Abstract
Al buffer layers with Al droplets-distributed surface have been employed to grow high-quality and stress-free GaN epitaxial films on Si substrates. The Al droplets are proved to efficiently improve the quality of as-grown GaN. On the one hand, they can act as nucleation seeds to facilitate the epitaxial growth, improving the crystalline quality and surface morphology of as-grown GaN epitaxial films. On the other hand, they also can compensate the huge compressive stress produced by Al buffer layer during the cooling process, achieving stress-free film. The density and volume of Al droplets greatly impact the properties of as-grown GaN epitaxial films. The GaN epitaxial film grown on the Al buffer layer with many small Al droplets uniformly distributed on it shows the best crystalline quality with the full-width at half maximum (FWHM) of GaN(0002) and GaN(10–12) as 0.5° and 0.7°, respectively, and flat surface with the smallest surface root-mean-square roughness of 3.8 nm. In addition, it also exhibits relatively better photoelectric properties with an FWHM of near band gap emission peak of 18 nm, carrier concentration of 2.0 × 1017 cm−3, and mobility of 137.1 cm2/Vs. This work has revealed the advantages of Al buffer layer and the important effects of buffer layer surface on achieving high-quality GaN by PLD, which is of significance for various applications of GaN-based devices.
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Dang S, Li C, Jia W, Liu H, Zhang Z, Li T, Liu X, Han P, Xu B (2013) Performance enhancement of GaN-based light-emitting diodes by surface plasmon coupling and scattering grating. J Mater Sci 48:5673–5679. doi:10.1007/s10853-013-7363-0
O’Leary SK, Foutz BE, Shur MS, Eastman LF (2006) Steady-state and transient electron transport within the III–V nitride semiconductors, GaN, AlN, and InN: a review. J Mater Sci 17:87–126. doi:10.1007/s10854-006-5624-2
Ahn KS, Kim DJ, Moon YT, Kim HG, Park SJ (2001) Effects of a two-step rapid thermal annealing process on Mg-doped p-type GaN films grown by metalorganic chemical vapor deposition. J Vac Sci Technol B 19:215. doi:10.1116/1.1338554
Mangla O, Srivastava MP (2013) GaN nanostructures by hot dense and extremely non-equilibrium plasma and their characterizations. J Mater Sci 48:304–310. doi:10.1007/s10853-012-6746-y
Li G, Wang W, Yang W, Wang H (2015) Epitaxial growth of group III-nitride films by pulsed laser deposition and their use in the development of LED devices. Surf Sci Rep 70:380–423
Kawashima T, Yoshikawa H, Adachi S, Fuke S, Ohtsuka K (1997) Optical properties of hexagonal GaN. J Appl Phys 82:3528–3535
Jones D, Lettington AH (1972) The electronic band structures of the wide band gap semiconductors GaN and A1N. Solid State Commun 11:701–705
Wang H, Wang W, Yang W, Zhou S, Lin Z, Li G (2015) Growth evolution of AlN films on silicon (111) substrates by pulsed laser deposition. J Appl Phys 117:185303
Li G, Wang W, Yang W, Lin Y, Wang H, Lin Z, Zhou S (2016) GaN-based light-emitting diodes on various substrates: a critical review. Rep Prog Phys 79:56501
Wang W, Yang W, Lin Y, Zhou S, Li G (2015) Microstructures and growth mechanisms of GaN films epitaxially grown on AlN/Si hetero-structures by pulsed laser deposition at different temperatures. Sci Rep 5:16453
Liu L, Edgar JH (2002) Substrates for gallium nitride epitaxy. Mater Sci Eng R Rep 37:61–127
Ishikawa H, Yamamoto K, Egawa T, Soga T, Jimbo T, Umeno M (1998) Thermal stability of GaN on (111) Si substrate. J Cryst Growth 189–190:178–182
Venugopal R, Wan J, Melloch M, Kim G, Zank G, Tsoi S, Ramdas A (2003) Comparison of various buffer schemes to grow GaN on large-area Si(111) substrates using metal-organic chemical-vapor deposition. J Electron Mater 32:371–374
Park JH, Park JH, Lee BT (2010) Effects of SiC buffer layer growth temperature on the residual strain of GaN/SiC/Si thin films. Mater Lett 64:1137–1139
