Effects of annealing temperature on  properties of gallium oxide thin films and ultraviolet detectors

Luo Ju-Xin; Gao Hong-Li; Deng Jin-Xiang; Ren Jia-Hui; Zhang Qing; Li Rui-Dong; Meng Xue

doi:10.7498/aps.72.20221716

Abstract

In this work, gallium oxide (Ga₂O₃) thin films are deposited on quartz substrates by radio frequency magnetron sputtering at room temperature and annealed in argon atmosphere at different temperatures. The influences of annealing temperatures in the argon atmosphere on crystal structure, transmittance, surface morphology, and optical band gap of the samples are investigated in detail. It is found that the annealing process can improve the crystalline quality of the film, but high-temperature annealing can also easily cause oxygen elements in the film to escape from the film to form oxygen vacancies, which is evidenced by XPS test results. To obtain the effect of the annealing process on the performance of gallium oxide thin film detector, the metal-semiconductor-metal (MSM) photodetector based on the sample annealed at 800 °C, which is compared with untreated sample operated at a reverse bias voltage of 1.1 V, can achieve excellent comprehensive photo-detection properties for 254 nm ultraviolet light: the light-dark current ratio (I₂₅₄/I_dark), responsivity and specific detectivity are as high as 1021.3, 0.106 A/W and 1.61 × 10¹² Jones, respectively, which are 7.5, 195 and 38.3 times those of the unannealed sample device. And the external quantum efficiency is improved by 51.6%. The rise time of sample detector (0.19/0.48 s) annealed at 800 ℃ decreases compared with that of the unannealed sample (0.93/0.93 s), and the descent time of 800 ℃ detector (0.64/0.72 s)increases compared with that of the unannealed sample (0.45/0.49 s), respectively. By comparing the parameters with those of other current gallium oxide-based MSM photodetectors, it is found that the detector parameters of this work have some gaps compared with the current optimal parameters, which is attributed to the fact that the quartz substrate is selected for this work and not the sapphire substrate that is better matching with gallium oxide, resulting in the poor quality of the film compared with that of the sample on the sapphire substrate, and in this work, the photodetector has the high light-dark current ratio (PDCR) and detection rate (D^*). In the end, the mechanism of increasing oxygen vacancies after being annealed, which leads to the improvement of detector performance parameters, is analyzed in detail.

Keywords:

Authors and contacts

Department of Physics, Beijing University of Technology, Beijing 100124, China

Corresponding author: Deng Jin-Xiang, jdeng@bjut.edu.cn

Funds: Project supported by the Beijing New-star Plan of Science and Technology, China (Grant No. Z211100002121079) and the Natural Science Foundation of Beijing City, China (Grant Nos. 4192016, 4102014).

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References

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图 1 氧化镓MSM探测器器件结构图

Figure 1. The device structure of the gallium oxide MSM detector.

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图 2 不同退火温度的XRD图谱

Figure 2. XRD patterns at different annealing temperatures.

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图 3 (a) 不同退火温度下的半峰宽和峰强度图像; (b)不同退火温度的平均晶粒尺寸图像

Figure 3. (a) Images of the half-peak width and peak intensity at different annealing temperatures; (b) images of average grain size at different annealing temperatures.

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图 4 退火温度分别为600 ℃ (a), 700 ℃ (b), 800 ℃ (c)和900 ℃ (d)的AFM图像, 以及4个样品的均方根粗糙度图像(e)

Figure 4. AFM images of annealing temperatures of 600 ℃ (a), 700 ℃ (b), 800 ℃ (c) and 900 ℃ (d), and RMS roughness images (e) of the four samples.

DownLoad: Full-Size Img PowerPoint

图 5 (a) 不同退火温度下的氧化镓薄膜透射光谱; (b) 不同退火温度薄膜样品光学带隙图像

Figure 5. (a) Transmission spectra of Ga₂O₃ thin films at different annealing temperatures; (b) optical band gap images of thin films at different annealing temperatures.

DownLoad: Full-Size Img PowerPoint

图 6 不同退火温度下薄膜样品的XPS测量全谱 (a) 以及沉积态 (b) 和退火样品 (c) 的O1s精细谱

Figure 6. XPS survey spectra (a) and high-resolution O_1s spectra for the as-grown (b), in different annealing temperatures (c) of Ga₂O₃ film.

DownLoad: Full-Size Img PowerPoint

图 7 室温下生长样品 (a) 和800 ℃ 退火样品 (b) 在黑暗环境下及254 nm 紫外光源照射下的I-V图像和半对数图像以及在5 V偏压下, 25 ℃ (c), 800 ℃ (d)的I-T图像及其双指数拟合I-T图像 (e) 和 (f)

Figure 7. I-V images and semi-logarithmic images of samples grown at room temperature (a) and annealed at 800 ℃ (b) in the dark under 254 nm UV light source and under 5 V bias, the I-T image of 25 ℃ (c), 800 ℃ (d) and its bi-exponential fitting I-T images (e), (f).

