Analysis of InGaN nanodots grown by droplet heteroepitaxy using grazing incidence small-angle X-ray scattering and electron microscopy

Woodward, J. M.; Nikiforov, A. Yu.; Ludwig, K. F.; Moustakas, T. D.

doi:10.1063/1.4986272

Analysis of InGaN nanodots grown by droplet heteroepitaxy using grazing incidence small-angle X-ray scattering and electron microscopy

Journal Article · Mon Aug 14 00:00:00 EDT 2017 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4986272· OSTI ID:1473886

^[1]; Nikiforov, A. Yu. ^[2]; Ludwig, K. F. ^[3]; Moustakas, T. D. ^[4]

Boston Univ., MA (United States). Dept. of Electrical and Computer Engineering, and Photonics Center; Department of Electrical and Computer Engineering, Boston University, Boston, Massachusetts 02215
Boston Univ., MA (United States). Photonics Center
Boston Univ., MA (United States). Dept. of Physics
Boston Univ., MA (United States). Dept. of Electrical and Computer Engineering, and Photonics Center, and Division of Materials Science and Engineering

We present a detailed structural investigation of self-assembled indium gallium nitride nanodots grown on c-plane aluminum nitride templates by the droplet heteroepitaxy technique in a plasma-assisted molecular beam epitaxy reactor. Various growth parameters, including the total coverage of the metal species, relative and total metal effusion fluxes, and nitridation temperature were investigated. Analyses of in situ reflection high-energy electron diffraction patterns and comparison with simulations showed that the resulting crystal structure was a mixture of wurtzite and twinned zinc blende phases, with the zinc blende phase increasingly dominant for lower metal coverages and lower nitridation temperatures, and the wurtzite phase increasingly dominant for higher nitridation temperature. Studies by field emission scanning electron microscopy and atomic force microscopy revealed that the nanodots exhibit trimodal size distributions, with the dot morphologies of the intermediate size mode often resembling aggregations of distinct clusters. Nanodots grown at higher nitridation temperatures had larger inter-dot spacings, with hexagonal in-plane ordering observable at a sufficiently high temperature. Using grazing incidence small angle X-ray scattering, we determined the nanodots to be approximately truncated cone shaped, and extracted the mean radius, height, and inter-dot distance for each distribution. Microstructural investigations of the nanodots by cross-sectional transmission electron microscopy indicated that the majority of the dots were formed in dislocation-free regions, and confirmed that the intermediate size dots were approximately truncated cone shaped and consisted of both zinc blende and wurtzite regions. Mapping of the elemental distributions by energy dispersive X-ray spectroscopy in scanning transmission electron microscopy mode indicated highly nonuniform indium distributions within both small and intermediate size dots which are potentially indicative of indium clustering and kinetically controlled nanoscale phase separation rather than the spinodal decomposition associated with bulk diffusion. In conclusion, the observed enrichment in indium concentration towards the tops of the nanodot layers could be ascribed to the compositional pulling effect.

View Accepted Manuscript (DOE)

Research Organization:: Boston Univ., MA (United States). Trustees

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-06ER46332

OSTI ID:: 1473886

Alternate ID(s):: OSTI ID: 1374928

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 6 Vol. 122; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (45)