Man BY, Yang C, Zhuang HZ, Liu M (2007) Effects of ZnO buffer layers on the fabrication of GaN films using pulsed laser deposition. J Appl Phys 101:93519
Park JH, Kim JH, Kim Y, Lee BT, Jang SJ, Moon CK, Song HJ (2003) Effects of silicon-on-insulator substrate on the residual stress within 3C-SiC/Si thin films. Appl Phys Lett 83:1989–1991
Hoshino K, Yanagita N, Araki M, Tadatomo K (2007) Effect of low-temperature GaN buffer layer on the crystalline quality of subsequent GaN layers grown by MOVPE. J Cryst Growth 298:232–234
Mohanta P, Singh D, Kumar R, Ganguli T, Srinivasa RS, Major SS (2013) Effect of ZnO buffer layer thickness on the epitaxial growth of GaN by reactive magnetron sputtering. Thin Solid Films 544:238–243
Wang H, Wang W, Yang W, Zhu Y, Lin Z, Li G (2016) Effect of residual stress on the microstructure of GaN epitaxial films grown by pulsed laser deposition. Appl Surf Sci 369:414–421
Barchuk M, Röder C, Shashev Y, Lukin G, Motylenko M, Kortus J, Pätzold O, Rafaja D (2014) Correlation between the residual stress and the density of threading dislocations in GaN layers grown by hydride vapor phase epitaxy. J Cryst Growth 386:1–8
Liu R, Ponce FA, Dadgar A, Krost A (2003) Atomic arrangement at the AlN/Si(111) interface. Appl Phys Lett 83:860–862
Fortuin AW, Alkemade PFA, Verbruggen AH, Steinfort AJ, Zandbergen H, Radelaar S (1996) Characterization of single-crystalline Al films grown on Si(111). Surf Sci 366:285–294
Bisch C, Boellaard E, Janssen GCAM, Alkemade PFA, Radelaar S (1998) Orientation of aluminum nuclei on Si(100) and Si(111). Thin Solid Films 336:84–88
Yang H, Wang W, Liu Z, Yang W, Li G (2014) Epitaxial growth mechanism of pulsed laser deposited AlN films on Si (111) substrates. CrystEngComm 16:3148–3154
Yang H, Wang W, Liu Z, Li G (2013) Epitaxial growth of 2 inch diameter homogeneous AlN single-crystalline films by pulsed laser deposition. J Phys D 46:105101–105106
Qiu XY, Liu HW, Fang F, Ha MJ, Liu JM (2006) Phase separation and interfacial reaction of high-kHfAlOx films prepared by pulsed-laser deposition in oxygen-deficient ambient. Appl Phys Lett 88:72906
Koblmueller G, Averbeck R, Geelhaar L, Riechert H, Hosler W, Pongratz P (2003) Growth diagram and morphologies of AlN thin films grown by molecular beam epitaxy. J Appl Phys 93:9591–9596
Takigawa S, Furuta K, Shimizu S, Shen XQ, Kitamura T, Okumura H (2004) Growth of droplet-free AlGaN buffer layer with +c polarity by molecular beam epitaxy. Jpn J Appl Phys 43:952–957
Jmerik VN, Mizerov AM, Nechaev DV, Aseev PA, Sitnikova AA, Troshkov SI, Kop’Ev PS, Ivanov SV (2012) Growth of thick AlN epilayers with droplet-free and atomically smooth surface by plasma-assisted molecular beam epitaxy using laser reflectometry monitoring. J Cryst Growth 354:188–192
Xiong H, Dai JN, Hui X, Fang YY, Tian W, Fu DX, Chen CQ, Li M, He Y (2013) Effects of the AlN buffer layer thickness on the properties of ZnO films grown on c-sapphire substrate by pulsed laser deposition. J Alloys Compd 554:104–109
Wang W, Wang H, Yang W, Zhu Y, Li G (2016) A new approach to epitaxially grow high-quality GaN films on Si substrates: the combination of MBE and PLD. Sci Rep 6:24448
Park BG, Kumar RS, Moon ML, Kim MD, Kang TW, Yang WC, Kim SG (2015) Comparison of stress states in GaN films grown on different substrates: langasite, sapphire and silicon. J Cryst Growth 425:149–153
Park BG (2015) Domain matching epitaxy of GaN films on a novel langasite substrate: an in-plane epitaxial relationship analysis. CrystEngComm 17:4455–4461
Wang W, Yang W, Liu Z, Lin Y, Zhou S, Lin Z, Wang H, Qian H, Li G (2015) Synthesis of high-quality AlN films on (La, Sr) (Al, Ta)O 3 substrates by pulsed laser deposition. Mater Lett 139:483–486
