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A green and low-cost method to prepare high-quality GaN (gallium nitride) nanowires is important for the applications of GaN-based devices on a large scale. In this work, high-quality GaN nanowires are successfully prepared by a green plasma enhanced chemical vapor deposition method without catalyst, with Al2O3 used as a substrate, metal Ga as a gallium source and N2 as a nitrogen source. The obtained GaN nanomaterials are investigated by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectroscopy, and photoluminescence (PL) spectroscopy. The XRD results demonstrate that hexagonal-wurtzite GaN is obtained and no other phases exist. The SEM results show that GaN nanowires and hexagonal GaN microsheets are obtained at different temperatures. When the growth temperature is at 950 ℃ (reaction time for 2 h), the hexagonal GaN microsheets each with a size of 15 μm are obtained. When the growth temperature is at 1000 ℃(reaction time for 2 h), the GaN nanowires with the lengths in a range of 10–20 μm are obtained. With the reaction temperature increasing from 0.5 h to 2 h, the lengths of GaN nanowires increase. The TEM results suggest that the GaN nanowires are of high crystallinity and the growth direction of GaN nanowires is in the [0001] direction. The Raman results indicate that there exists a compressive stress in the GaN nanowires and its value is 0.84 GPa. Meanwhile, the growth mechanism of GaN nanowires is also proposed. The morphologies of GaN nanomaterials are tailed by the growth temperature, which may be caused by Ga atomic surface diffusion. Ga atoms have low diffusion energy and small diffusion length at 950 ℃. They gather in the non-polar m-plane. The (0001) plane with the lowest energy begins to grow. Then, hexagonal GaN microsheets are obtained. When reaction temperature is at 1000 ℃, the diffusion length of Ga atoms increases. Ga atoms can diffuse into (0001) plane. In order to maintain the lowest surface energy, the GaN nanowires grow along the [0001] direction. The PL results indicate that the obtained GaN nanowires have just an intrinsic and sharp luminescence peak at 360 nm, which possesses promising applications in photoelectric devices such as ultraviolet laser emitter. Our research will also provide a low-cost and green technical method of fabricating the new photoelectric devices.
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Keywords:
- GaN nanowires /
- plasma enhanced chemical vapor deposition /
- no catalyst /
- growth mechanism
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图 1 950 ℃和1000 ℃下获得样品的XRD图(反应时间为2 h)
Figure 1. X-ray diffraction patterns of the samples fabricated at 950 ℃ and 1000 ℃ (Reaction time is 2 h)
图 2 反应温度为1000 ℃时, 不同反应时间获得GaN样品的SEM图 (a) 0.5 h, (b) 1 h, (c) 2 h; (d) 950 ℃下获得GaN样品的SEM图
Figure 2. SEM images of GaN samples fabricated at different reaction time (Reaction temperature is 1000 ℃): (a) 0.5 h, (b) 1 h, (c) 2 h; (d) SEM image of GaN sample fabricated at 950 ℃.
图 3 1000 ℃反应2 h获得GaN纳米线的TEM图 (a) 单根GaN纳米线的TEM照片; (b) 图(a)中的GaN纳米线的高倍TEM照片; (c) 另一根GaN纳米线的TEM照片; (d) 图(c)中的GaN纳米线的高倍TEM照片
Figure 3. TEM images of GaN nanowires fabricated at 1000 ℃ (Reaction time is 2 h): (a) TEM image of single GaN nanowire; (b) HR-TEM image of GaN nanowire in (a); (c) TEM image of another GaN nanowire; (d) HR-TEM image of GaN nanowire in (c).
图 4 1000 ℃反应2 h获得GaN纳米线的Raman谱图
Figure 4. Raman spectra of GaN nanowires fabricated at 1000 ℃ (Reaction time is 2 h).
图 5 GaN纳米材料的生长机理示意图
Figure 5. Growth mechanism diagram of GaN nanomaterials.
图 6 1000 ℃反应2 h获得GaN纳米线的PL谱图
Figure 6. PL spectrum of GaN nanowires fabricated at 1000 ℃ (Reaction time is 2 h).