Growth of III-nitride quantum dots and their applications to blue-green LEDs Moustakas, T. D.; Xu, Tao; Thomidis, C. physica status solidi (a), Vol. 205, Issue 11 https://doi.org/10.1002/pssa.200880222	journal	November 2008
Analysis of InGaN/GaN single quantum wells by X-ray scattering and transmission electron microscopy Smeeton, T. M.; Kappers, M. J.; Barnard, J. S. physica status solidi (b), Vol. 240, Issue 2 https://doi.org/10.1002/pssb.200303262	journal	November 2003
InGaN quantum dot growth in the limits of Stranski-Krastanov and spinodal decomposition: InGaN quantum dots Figge, Stephan; Tessarek, Christian; Aschenbrenner, Timo physica status solidi (b), Vol. 248, Issue 8 https://doi.org/10.1002/pssb.201147165	journal	July 2011
Microstructural and compositional analyses of GaN-based nanostructures: Microstructural and compositional analyses of GaN-based nanostructures Pretorius, Angelika; Schmidt, Thomas; Aschenbrenner, Timo physica status solidi (b), Vol. 248, Issue 8 https://doi.org/10.1002/pssb.201147175	journal	July 2011
Transmission Electron Microscopy Williams, David B.; Carter, C. Barry https://doi.org/10.1007/978-0-387-76501-3	book	January 2009
The Ga-In (Gallium-Indium) System Anderson, T. J.; Ansara, I. Journal of Phase Equilibria, Vol. 12, Issue 1 https://doi.org/10.1007/BF02663677	journal	February 1991
New MBE growth method for InSb quantum well boxes Koguchi, Nobuyuki; Takahashi, Satoshi; Chikyow, Toyohiro Journal of Crystal Growth, Vol. 111, Issue 1-4 https://doi.org/10.1016/0022-0248(91)91064-H	journal	May 1991
Stresses in thin films: The relevance of grain boundaries and impurities Hoffman, R. W. Thin Solid Films, Vol. 34, Issue 2 https://doi.org/10.1016/0040-6090(76)90453-3	journal	May 1976
Ga-droplet-induced formation of GaAs nano-islands by chemical beam epitaxy Ro, Jeong-Rae; Kim, Sung-Bock; Park, Kyoungwan Journal of Crystal Growth, Vol. 201-202 https://doi.org/10.1016/S0022-0248(99)00034-2	journal	May 1999
Molecular beam epitaxy of GaN, AlN, InN and related alloys: from two- to three-dimensional growth mode Daudin, B.; Feuillet, G.; Mula, Guido Diamond and Related Materials, Vol. 9, Issue 3-6 https://doi.org/10.1016/S0925-9635(99)00220-4	journal	April 2000
Phase separation in thick InGaN layers – A quantitative, nanoscale study by pulsed laser atom probe tomography Müller, M.; Smith, G. D. W.; Gault, B. Acta Materialia, Vol. 60, Issue 10 https://doi.org/10.1016/j.actamat.2012.04.030	journal	June 2012
Influence of a low-temperature capping on the crystalline structure and morphology of InGaN quantum dot structures Krause, B.; Miljevic, B.; Aschenbrenner, T. Journal of Alloys and Compounds, Vol. 585 https://doi.org/10.1016/j.jallcom.2013.09.005	journal	February 2014
Control of threading dislocation density at the initial growth stage of AlN on c-sapphire in plasma-assisted MBE Nechaev, D. V.; Aseev, P. A.; Jmerik, V. N. Journal of Crystal Growth, Vol. 378 https://doi.org/10.1016/j.jcrysgro.2012.12.080	journal	September 2013
Density functional calculations of the strain effects on binding energies and adatom diffusion on (0001) GaN surfaces Grandusky, J. R.; Jindal, V.; Raynolds, J. E. Materials Science and Engineering: B, Vol. 158, Issue 1-3 https://doi.org/10.1016/j.mseb.2008.12.042	journal	February 2009
Growth of InGaN quantum dots with AlGaN barrier layers via modified droplet epitaxy Oliver, Rachel A.; El-Ella, Haitham A. R.; Collins, Daniel P. Materials Science and Engineering: B, Vol. 178, Issue 20 https://doi.org/10.1016/j.mseb.2013.08.011	journal	December 2013
