Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Atomistics of vapour–liquid–solid nanowire growth

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms2956· OSTI ID:1623911
 [1];  [2];  [3];  [4]
  1. Northeastern Univ., Boston, MA (United States). Dept. of Mechanical and Industrial Engineering. Group for Simulation and Theory of Atomic-Scale Material Phenomena (stAMP); Brown Univ., Providence, RI (United States). School of Engineering; DOE/OSTI
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate; Colorado School of Mines, Golden, CO (United States). Division of Engineering
  4. Northeastern Univ., Boston, MA (United States). Dept. of Mechanical and Industrial Engineering. Group for Simulation and Theory of Atomic-Scale Material Phenomena (stAMP); Northeastern Univ., Boston, MA (United States). Dept. of Bioengineering

Vapour–liquid–solid route and its variants are routinely used for scalable synthesis of semiconducting nanowires, yet the fundamental growth processes remain unknown. Here we employ atomic-scale computations based on model potentials to study the stability and growth of gold-catalysed silicon nanowires. Equilibrium studies uncover segregation at the solid-like surface of the catalyst particle, a liquid AuSi droplet, and a silicon-rich droplet–nanowire interface enveloped by heterogeneous truncating facets. Supersaturation of the droplets leads to rapid one-dimensional growth on the truncating facets and much slower nucleation-controlled two-dimensional growth on the main facet. Surface diffusion is suppressed and the excess Si flux occurs through the droplet bulk which, together with the Si-rich interface and contact line, lowers the nucleation barrier on the main facet. The ensuing step flow is modified by Au diffusion away from the step edges. Our study highlights key interfacial characteristics for morphological and compositional control of semiconducting nanowire arrays.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1623911
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 4; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (66)

Silicon Nanowires: A Review on Aspects of their Growth and their Electrical Properties journal June 2009
Formation of Single Tiers of Bridging Silicon Nanowires for Transistor Applications Using Vapor-Liquid-Solid Growth from Short Silicon-on-Insulator Sidewalls journal November 2009
Three-Dimensional Nanoscale Composition Mapping of Semiconductor Nanowires journal February 2006
Elementary Processes in Nanowire Growth journal February 2011
Catalyst Incorporation at Defects during Nanowire Growth journal December 2011
Kinetically Induced Kinking of Vapor−Liquid−Solid Grown Epitaxial Si Nanowires journal November 2009
The Incredible Shrinking Circuit journal September 2001
Wetting of Si surfaces by Au–Si liquid alloys journal April 2003
Control of growth mechanisms and orientation in epitaxial Si nanowires grown by electron beam evaporation journal March 2009
Some Theorems on the Free Energies of Crystal Surfaces journal April 1951
Diameter dependence of the growth velocity of silicon nanowires synthesized via the vapor-liquid-solid mechanism journal January 2007
Angular-dependent embedded atom method potential for atomistic simulations of metal-covalent systems journal November 2009
Growth rate of a crystal facet of arbitrary size and growth kinetics of vertical nanowires journal September 2004
Atomistic simulation study of the structure and dynamics of a faceted crystal-melt interface journal September 2008
From Droplets to Nanowires: Dynamics of Vapor-Liquid-Solid Growth journal May 2009
Determination of Size Effects during the Phase Transition of a Nanoscale Au-Si Eutectic journal October 2009
Periodically Changing Morphology of the Growth Interface in Si, Ge, and GaP Nanowires journal July 2011
Geometrical Frustration in Nanowire Growth journal December 2011
Liquid/Vapor Surface Tension of Metals: Embedded Atom Method with Charge Gradient Corrections journal March 2001
Sawtooth Faceting in Silicon Nanowires journal September 2005
Diameter-Independent Kinetics in the Vapor-Liquid-Solid Growth of Si Nanowires journal March 2006
Kinetics of Individual Nucleation Events Observed in Nanoscale Vapor-Liquid-Solid Growth journal November 2008
Oscillatory Mass Transport in Vapor-Liquid-Solid Growth of Sapphire Nanowires journal October 2010
Surface Crystallization in a Liquid AuSi Alloy text January 2006
Fundamental aspects of VLS growth journal December 1975
The Au/Si(111) interface: Growth mode, energetics, structural and electronic properties journal September 1981
One-dimensional nanostructures: Chemistry, physics & applications journal August 1998
Size and habit evolution of PETN crystals—a lattice Monte Carlo study journal June 2006
Semiconductor nanowires for novel one-dimensional devices journal March 2004
Structural investigation of silicon nanowires using GIXD and GISAXS: Evidence of complex saw-tooth faceting journal August 2008
Cyclic Supersaturation and Triple Phase Boundary Dynamics in Germanium Nanowire Growth journal February 2011
On the Nature and Origin of Si Surface Segregation in Amorphous AuSi Alloys journal February 2010
Diameter-Dependent Growth Direction of Epitaxial Silicon Nanowires journal April 2005
Single-crystal metallic nanowires and metal/semiconductor nanowire heterostructures journal July 2004
The influence of the surface migration of gold on the growth of silicon nanowires journal January 2006
Colossal injection of catalyst atoms into silicon nanowires journal April 2013
Direct measurement of dopant distribution in an individual vapour–liquid–solid nanowire journal March 2009
Critical surface roughening journal January 1976
Vapor-liquid-solid mechanism of single crystal growth journal March 1964
Steady growth of nanowires via the vapor-liquid-solid method journal August 2007
Doping nanowires grown by the vapor-liquid-solid mechanism journal August 2009
Diffusion coefficient of 195 Au in the liquid Au 0.81 Si 0.19 alloy journal May 1982
Controlling nanowire structures through real time growth studies journal October 2010
The Growth of Crystals and the Equilibrium Structure of their Surfaces
  • Burton, W. K.; Cabrera, N.; Frank, F. C.
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 243, Issue 866 https://doi.org/10.1098/rsta.1951.0006
journal June 1951
Some Theorems on the Free Energies of Crystal Surfaces journal April 1951
Energy and vibrational spectrum of the Si(111) (7×7) surface from empirical potentials journal August 1988
Structural phase transitions of Si ( 111 ) − ( 3 × 3 ) R 30 ° − Au : Phase transitions in domain-wall configurations journal April 1998
Size-dependent elasticity of nanowires: Nonlinear effects journal June 2005
Diameter dependence of the growth velocity of silicon nanowires synthesized via the vapor-liquid-solid mechanism journal January 2007
Angular-dependent embedded atom method potential for atomistic simulations of metal-covalent systems journal November 2009
Role of nonlinear effects in nanowire growth and crystal phase journal November 2009
Growth rate of a crystal facet of arbitrary size and growth kinetics of vertical nanowires journal September 2004
Atomistic simulation study of the structure and dynamics of a faceted crystal-melt interface journal September 2008
Size-dependent nucleation kinetics at nonplanar nanowire growth interfaces journal November 2009
From Droplets to Nanowires: Dynamics of Vapor-Liquid-Solid Growth journal May 2009
Determination of Size Effects during the Phase Transition of a Nanoscale Au-Si Eutectic journal October 2009
Periodically Changing Morphology of the Growth Interface in Si, Ge, and GaP Nanowires journal July 2011
Geometrical Frustration in Nanowire Growth journal December 2011
Liquid/Vapor Surface Tension of Metals: Embedded Atom Method with Charge Gradient Corrections journal March 2001
Sawtooth Faceting in Silicon Nanowires journal September 2005
Diameter-Independent Kinetics in the Vapor-Liquid-Solid Growth of Si Nanowires journal March 2006
Nucleation Energy Barriers for Volume-Conserving Shape Changes of Crystals with Nonequilibrium Morphologies journal September 2001
Surface Crystallization in a Liquid AuSi Alloy journal July 2006
Molecular dynamics simulations of gold-catalyzed growth of silicon bulk crystals and nanowires journal June 2011
Elastic and Anelastic Behavior of Materials in Small Dimensions journal January 2002
Nanoscale Science and Technology: Building a Big Future from Small Things journal July 2003

