and solvent are mixed. The effects of this novel solvent on the structural, morphological, electrical and optical properties are discussed using XRD, SEM, a four-point probe and UV-VIS spectrophotometry. It was found that the films produced with PGME showed a high-preferential c-axis orientation and compact microstructure in comparison films produced using EGME. The electrical resistivity of AZO thin films produced with PGME solvent was lowered to 3.474 × 10^− 3Ω cm after annealing in 95 N₂/5H₂ atmosphere. In addition, the optical transmittances of AZO thin films on glass plates were higher than 90% in the visible wavelength region.