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A Study on Solution-Processed Y2O3 Films Modified by Atomic Layer coatings Article A Study on Solution-Processed Y2O3 Films Modified by Atomic Layer Deposition Al2O3 as Dielectrics in ZnO Thin Film Transistor Haiyang Xu 1, Xingwei Ding 1,2,*, Jie Qi 3, Xuyong Yang 1,2 and Jianhua Zhang 1,2 1 Key Laboratory of Advanced Display and System Application, Ministry of Education, Shanghai University, Shanghai 200072, China; [email protected] (H.X.); [email protected] (X.Y.); [email protected] (J.Z.) 2 School of Mechatronics and Automation, Shanghai University, Shanghai 200072, China 3 Research and Development Department, Air Liquide Innovation Campus Shanghai, Shanghai 201108, China; [email protected] * Correspondence: [email protected]; Tel.: +86-21-5633-1976; Fax: +86-21-3998-8216 Abstract: In this work, Y2O3–Al2O3 dielectrics were prepared and used in ZnO thin film transistor as gate insulators. The Y2O3 film prepared by the sol–gel method has many surface defects, resulting in a high density of interface states with the active layer in TFT, which then leads to poor stability of the devices. We modified it by atomic layer deposition (ALD) technology that deposited a thin Al2O3 film on the surface of a Y2O3 dielectric layer, and finally fabricated a TFT device with ZnO as the active layer by ALD. The electrical performance and bias stability of the ZnO TFT with a Y2O3–Al2O3 laminated dielectric layer were greatly improved, the subthreshold swing was reduced from 147 to 6 8 88 mV/decade, the on/off-state current ratio was increased from 4.24 × 10 to 4.16 × 10 , and the threshold voltage shift was reduced from 1.4 to 0.7 V after a 5-V gate was is applied for 800 s. Citation: Xu, H.; Ding, X.; Qi, J.; Yang, X.; Zhang, J. A Study on Keywords: Y2O3 films; Y2O3–Al2O3 laminated dielectric; atomic layer deposition; thin film transistors Solution-Processed Y2O3 Films Modified by Atomic Layer Deposition Al2O3 as Dielectrics in ZnO Thin Film Transistor. Coatings 2021, 11, 969. 1. Introduction https://doi.org/10.3390/ In recent years, metal oxide thin film transistors (TFT) have attracted a lot of attention coatings11080969 due to their high transmittance, high current switching ratio, insensitivity to visible light, and technical advantages, such as solution processing and low temperature deposition. Academic Editor: Angela De Bonis They are widely used in flat panel displays and large-scale integrated circuits and, thus, show a huge application value [1,2]. Among the various metal oxide TFTs, transparent Received: 26 July 2021 ZnO-based TFTs have been extensively studied as a replacement for silicon-based TFTs in Accepted: 13 August 2021 Published: 15 August 2021 large area electronic displays [3–5]. In this regard, ZnO-based TFTs exhibit good electrical and optical properties such as high electron mobility, good uniformity, and excellent Publisher’s Note: MDPI stays neutral transparency to visible light, making them a promising candidate for practical application with regard to jurisdictional claims in in next generation flat panel displays [6,7]. In this work, ZnO thin films in TFT were published maps and institutional affil- deposited by ALD technology. iations. As an important part of TFT, the gate dielectric layer plays an important role in the performance of TFT. With the reduction in the critical size of semiconductor devices, a traditional SiO2 dielectric layer, which has a low dielectric constant, can no longer meet the requirements of device preparation due to the secondary effect becoming prominent [8]. Therefore, a new high-performance dielectric layer is developed to replace it. Therefore, Copyright: © 2021 by the authors. Licensee MDPI, Basel, Switzerland. high-k materials, such as ZrO2 [9,10], HfO2 [11], and TiO2 [12], have received extensive This article is an open access article attention from researchers. However, high-k materials are difficult to apply on a large distributed under the terms and scale due to their high cost, easy crystallization, large leakage current, and high surface conditions of the Creative Commons roughness [13]. The interface modification method, i.e., the emergence of laminated Attribution (CC BY) license (https:// dielectric layers, has better solved the problems faced by high-k materials, and further creativecommons.org/licenses/by/ promoted the large-scale application of high-k dielectric layers. Waggoner et al. successfully 4.0/). prepared the ZrO2–Al2O3 laminated dielectric layer and realized the regulation of its Coatings 2021, 11, 969. https://doi.org/10.3390/coatings11080969 https://www.mdpi.com/journal/coatings Coatings 2021, 11, 969 2 of 7 dielectric properties [14]. Chang et al. successfully applied the gate dielectric layer of the Al2O3/HfO2/Al2O3 