DownLoad: Full-Size Img PowerPoint

图 8 光开启时 (a) 和光关闭后 (b) 氧化镓MSM器件能带示意图, 途径1表示光生载流子的产生 (a) 与复合 (b), 途径2表示氧空位缺陷捕获 (a) 和释放 (b) 光生电子

Figure 8. Schematic diagram of the energy band of the gallium oxide MSM device when the light is turned on (a) and after the light is turned off (b). Pathway 1 represents the generation (a) and recombination (b) of photogenerated carriers, and pathway 2 represents oxygen vacancy defect trapping (a) and release (b) photogenerated electrons.

DownLoad: Full-Size Img PowerPoint

表 1 在5 V偏压下I-T双指数拟合图像响应时间参数表

Table 1. I-T Bi-exponential fitted image response time parameters at 5 V bias.

Photodetector	τ_r1/s	τ_r2/s	τ_d1/s	τ_d2/s
25 ℃	0.93	0.93	0.45	0.49
800 ℃	0.19	0.48	0.64	0.72

DownLoad: CSV

表 2 在–1.1 V偏压下的探测器参数汇总表

Table 2. Summary table of detector parameters at –1.1 V bias.

Photodetector	I_dark/nA	PDCR(I₂₅₄/I_dark)	R_λ/(A·W^–1)	EQE/%	D*/Jones
25 ℃	0.0262	136	5.54 × 10^–4	0.2	4.21 × 10¹⁰
800 ℃	0.677	1021.3	0.106	51.8	1.61 × 10¹²

DownLoad: CSV

表 3 当前氧化镓基MSM结构光电探测器主要性能参数汇总表

Table 3. Comparison of main performance parameters of current gallium oxide-based MSM photodetectors

Photodetector	Method	I_d/nA	PDCR	R₂₅₄/ (A·W^–1)	D*/Jones	Ref.
Ga₂O₃/Al₂O₃	Sol-gel	0.125@15 V	673	0.04	4.6 × 10¹¹	[14]
Ga₂O₃/SiC	Sputtering	7.6@10 V	383	2.6	1.6 × 10¹²	[17]
Ga₂O₃/Al₂O₃	PLD	0.1@20 V	520	60	—	[27]
N:Ga₂O₃/Al₂O₃	Sputtering	0.01@10 V	—	0.013	6.1 × 10¹⁰	[30]
Ga₂O₃/Al₂O₃	MOCVD	0.17@10 V	4.53	9.4	0.17 × 10¹²	[31]
Ga₂O₃/Al₂O₃	Sputtering	8.2 × 10^–5@10 V	3.58 × 10⁵	1.93	6.53 × 10¹³	[32]
Ga₂O₃/Quartz	Sputtering	0.677@1.1 V	1021.3	0.106	1.61 × 10¹²	This work