Probing surface and interface morphology with Grazing Incidence Small Angle X-Ray Scattering Renaud, Gilles; Lazzari, Rémi; Leroy, Frédéric Surface Science Reports, Vol. 64, Issue 8 https://doi.org/10.1016/j.surfrep.2009.07.002	journal	August 2009
Vaporization Catalysis. The Decomposition of Gallium Nitride ¹ Schoonmaker, Richard C.; Buhl, Albert; Lemley, James The Journal of Physical Chemistry, Vol. 69, Issue 10 https://doi.org/10.1021/j100894a035	journal	October 1965
Solid phase immiscibility in GaInN Ho, I‐hsiu; Stringfellow, G. B. Applied Physics Letters, Vol. 69, Issue 18 https://doi.org/10.1063/1.117683	journal	October 1996
Real time control of InxGa1−xN molecular beam epitaxy growth Grandjean, N.; Massies, J. Applied Physics Letters, Vol. 72, Issue 9 https://doi.org/10.1063/1.120970	journal	March 1998
Nanometer-scale InGaN self-assembled quantum dots grown by metalorganic chemical vapor deposition Tachibana, K.; Someya, T.; Arakawa, Y. Applied Physics Letters, Vol. 74, Issue 3 https://doi.org/10.1063/1.123078	journal	January 1999
Self-assembled carbon-induced germanium quantum dots studied by grazing-incidence small-angle x-ray scattering Stangl, J.; Holý, V.; Mikulı́k, P. Applied Physics Letters, Vol. 74, Issue 25 https://doi.org/10.1063/1.124179	journal	June 1999
Metalorganic chemical vapor deposition selective growth and characterization of InGaN quantum dots Wang, J.; Nozaki, M.; Lachab, M. Applied Physics Letters, Vol. 75, Issue 7 https://doi.org/10.1063/1.124564	journal	August 1999
Self-assembled InGaN quantum dots grown by molecular-beam epitaxy Adelmann, C.; Simon, J.; Feuillet, G. Applied Physics Letters, Vol. 76, Issue 12 https://doi.org/10.1063/1.126098	journal	March 2000
Selective growth of InGaN quantum dot structures and their microphotoluminescence at room temperature Tachibana, Koichi; Someya, Takao; Ishida, Satomi Applied Physics Letters, Vol. 76, Issue 22 https://doi.org/10.1063/1.126632	journal	May 2000
Growth of self-assembled GaN quantum dots via the vapor–liquid–solid mechanism Hu, C. -W.; Bell, A.; Ponce, F. A. Applied Physics Letters, Vol. 81, Issue 17 https://doi.org/10.1063/1.1514394	journal	October 2002
Droplet heteroepitaxy of GaN quantum dots by metal-organic chemical vapor deposition Gherasimova, M.; Cui, G.; Jeon, S. -R. Applied Physics Letters, Vol. 85, Issue 12 https://doi.org/10.1063/1.1793343	journal	September 2004
Real-time x-ray studies of gallium nitride nanodot formation by droplet heteroepitaxy Wang, Yiyi; Özcan, Ahmet S.; Sanborn, Christopher Journal of Applied Physics, Vol. 102, Issue 7 https://doi.org/10.1063/1.2786578	journal	October 2007
Optical properties of GaSb/GaAs type-ІІ quantum dots grown by droplet epitaxy Kawazu, Takuya; Mano, Takaaki; Noda, Takeshi Applied Physics Letters, Vol. 94, Issue 8 https://doi.org/10.1063/1.3090033	journal	February 2009
Heteroepitaxy, polymorphism, and faulting in GaN thin films on silicon and sapphire substrates Lei, T.; Ludwig, K. F.; Moustakas, T. D. Journal of Applied Physics, Vol. 74, Issue 7 https://doi.org/10.1063/1.354414	journal	October 1993
Temperature dependent transport studies in InN quantum dots grown by droplet epitaxy on silicon nitride/Si substrate Kumar, Mahesh; Roul, Basanta; Shetty, Arjun Applied Physics Letters, Vol. 99, Issue 15 https://doi.org/10.1063/1.3651762	journal	October 2011
