© 2005 The Royal Microscopical Society
Journal of Microscopy, Vol. 219, Pt 2 August 2005, pp. 69– 75
Received 23 December 2004; accepted 23 May 2005
Blackwell Publishing, Ltd.
Cross-sectional TEM investigation of nickel-catalysed carbon
nanotube films grown by plasma-enhanced CVD
Y. YAO, L. K. L. FALK, R. E. MORJAN,* O. A. NERUSHEV* &
E. E. B. CAMPBELL*
Department of Applied Physics, Chalmers University of Technology, SE-412 96 Göteborg, Sweden
*Department of Physics, Göteborg University, SE-412 96 Göteborg, Sweden
Key words. CNT film, cross-sectional TEM, interface, metal dusting, Ni-catalyst,
nucleation.
Received 23 December 2004; accepted 23 May 2005
Summary
Nickel-catalysed multiwall carbon nanotubes synthesized by
plasma-enhanced chemical vapour deposition on a silicon substrate
with acetylene and ammonia at 700 °C have been characterized
by high-resolution and analytical transmission electron micro-
scopy. The nucleation of the carbon nanotubes occurs as a con-
sequence of the carburization and dusting of supported preformed
nickel- and silicon-rich particles. This process yields disintegrated
silicon-containing nickel particles dispersed in dome-shaped
carbon islands adherent to the substrate. The particles act as
catalysts for tube growth, resulting in aligned multiwall carbon
nanotubes with a bamboo-like structure anchored to the dome-
shaped carbon islands. The bottom part of the carbon islands
contains bundles of graphene sheets orientated parallel to the
substrate. The nanotubes are capped with fcc nickel particles
containing dissolved silicon. Most of these particles have a conical
shape orientated with a <110> direction along the tube growth
axis, and with {110} and {111} planes as exposed faces.
Introduction
In light of the possible applications of carbon nanotubes (CNTs)
for nano-electronic devices and electron field-emission sources,
plasma-enhanced chemical vapour deposition (PECVD) has
attracted considerable attention in recent years. The PECVD
technique provides a promising synthesis method to satisfy the
demands for micro/nano-electronic devices, e.g. highly ordered
orientation, low defect level, reproducibility and controllable
properties. A uniform and high growth rate of CNT films using
different plasma CVD techniques has been achieved with con-
trolled alignment, precise positioning, and controlled height and
diameter of the structures (Ren et al., 1998; Choi et al., 2000,
2003; Merkulov et al., 2000; Chowalla et al., 2001; Chang
et al., 2002; Morjan et al., 2004).
Generally, nickel-catalysed CNTs grown by PECVD show a tip-
growth behaviour, which has been explained by the weak inter-
action between the nickel catalysts and the silicon substrate. The
generally accepted mechanism for tip growth (Baker et al., 1972)
suggests that the carbon from decomposed hydrocarbon stock
gas is dissolved at the front surface of the catalytic particle causing
oversaturation, diffusion and precipitation on the rear surface
to form graphene sheets with a tubular structure. The detailed
structure at the base of the CNTs at the interface with the substrate,
which contains the essential information on nucleation and
growth, is, however, usually disregarded in the literature. This
is because CNTs are usually characterized using dispersed CNT
samples in transmission electron microscopy (TEM).
In this paper we report cross-sectional TEM observations and
local analyses at the base of nickel-catalysed CNT films synthesized
by PECVD. The purpose is to characterize fully the interface
between the silicon substrate and the film of tip-grown CNTs,
and to develop a better understanding of the nucleation and
growth of CNTs on the microscopic scale.
Materials and methods
A nickel thin film with nominal thickness of 30 nm was depos-
ited on polished silicon (002) wafers by electron beam evapo-
ration at room temperature. The substrate was ultrasonically
cleaned in isopropanol before deposition, and dried in flowing
nitrogen. The coated substrate was then transferred into a
CVD chamber and heated at 700 °C for 15 min in flowing
argon and hydrogen. The nanotubes were thereafter grown
in an acetylene : ammonia = 1 : 5 atmosphere at a pressure of
4 torr for 1, 5 and 10 min. A DC voltage of 400 V was supplied
for plasma production with a current density of 0.5–1 mA cm
-2
.
Samples taken for characterization after heat treatment only
and after nanotube growth were furnace cooled in a mixture
of flowing argon and hydrogen.
The reaction products were characterized by scanning electron
microscopy (SEM) of the exposed surfaces. The nanotubes grown Correspondence to: Professor Lena K. L. Falk. E-mail: lklfalk@fy.chalmers.se