Chang CC, Wu XD, Ramesh R, Xi XX, Ravi TS, Venkatesan T, Hwang DM, Muenchausen RE, Foltyn S, Nogar NS (1990) Origin of surface roughness for c-axis oriented Y-Ba-Cu-O superconducting films. Appl Phys Lett 57:1814–1816
Warrender JM, Aziz MJ (2007) Effect of deposition rate on morphology evolution of metal-on-insulator films grown by pulsed laser deposition. Phys Rev B 75:794–802
Nootz G, Schulte A, Chernyak L, Osinsky A, Jasinski J, Benamara M, Lilientalweber Z (2002) Correlations between spatially resolved Raman shifts and dislocation density in GaN films. Appl Phys Lett 80:1355–1357
Zhu D, Wallis DJ, Humphreys CJ (2013) Prospects of III-nitride optoelectronics grown on Si. Rep Prog Phys 76:106501
Spaepen F (2000) Interfaces and stresses in thin films. Acta Mater 48:31–42
Kim C, Robinson IK, Myoung J, Shim K, Yoo MC, Kim K (1996) Critical thickness of GaN thin films on sapphire (0001). Appl Phys Lett 69:2358–2360
Parker CA, Roberts JC, Bedair SM, Reed MJ, Liu SX, El-Masry NA (1999) Determination of the critical layer thickness in the InGaN/GaN heterostructures. Appl Phys Lett 75:2776–2778
Andersson TG, Chen ZG, Kulakovskii VD, Uddin A, Vallin JT (1987) Variation of the critical layer thickness with In content in strained InxGa1−xAs-GaAs quantum wells grown by molecular beam epitaxy. Appl Phys Lett 51:752–754
Zhang L, Cheng K, Degroote S, Leys M, Germain M, Borghs G (2010) Strain effects in GaN epilayers grown on different substrates by metal organic vapor phase epitaxy. J Appl Phys 108:73522
Kushvaha SS, Kumar MS, Yadav BS, Tyagi PK, Ojha S, Maurya KK, Singh BP (2016) Influence of laser repetition rate on the structural and optical properties of GaN layers grown on sapphire (0001) by laser molecular beam epitaxy. CrystEngComm 18:744–753
Zhao DG, Xu SJ, Xie MH, Tong SY, Yang H (2003) Stress and its effect on optical properties of GaN epilayers grown on Si(111), 6H-SiC(0001), and c-plane sapphire. Appl Phys Lett 83:677–679
Davydov VY, Averkiev NS, Goncharuk IN, Nelson DK (1997) Raman and photoluminescence studies of biaxial strain in GaN epitaxial layers grown on 6H-SiC. J Appl Phys 82:5097–5102
Zhang L, Shao Y, Hao X, Wu Y, Zhang H, Qu S, Chen X, Xu X (2011) Improvement of crystal quality HVPE grown GaN on an H3PO4 etched template. CrystEngComm 13:5001–5004
Kong W, Jiao WY, Li JC, Collar K, Kim TH, Leach JH, Brown AS (2015) Effect of strain in sputtered AlN buffer layers on the growth of GaN by molecular beam epitaxy. Appl Phys Lett 107:353
Zhang GY, Tong YZ, Yang ZJ, Jin SX, Li J, Gan ZZ (1997) Relationship of background carrier concentration and defects in GaN grown by metalorganic vapor phase epitaxy. Appl Phys Lett 71:3376–3378
Shi JY, Yu LP, Wang YZ, Zhang GY, Zhang H (2002) Influence of different types of threading dislocations on the carrier mobility and photoluminescence in epitaxial GaN. Appl Phys Lett 80:2293–2295
Wang W, Chua SJ, Li G (2000) The hall mobility and its relationship with persistent photoconductivity of undoped GaN. J Electron Mater 29:27–30
Acknowledgements
This work is supported by National Science Fund for Excellent Young Scholars of China (No. 51422203), National Natural Science Foundation of China (Nos. 51572091 and 51372001), Outstanding Youth Foundation of Guangdong Scientific Committee (No. S2013050013882), Key Project in Science and Technology of Guangdong Province (Nos. 2014B010119001, 2014B010121004, and 2011A080801018), and Strategic Special Funds for LEDs of Guangdong Province (Nos. 2011A081301010, 2011A081301012, and 2012A080302002).
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Wang, H., Wang, W., Yang, W. et al. Employing Al buffer layer with Al droplets-distributed surface to obtain high-quality and stress-free GaN epitaxial films on Si substrates. J Mater Sci 52, 1318–1329 (2017). https://doi.org/10.1007/s10853-016-0427-1
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DOI: https://doi.org/10.1007/s10853-016-0427-1