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[1] Lin Y, Yang M, Wang W, Lin Z, Li G 2016 Cryst. Eng. Comm. 18 8926
Google Scholar
[2] Takekawa N, Hayashida N, Ohzeki D, Yamaguchi A, Murakami H, Kumagai Y, Matsumoto K, Koukitu A 2018 J. Cryst. Growth 502 7
Google Scholar
[3] Wang X F, Zhang Y, Chen X M, He M, Liu C, Yin Y A, Zou X S, Li S T 2014 Nanoscale 6 12009
Google Scholar
[4] Patsha A, Amirthapandian S, Pandian R, Dhara S 2013 J. Mater. Chem. C 1 8086
Google Scholar
[5] 陈程程, 刘立英, 王如志, 宋雪梅, 王波, 严辉 2013 62 177701
Google Scholar
Chen C C, Liu L Y, Wang R Z, Song X M, Wang B, Yan H 2013 Acta Phys. Sin. 62 177701
Google Scholar
[6] Calarco R, Meijers R J, Debnath K R, Stoica T, Sutter E, Luth H 2007 Nano Lett. 7 2248
Google Scholar
[7] Kumaresan V, Largeau L, Madouri A, Glas F, Zhang H Z, Oehler F, Cavanna A, Babichev A, Travers L, Gogneau N, Tchernycheva M, Harmand C J 2016 Nano Lett. 16 4895
Google Scholar
[8] Kesaria M, Shetty S, Shivaprasad M S 2011 Cryst. Growth Des. 11 4900
Google Scholar
[9] Kuykendall T, Pauzauskie P, Lee S K, Zhang Y F, Goldberger J, Yang P D 2003 Nano Lett. 3 1063
Google Scholar
[10] Ji Y H, Wang R Z, Feng X Y, Zhang Y F, Yan H 2017 J. Phys. Chem. C 121 24804
Google Scholar
[11] Wang Y Q, Wang R Z, Li Y J, Zhang Y F, Zhu M K., Wang B B, Yan H 2013 Cryst. Eng. Comm 15 1626
Google Scholar
[12] Zhao J W, Zhang Y F, Li Y H, Su C H, Song X M, Yan H, Wang R Z 2015 Sci. Rep. 5 17692
Google Scholar
[13] Jacobs B W, Crimp M A, McElroy K, Ayres V M 2008 Nano Lett. 8 4353
Google Scholar
[14] Chang K W, Wu J J 2002 J. Phys. Chem. B 106 7796
Google Scholar
[15] Stamplecoskie K G, Ju L, Farvid S S, Radovanovic P V 2008 Nano Lett. 8 2674
Google Scholar
[16] Li C, Bando Y, Golberg D 2010 ACS Nano 4 2422
Google Scholar
[17] 赵军伟, 张跃飞, 宋雪梅, 严辉, 王如志 2014 63 117702
Google Scholar
Zhao J W, Zhang Y F, Song X M, Yan H, Wang R Z 2014 Acta Phys. Sin. 63 117702
Google Scholar
[18] Schiaber Z D, Calabrese G, Kong X, Trampert A, Jenichen B, de Silva J HD, Geelhaar L, Brandt O, Fermandez-Garrido S 2017 Nano Lett. 17 63
Google Scholar
[19] Choi S, Song H G, Yoo Y S, Lee C, Woo K Y, Lee E, Roh S D, Cho Y H 2018 ACS Photonics 5 2825
Google Scholar
[20] Feng X Y, Wang R Z, Liang Q, Ji Y H, Yang M Q 2019 Cryst. Growth Des. 19 2687
Google Scholar
[21] Wei X F, Shi F 2011 Appl. Surf. Sci. 257 9931
Google Scholar
[22] Shen L H, Cheng T M, Wu L J, Li X G, Cui Q L 2008 J. Alloys Compd. 465 562
Google Scholar
[23] Ramesh C, Tyagi P, Bhattacharyya B, Husale S, Maurya K K, Kumar M S, Kushvaha S S 2019 J. Alloys Compd. 770 572
Google Scholar
[24] Purushothaman V, Ramakrishnan V, Jeganathan K 2012 Cryst. Eng. Comm. 14 8390
Google Scholar
[25] Purushothaman V, Ramakrishnan V, Jeganathan K 2012 RSC Adv. 2 4802
Google Scholar
[26] Li Y, Wang W L, Li X C, Huang L G, Lin Z T, Zheng Y L, Chen X F, Li G Q 2019 J. Alloys Compd. 771 1000
Google Scholar
[27] Wei P C, Chen L C, Chen K H 2014 J. Appl. Phys. 116 124301
Google Scholar
[28] Wu C, Yu J D, E Y X, Luo Y, Hao Z B, Wang J, Wang L, Sun C Z, Xiong B, Han Y J, Li H T 2016 Cryst. Growth Des. 16 5023
Google Scholar
[29] Xian Y L, Huang S J, Zheng Z Y, Fan B F, Wu Z S, Jiang H, Wang G 2011 J. Cryst. Growth 325 32
Google Scholar
[30] Matoussi A, Nasr F B, Boufaden T, Salh R, Fakhfakh Z, Guermazi S, ElJani B, Fitting H J 2010 J. Lumin. 130 399
Google Scholar
[31] Sun R, Wang G G, Peng Z C 2018 Mater. Lett. 217 288
Google Scholar
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