structure to the ZnO TFT. Compared with a single HfO2 dielectric layer, its hysteresis has been significantly improved, and it has higher electrical stability [15]. Ding et al. reported that, by inserting Al2O3 as a modified layer into the IGZO TFT with ZrO2 as the dielectric layer, the gate leakage current was obviously reduced and better transfer and output characteristics were obtained [12]. Y2O3 is a promising candidate for use as a gate insulator since it could present low leakage current, high breakdown voltage, and good high-temperature reliability due to both wide band gap (5–6 eV) and excellent thermal stability. Many research groups have studied IGZO transistors employing Y2O3 as gate insulator [16–18]. We prepared a Y2O3 dielectric layer by the sol–gel method and modified it by ALD Al2O3. The Y2O3 film prepared by the sol–gel method has many surface defects, resulting in a high density of interface states with the active layer in TFT, leading to poor stability of the devices. We modified it by atomic layer deposition (ALD) technology that deposited a thin Al2O3 film on the surface of the Y2O3 dielectric layer. This ALD technology has many advantages. For example, the prepared film has a uniform surface, high thickness controllability, excellent repeatability, and low deposition temperature [19]. At the meanwhile, an Al2O3 film is prepared by a direct spin-coating process to modify the Y2O3. This would make it clear that there is a distinct advantage of using an additional ALD layer rather than a direct spin- coating process. The performance of ZnO–Y2O3 (named ‘device A’) and ZnO–Y2O3–ALD and Al2O3 (named ‘device B’) TFT were examined to confirm the expected performance of Y2O3 and the effect of ALD Al2O3. 2. Experiments A 0.2-M Y2O3 and 0.4-M Al2O3 precursor solution were synthesized by dissolving a certain amount of Y(CH3COO)3·xH2O and Al(NO3)3·9H2O in ethylene glycol methyl ether. After the precursor solution was placed in a magnetic stirrer and stirred for 10 min to completely dissolve the solute, ethanolamine was added as a stabilizer to avoid turbidity and precipitation of the precursor solution. The preparation process of precursor solution was carried out in a glove box filled with nitrogen to isolate water and oxygen in the air. The prepared precursor solution was stirred in a water bath heating pot with a magnetic stirrer at 60 ◦C for 2 h, and then aged at room temperature for 12 h to obtain homogeneous hydrolysis and the best viscosity. Before depositing the film, the p-type Si substrate was ultrasonically cleaned in acetone, alcohol, and deionized water for 10 min to remove stains and grease. Then, the Si substrate was treated in an ozone and ultraviolet environment for 10 min to improve the hydrophobicity of the substrate surface and enhance the uniformity of film growth. Next, the Y2O3 precursor solution was dropped onto the Si substrate through a syringe, first spin-coated at a speed of 500 r/min for 5 s, and then at a speed of 3000 r/min for 30 s. This process was repeated three times to obtain a 60-nm-thick films. The Al2O3 precursor solution was spin-coated on it at a speed of 2000 r/min for 20 s to obtain a 10-nm-thick film. Then, the film was placed on a hot plate at 120 ◦C to cure for 10 min. The film was ◦ then placed in a muffle furnace and annealed at 400 C for 2 h. Subsequently, an Al2O3 film of approximately 10 nm was deposited on another solution-processed 60-nm-thick ◦ Y2O3 film by ALD (TFS-200, Beneq) at 200 C using trimethylaluminum and deionized water. Then, high-purity diethyl zinc (DEZ) and deionized water were used to deposit a 20-nm ZnO active layer at 150 ◦C on the dielectric layer, with a purge time of 5 s. Finally, Al films deposited by thermal evaporation were used as source/drain electrode of TFTs with channel width (W) = 1000 µm and channel length (L) = 200 µm, respectively. The schematic structure of the ZnO TFT with Y2O3–Al2O3 (ALD) as gate insulator are shown in Figure1a. The surface morphology of the films was characterized by atomic force microscope (AFM, nanonaviSPA-400 SPM, SII Nano Technology Inc. Chiba City, Japan). The AFM measurement mode used was a tapping mode. The parameters of the AFM tip (Tap150AL- G) were of a resonant freq. of 150 KHz and a force constant of 5 N/m. The measurement Coatings 2021, 11, x FOR PEER REVIEW 3 of 8 The surface morphology of the films was characterized by atomic force microscope (AFM, nanonaviSPA-400 SPM, SII Nano Technology Inc. Chiba City, Japan). The AFM measurement mode used was a tapping mode. The parameters of the AFM tip (Tap150AL-G) were of a resonant freq. of 150 KHz and a force constant of 5N/m. The measurement geometry was rectangle and the acquisition time was 4 min.
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