Quantitative Analysis of Nanoscale Step Dynamics in High-Temperature Solution-Grown Single Crystal 4H-SiC via In Situ Confocal Laser Scanning Microscope

Nanoscale understanding of high-temperature crystal growth dynamics in solution has been a challenge to be tackled by many researchers engaged in investigating solution processes for bulk single crystal growth. Here we propose a new approach to in situ observation at a buried solid/liquid interface in high-temperature solution using a conventional confocal laser scanning microscope. In the solution growth of 4H-SiC with Si–Ni based alloy flux as a model system, we show the ability to quantitatively analyze step motions at the growing SiC crystal on the nanoscale at high temperatures up to 1700 °C in a vacuum. The temperature-dependent step-advance rates for various steps with different step heights demonstrated the advantageous effect of adding Al to the flux on the step-flow growth of SiC: addition of just 4 at% Al effectively suppressed step-bunching. These experiments point to the importance of in situ nanoscale observation in understanding solution growth mechanisms, and hence the potential to acceler...

[1]  K. Fujiwara,et al.  In-situ observations of melt growth behavior of polycrystalline silicon , 2004 .

[2]  Y. Yonezawa,et al.  Screening of metal flux for SiC solution growth by a thin-film combinatorial method , 2011, Science and technology of advanced materials.

[3]  Hiroshi Nakagawa,et al.  Self-ordering of nanofacets on vicinal SiC surfaces. , 2003, Physical review letters.

[4]  S. Kawanishi,et al.  Real-time observation of the interface between SiC and a liquid alloy and its application to the dissolution behavior of SiC at 1573 K , 2013 .

[5]  S. Maruyama,et al.  Uniform growth of SiC single crystal thin films via a metal–Si alloy flux by vapour–liquid–solid pulsed laser deposition: the possible existence of a precursor liquid flux film , 2016 .

[6]  P. Hansma,et al.  Atomic-scale imaging of calcite growth and dissolution in real time , 1992 .

[7]  J. García‐Ruiz,et al.  In Situ Observation of Step Dynamics on Gypsum Crystals , 2010 .

[8]  H. Shibata,et al.  “In-situ” Real Time Observation of Planar to Cellular and Cellular to Dendritic Transition of Crystals Growing in Fe–C Alloy Melts , 1996 .

[9]  K. Fujiwara,et al.  In situ observations of crystal growth behavior of silicon melt , 2002 .

[10]  P. Vekilov,et al.  Characteristic lengthscales of step bunching in KDP crystal growth: in situ differential phase-shifting interferometry study , 2002 .

[11]  G. Sazaki,et al.  Elementary steps at the surface of ice crystals visualized by advanced optical microscopy , 2010, Proceedings of the National Academy of Sciences.

[12]  S. Nishitani,et al.  Metastable solvent epitaxy of SiC , 2008 .

[13]  H. Okumura,et al.  Growth rate and surface morphology of 4H–SiC crystals grown from Si–Cr–C and Si–Cr–Al–C solutions under various temperature gradient conditions , 2014 .

[14]  I. Sunagawa,et al.  Nucleation, growth and stability of CaAl2Si2O8 polymorphs , 1991 .

[15]  K. Tsukamoto,et al.  In situ observation of elementary growth steps on the surface of protein crystals by laser confocal microscopy , 2004 .

[16]  S. Kawanishi,et al.  Real-Time Observation of High Temperature Interface between SiC Substrate and Solution during Dissolution of SiC , 2013 .

[17]  吉三 猪股,et al.  4H-, 6H-SiCの安定性に及ぼす不純物アルミニウムの影響 , 1970 .

[18]  K. Kuribayashi,et al.  Rapid solidification processes of semiconductors from highly undercooled melts , 2001 .

[19]  S. Nakadate,et al.  Application of real time phase shift interferometer to the measurement of concentration field , 1993 .

[20]  M. Boćkowski,et al.  Real-time observation system development for high-temperature liquid/solid interfaces and its application to solid-source solution growth of AlN , 2015 .

[21]  T. Itoh,et al.  In Situ Visualization of Lithium Ion Intercalation into MoS2 Single Crystals using Differential Optical Microscopy with Atomic Layer Resolution. , 2016, Journal of the American Chemical Society.

[22]  T. Martin,et al.  Substrate temperature reference using SiC absorption edge measured by in situ spectral reflectometry , 2003 .

[23]  M. Sleutel,et al.  In situ measurement of crystal surface dynamics in pure and contaminated solutions by Confocal Microscopy and Atomic Force Microscopy , 2013 .

[24]  D. Hofmann,et al.  Prospects of the use of liquid phase techniques for the growth of bulk silicon carbide crystals , 1999 .

[25]  S. Kawanishi,et al.  Analysis of the Spiral Step Structure and the Initial Solution Growth Behavior of SiC by Real-Time Observation of the Growth Interface , 2016 .

[26]  K. Tsukamoto In Situ observation of mono-molecular growth steps on crystals growing in aqueous solution. I , 1983 .

[27]  K. Tsukamoto,et al.  Step velocity in tetragonal lysozyme growth as a function of impurity concentration and mass transport conditions , 2006 .

[28]  K. Tsukamoto,et al.  Chiral and Achiral Mechanisms of Regulation of Calcite Crystallization , 2008 .

[29]  S. Maruyama,et al.  Effect of Al addition to Si–Ni flux on pulsed laser deposition of SiC thin films , 2016 .

[30]  E. Oelkers,et al.  Magnesite growth rates as a function of temperature and saturation state , 2009 .

[31]  Q. Wahab,et al.  Liquid phase epitaxial growth of SiC , 1999 .

[32]  A. Lupulescu,et al.  In Situ Imaging of Silicalite-1 Surface Growth Reveals the Mechanism of Crystallization , 2014, Science.