Evolution of shape, size, and areal density of a single plane of Si nanocrystals embedded in SiO2 matrix studied by atom probe tomography

Single planes of Si nanocrystals (NCs) embedded in a SiO2 matrix were synthesized by annealing SiO2/SiO/SiO2 multilayer structures deposited on Si (100) substrates by e-beam evaporation. The dependence of the shape, size, and areal density of Si NCs on the thickness of the initial SiO layer was investigated using atom probe tomography and validated by energy filtered transmission electron microscopy. Three kinds of samples were prepared with SiO layer thicknesses of 4, 6, and 10 nm. The size of Si NCs enlarged with increasing SiO layer thickness. The shape of Si NCs was mainly extended spheroid in all three kinds of samples. In the sample with the 4 nm-thick SiO layer, the Si NCs were more prolate than those in the other two samples. Moreover, many rod-shaped Si NCs appeared in the sample with the 10 nm-thick SiO layer. These rod-shaped Si NCs were found to be connected by small Si NCs. The areal densities of Si NCs were in the order of 1012 NCs per cm2 in all samples.

[1]  M. Zacharias,et al.  Si nanocrystal based memories: Effect of the nanocrystal density , 2006 .

[2]  T. Gregorkiewicz,et al.  Direct generation of multiple excitons in adjacent silicon nanocrystals revealed by induced absorption , 2012, Nature Photonics.

[3]  Baptiste Gault,et al.  Reconstructing atom probe data: a review. , 2013, Ultramicroscopy.

[4]  Di Liang,et al.  Recent progress in lasers on silicon , 2010 .

[5]  Panagiotis Dimitrakis,et al.  Manipulation of two-dimensional arrays of Si nanocrystals embedded in thin SiO2 layers by low energy ion implantation , 2004 .

[6]  Sandip Tiwari,et al.  A silicon nanocrystals based memory , 1996 .

[7]  S. Lombardo,et al.  Observation of the nucleation kinetics of Si quantum dots on SiO2 by energy filtered transmission electron microscopy , 2003 .

[8]  Brian P. Gorman,et al.  Atom Probe Tomography of Electronic Materials , 2007 .

[9]  T. Mikolajick,et al.  Sponge-like Si-SiO2 nanocomposite—Morphology studies of spinodally decomposed silicon-rich oxide , 2013 .

[10]  R. Walters,et al.  Field-effect electroluminescence in silicon nanocrystals , 2005, Nature materials.

[11]  M. Perego,et al.  Behavior of phosphorous and contaminants from molecular doping combined with a conventional spike annealing method. , 2014, Nanoscale.

[12]  M. Zacharias,et al.  Phosphorus doping of Si nanocrystals embedded in silicon oxynitride determined by atom probe tomography , 2014 .

[13]  N. Cherkashin,et al.  Imaging Si nanoparticles embedded in SiO(2) layers by (S)TEM-EELS. , 2008, Ultramicroscopy.

[14]  S. Ringer,et al.  Quantitative atom probe analysis of nanostructure containing clusters and precipitates with multiple length scales. , 2011, Ultramicroscopy.

[15]  Synthesis of mono and bi-layer of Si nanocrystals embedded in a dielectric matrix by e-beam evaporation of SiO/SiO2 thin films , 2006 .

[16]  L. Kourkoutis,et al.  Three-dimensional imaging for precise structural control of Si quantum dot networks for all-Si solar cells. , 2013, Nanoscale.

[17]  D. Seidman,et al.  Best-fit ellipsoids of atom-probe tomographic data to study coalescence of γ′ (L12) precipitates in Ni–Al–Cr , 2007, cond-mat/0703452.

[18]  Stephen Y. Chou,et al.  A Silicon Single-Electron Transistor Memory Operating at Room Temperature , 1997, Science.

[19]  J. Heitmann,et al.  Size-controlled highly luminescent silicon nanocrystals: A SiO/SiO2 superlattice approach , 2002 .

[20]  F. Gourbilleau,et al.  Phase transformation in SiOx/SiO₂ multilayers for optoelectronics and microelectronics applications. , 2013, Ultramicroscopy.

[21]  M. Roussel,et al.  Efficient n-type doping of Si nanocrystals embedded in SiO2 by ion beam synthesis , 2013 .

[22]  A. Pérez‐Rodríguez,et al.  Influence of average size and interface passivation on the spectral emission of Si nanocrystals embedded in SiO2 , 2002 .

[23]  M. Perego,et al.  Scaling size of the interplay between quantum confinement and surface related effects in nanostructured silicon , 2013 .

[24]  Size and location control of Si nanocrystals at ion beam synthesis in thin SiO2 films , 2002, cond-mat/0208137.

[25]  M. Ueda,et al.  Focused ion beam direct deposition and its applications , 1998 .

[26]  David J. Larson,et al.  Atom Probe Tomography 2012 , 2012 .

[27]  A. Nishida,et al.  Phosphorus and boron diffusion paths in polycrystalline silicon gate of a trench-type three-dimensional metal-oxide-semiconductor field effect transistor investigated by atom probe tomography , 2015 .

[28]  G. Hwang,et al.  On the origin of Si nanocrystal formation in a Si suboxide matrix , 2007 .

[29]  D. Muller,et al.  Three-dimensional imaging of nonspherical silicon nanoparticles embedded in silicon oxide by plasmon tomography , 2006 .

[30]  J. Leburton,et al.  Intraband absorption in silicon nanocrystals: The combined effect of shape and crystal orientation , 2005 .

[31]  K. Wilford,et al.  A sensitivity analysis of the maximum separation method for the characterisation of solute clusters. , 2011, Ultramicroscopy.

[32]  Chang-Hee Cho,et al.  Quantum confinement effect in crystalline silicon quantum dots in silicon nitride grown using SiH4 and NH3 , 2006 .

[33]  F. Gourbilleau,et al.  Confined phase separation in SiOx nanometric thin layers , 2013 .

[34]  A. Nishida,et al.  Three-Dimensional Dopant Characterization of Actual Metal–Oxide–Semiconductor Devices of 65 nm Node by Atom Probe Tomography , 2013 .

[35]  Fabio Iacona,et al.  Correlation between luminescence and structural properties of Si nanocrystals , 2000 .

[36]  Sang Kyun Kim,et al.  Strong size-dependent characteristics of carrier injection in quantum-confined silicon nanocrystals , 2009 .

[37]  E A Kenik,et al.  Atom Probe Tomography: A Technique for Nanoscale Characterization , 2004, Microscopy and Microanalysis.

[38]  Michael P Moody,et al.  New Techniques for the Analysis of Fine-Scaled Clustering Phenomena within Atom Probe Tomography (APT) Data , 2007, Microscopy and Microanalysis.

[39]  Naoki Yokoyama,et al.  MICROSTRUCTURE AND OPTICAL ABSORPTION PROPERTIES OF SI NANOCRYSTALS FABRICATED WITH LOW-PRESSURE CHEMICAL-VAPOR DEPOSITION , 1996 .

[40]  F. Gourbilleau,et al.  Atomic characterization of Si nanoclusters embedded in SiO2 by atom probe tomography , 2011, Nanoscale research letters.

[41]  M. Perego,et al.  Silicon crystallization in nanodot arrays organized by block copolymer lithography , 2014, Journal of Nanoparticle Research.

[42]  A Membrane Device for Substrate‐Free Photovoltaic Characterization of Quantum Dot Based p‐i‐n Solar Cells , 2012, Advanced materials.

[43]  Orsay,et al.  Multi-dot floating-gates for nonvolatile semiconductor memories: Their ion beam synthesis and morphology , 2004, cond-mat/0407329.