DownLoad: CSV

[1]	Liu X Z, Guo P, Sheng T, Qian L X, Zhang W L, Li Y R 2016 Opt. Mater. 51 203 Google Scholar
[2]	Xu J J, Zheng W, Huang F 2019 J. Mater. Chem. C 7 8753 Google Scholar
[3]	Wang H, Ma J, Cong L, Zhou H, Li P, Fei L, Li B, Xu H, Liu Y 2021 Mater. Today Phys. 20 100464 Google Scholar
[4]	Xie C, Lu X T, Liang Y, Chen H H, Wang L, Wu C Y, Wu D, Yang W H, Luo L B 2021 J. Mater. Sci. Technol. 72 189 Google Scholar
[5]	Guo X C, Hao N H, Guo D Y, Wu Z P, An Y H, Chu X L, Li L H, Li P G, Lei M, Tang W H 2016 J. Alloys Compd. 660 136 Google Scholar
[6]	Lu N Y, Gu Y, Weng Y Y, Da Z C, Ding Y 2019 Mater. Res. Express 6 095033 Google Scholar
[7]	Wang L, Gu D W, Shen L J 2017 Solid State Sci. 72 10 Google Scholar
[8]	Yu M, Wang H Q, Wei W, Peng B, Yuan L, Hu J C, Zhang Y M, Jia R X 2021 Appl. Surf. Sci. 568 150826 Google Scholar
[9]	Ghosh S, Baral M, Kamparath R, Singh S D, Gangul T 2019 Appl. Phys. Lett. 115 251603 Google Scholar
[10]	Kaur D, Kumar M 2021 Adv. Opt. Mater. 3 2002160 Google Scholar
[11]	Wang D, Ma X C, Xiao H D, Chen R R, Le Yong, Luan C N, Zhang B, Ma J 2022 Mater. Res. Bull. 149 111718 Google Scholar
[12]	Mukhopadhyay P, Hatipoglu I, Sakthivel T S, Hunter D A, Edwards P R, Martin R W, Naresh-Kumar G, Seal S, Schoenfeld W V 2021 Adv. Photonics Res. 2 2000067 Google Scholar
[13]	Jeong S H, Vu Ti K O, Kim E K 2021 J. Alloys Compd. 877 160291 Google Scholar
[14]	Yu M, Lv C D, Yu J G, Shen Y M, Yuan L, Hu J C, Zhang S N, Cheng H J, Zhang Y M, Jia R X 2020 Mater. Today Commun. 25 101532 Google Scholar
[15]	Shen H, Yin Y N, Tian K, Baskaran K, Duan L B, Zhao X R, Tiwari A 2018 J. Alloys Compd. 766 601 Google Scholar
[16]	Patila V, Lee B T, Jeong S H 2022 J. Alloys Compd. 894 162551 Google Scholar
[17]	Li M Q, Yang N, Wang G G, Zhang H Y, Han J C 2019 Appl. Surf. Sci. 471 694 Google Scholar
[18]	Zhang Y J, Yan J L, Li Q S, Qu C, Zhang L Y, Li T 2011 Physica B 406 3079 Google Scholar
[19]	Goyal A, Yadav B S, Thakur O P, Kapoor A K, Muralidharan R 2014 J. Alloys Compd. 583 214 Google Scholar
[20]	Feng Z Q, Huang L, Feng Q, Li X, Zhang H, Tang W h, Zhang J C, Hao Y 2018 Opt. Mater. Express 8 2229 Google Scholar
[21]	Tien C H, Hsiao B W, Chen C M, Chen M I, Chiang J L, Wuu D S 2020 Ceram. Int. 46 24147 Google Scholar
[22]	Singh A K, Gupta M, Sathe V, Katharria Y S 2021 Superlattice Microst. 156 106976 Google Scholar
[23]	Yu J G, Nie Z Z, Dong L P, Yuan L, Li D J, Huang Y, Zhang L C, Zhang Y M, Jia R X 2019 J. Alloys Compd. 798 458 Google Scholar
[24]	Wang H Y, Tang C M, Yang W J, Zhao J J, Liu L H, Mu J X, Zhang Y P, Zeng C Y 2022 Ceram. Int. 48 3481 Google Scholar
[25]	Cui R R, Zhang J, Luo Z J, Guo X, Ding Z, Deng C Y 2021 Chinese Phys. B 2 028505 Google Scholar
[26]	Wei P, Zhu D M, Huang S S, Zhou W C, Luo F 2013 Appl. Surf. Sci. 285P 577
[27]	Zhou H T, Cong L J, Ma J G, Chen M Z, Song D Y, Wang H B, Li P, Li B S, Xu H Y, Liu Y C 2020 J. Alloys Compd. 847 156536 Google Scholar
[28]	Han J F, Yang D Z, Ma D G, Qiao W Q, Wang Z Y 2019 Org. Electron. 68 242 Google Scholar
[29]	Gong. X, Tong M, Xia Y J, Cai W Z, Moon J S, Cao Y, Yu G, Shieh C L, Nilsson B, Heeger A J 2009 Science 325 1665 Google Scholar
[30]	周树仁, 张红, 莫慧兰, 刘浩文, 熊元强, 李泓霖, 孔春阳, 叶利娟, 李万俊 2021 物理学报 70 178503 Google Scholar Zhou S R, Zhang H, Mo H L, Liu H W, Xiong Y Q, Li H L, Kong C Y, Ye L J, Li W J 2021 Acta Phys. Sin. 70 178503 Google Scholar
[31]	Xu R, Ma X C, Chen Y H, Mei Y, Ying L Y, Zhang B P, Long H 2022 Mat. Sci. Semicon. Proc. 144 106621 Google Scholar
[32]	Zhou S, Peng X, Liu H W, Zhang Z F, Ye L J, Li H L, Xiong Y Q, Niu L B, Chen F L, Fang L, Kong C Y, Li W J, Yang X, Zhang A H 2022 Opt. Mater. Express 12 327
[33]	Wang Q L, Huang P, Liu Q, Li Y X, Qu Q L, Li M K, Homewood K P, Lu Y M, He Y B 2020 J. Alloys Compd. 834 155036 Google Scholar

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