Cited By (9)

Atomic Resolution Monitoring of Cation Exchange in CdSe-PbSe Heteronanocrystals during Epitaxial Solid–Solid–Vapor Growth journal May 2014
Non-equilibrium induction of tin in germanium: towards direct bandgap Ge1−xSnx nanowires journal April 2016
Flexible and Ultrasoft Inorganic 1D Semiconductor and Heterostructure Systems Based on SnIP journal February 2019
Inducing imperfections in germanium nanowires journal March 2017
A surface curvature oscillation model for vapour–liquid–solid growth of periodic one-dimensional nanostructures journal March 2015
In situ characterization of kinetics and mass transport of PbSe nanowire growth via LS and VLS mechanisms journal January 2019
The structural and optical properties of black silicon by inductively coupled plasma reactive ion etching journal November 2014
Growth dynamics of SiGe nanowires by the vapour–liquid–solid method and its impact on SiGe/Si axial heterojunction abruptness journal June 2018
CMOS-Compatible Silicon Nanowire Field-Effect Transistor Biosensor: Technology Development toward Commercialization journal May 2018

Similar Records

Synthesis of nanostructures in nanowires using sequential catalyst reactions
Journal Article · Mon Jul 13 00:00:00 EDT 2015 · Nature Materials · OSTI ID:1235860

Effect of catalyst diameter on vapour-liquid-solid growth of GaAs nanowires
Journal Article · Thu Aug 14 00:00:00 EDT 2014 · Journal of Applied Physics · OSTI ID:22314594

Vapor-liquid-solid growth of <110> silicon nanowire arrays
Journal Article · Thu Sep 19 00:00:00 EDT 2013 · Proceedings of SPIE - The International Society for Optical Engineering · OSTI ID:1149578