Phase separation in strained epitaxial InGaN islands Niu, Xiaobin; Stringfellow, Gerald B.; Liu, Feng Applied Physics Letters, Vol. 99, Issue 21 https://doi.org/10.1063/1.3662927	journal	November 2011
Nucleation and growth of thin films Venables, J. A.; Spiller, G. D. T.; Hanbucken, M. Reports on Progress in Physics, Vol. 47, Issue 4 https://doi.org/10.1088/0034-4885/47/4/002	journal	April 1984
GaSb/GaAs type-II quantum dots grown by droplet epitaxy Liang, Baolai; Lin, Andrew; Pavarelli, Nicola Nanotechnology, Vol. 20, Issue 45 https://doi.org/10.1088/0957-4484/20/45/455604	journal	October 2009
Anomalous Surface Reflection of X Rays Yoneda, Y. Physical Review, Vol. 131, Issue 5 https://doi.org/10.1103/PhysRev.131.2010	journal	September 1963
Kinetics of droplet growth processes: Simulations, theory, and experiments Family, Fereydoon; Meakin, Paul Physical Review A, Vol. 40, Issue 7 https://doi.org/10.1103/PhysRevA.40.3836	journal	October 1989
X-ray and neutron scattering from rough surfaces Sinha, S. K.; Sirota, E. B.; Garoff, S. Physical Review B, Vol. 38, Issue 4 https://doi.org/10.1103/PhysRevB.38.2297	journal	August 1988
Compositional pulling effects in In x Ga 1 − x N / G a N layers: A combined depth-resolved cathodoluminescence and Rutherford backscattering/channeling study Pereira, S.; Correia, M. R.; Pereira, E. Physical Review B, Vol. 64, Issue 20 https://doi.org/10.1103/PhysRevB.64.205311	journal	November 2001
Strong phase separation of strained In x Ga 1 − x N layers due to spinodal and binodal decomposition: Formation of stable quantum dots Tessarek, C.; Figge, S.; Aschenbrenner, T. Physical Review B, Vol. 83, Issue 11 https://doi.org/10.1103/PhysRevB.83.115316	journal	March 2011
Analysis of island shape evolution from diffuse x-ray scattering of organic thin films and implications for growth Frank, C.; Banerjee, R.; Oettel, M. Physical Review B, Vol. 90, Issue 20 https://doi.org/10.1103/PhysRevB.90.205401	journal	November 2014
Nonequilibrium Composition Profiles of Alloy Quantum Dots and their Correlation with the Growth Mode Niu, X. B.; Stringfellow, G. B.; Liu, Feng Physical Review Letters, Vol. 107, Issue 7 https://doi.org/10.1103/PhysRevLett.107.076101	journal	August 2011
Scaling of the Droplet-Size Distribution in Vapor-Deposited Thin Films Family, Fereydoon; Meakin, Paul Physical Review Letters, Vol. 61, Issue 4 https://doi.org/10.1103/PhysRevLett.61.428	journal	July 1988
A Threshold Selection Method from Gray-Level Histograms Otsu, Nobuyuki IEEE Transactions on Systems, Man, and Cybernetics, Vol. 9, Issue 1 https://doi.org/10.1109/TSMC.1979.4310076	journal	January 1979
New Self-Organized Growth Method for InGaAs Quantum Dots on GaAs(001) Using Droplet Epitaxy Mano, Takaaki; Watanabe, Katsuyuki; Tsukamoto, Shiro Japanese Journal of Applied Physics, Vol. 38, Issue Part 2, No. 9A/B https://doi.org/10.1143/JJAP.38.L1009	journal	September 1999
InAs Quantum Dots Growth by Modified Droplet Epitaxy Using Sulfur Termination Mano, Takaaki; Watanabe, Katsuyuki; Tsukamoto, Shiro Japanese Journal of Applied Physics, Vol. 39, Issue Part 1, No. 7B https://doi.org/10.1143/JJAP.39.4580	journal	July 2000
Gwyddion: an open-source software for SPM data analysis Nečas, David; Klapetek, Petr Open Physics, Vol. 10, Issue 1 https://doi.org/10.2478/s11534-011-0096-2	journal	January 2012

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