234
2, APRIL 2005
Plasma–Surface Interaction and Surface Diffusion
During Silicon-Based Thin-Film Growth
J. P. M. Hoefnagels, E. Langereis, W. M. M. Kessels, and M. C. M. van de Sanden
Abstract—Insight into the interaction between plasma and the
surface can be obtained from well-defined radical and ion beam
studies using advanced surface diagnostics. Therefore, in this
paper, a new ultrahigh vacuum setup is presented for a funda-
mental study of the plasma deposition process of hydrogenated
amorphous silicon (a-Si:H). A first study of the surface diffusion
process of plasma radicals is presented by visualizing the surface
roughness evolution of the films as a function of bulk thickness
and substrate temperature.
Index Terms—Plasma deposition, surface diffusion, surface
reactions.
U NDERSTANDING of the plasma-surface interaction is
a major effort in plasma materials processing in which
plasmas are used for the synthesis and modification of thin films
and micro- and nano-structures. One of the most extensively
studied systems is the deposition process of a-Si:H which has
been studied even to such an extent that it has basically become
a model system for understanding thin film growth [1], [2]. Most
of these investigations have been carried out under regular, but
sometimes rather well-defined operating conditions for a-Si:H
deposition [3]. As a result, several surface reactions have been
proposed for the key growth precursor of a-Si:H, i.e., the SiH
radical (cf. Fig. 1). The reactions proposed have mainly been
concentrated on the adsorption mechanism of SiH (e.g., does
SiH adsorption require surface dangling bonds?) and the pos-
sible surface diffusion process of the radical. The latter aspect is
considered to be the explanation for the remarkable smoothness
of a-Si:H.
To reach the next level of understanding, i.e., detailed insight
into the surface reactions at the atomic scale, surface science-
like studies under very well defined and idealized conditions
will be required. Such studies can for example be carried out
by mimicking a-Si:H film growth using several radical and ion
beams as, e.g., done for Si plasma etching [4]. In this paper,
we present a new experimental setup for beam studies of a-Si:H
film growth. In the design of this setup (cf. Fig. 2), three basic
criteria have been taken into account.
1) The substrate, onto which the film is deposited, is easily
accessible by optical diagnostics. Different kinds of sub-
strates can be used and their surface remains clean for
Manuscript received June 29, 2004; revised September 16, 2004. This work
was supported in part by the Netherlands Foundation for Fundamental Research
on Matter (FOM) and in part the Netherlands Royal Academy of Arts and
Sciences (KNAW).
The authors are with the Department of Applied Physics, Eindhoven Univer-
sity of Technology, 5600 MB Eindhoven, The Netherlands (e-mail: j.p.m.hoef-
nagels@tue.nl; w.m.m.kessels@tue.nl).
Digital Object Identifier 10.1109/TPS.2005.845132
0093-3813/$20.00 © 2005 IEEE
IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 33, NO.
Fig. 1. Possible surface reactions of SiH radicals with the a-Si:H surface.
(a) Production of surface dangling bonds by H abstraction by SiH .
(b) Adsorption of SiH on a dangling bond and (c) insertion of SiH in
a surface Si–Si bond. In reactions (b) and (c), surface diffusion of the SiH
growth precursor may be involved.
a sufficiently long time due to the high level of vacuum
reached in the setup.
2) With well-defined radical (and ion) beams, film growth
under regular deposition conditions can be mimicked. For
a-Si:H, radical beams of SiH and H are most appropriate.
3) The growth process can be investigated by advanced in
situ diagnostics which are “all-optical” techniques able to
monitor film growth in real time. The techniques avail-
able or currently under development are innovative and
are mainly focused on the detection of surface hydrogen
and surface dangling bonds (cf. Fig. 2) such that key ques-
tions of a-Si:H film growth can be addressed.
A first major issue addressed is the diffusion process of
surface species such as adsorbed SiH radicals. As shown by
Collins et al. [4], insight into surface diffusion processes can
be obtained by monitoring the surface roughness evolution as a
function of film bulk thickness by spectroscopic ellipsometry.
Ellipsometry with a photon energy range of 0.7–5.0 eV has
therefore been used to monitor film growth between substrate
temperatures of 70 C and 450 C under SiH dominated
conditions (11-A filament current, 3 standard cm /min SiH
flow, 8-mtorr pressure). The resulting a-Si:H deposition rates
on the c-Si substrates range from 78 to 102 Å/min. The ellip-
sometry data has been analyzed by a two layer model (bulk
a-Si:H/surface roughness) with the common Bruggeman effec-
tive medium approximation of 50% voids and 50% bulk a-Si:H
for the surface roughness layer. The Tauc–Lorentz formalism
is assumed for the a-Si:H dielectric function [5]. A contour
plot of the surface roughness as a function of bulk thickness
and substrate temperature, as shown in Fig. 3, is generated by
interpolation between the different substrate temperatures used.
Fig. 3 shows an initial surface roughness of at the
onset of bulk growth for all substrate temperatures. This initial
surface roughness is induced by the nucleation process of a-Si:H
on the native-oxide surface which takes place by Volmer–Weber
type of growth leading to hemisphere-like nucleation sites. For
HOEFNAGELS et al.: PLASMA-SURFACE INTERACTION AND SURFACE DIFFUSION DURING SILICON-BASED THIN FILM GROWTH 235

Fig. 2. (a) Side view picture and (b) schematic top view of the new UHV setup. On the right side, the different plasma and radicals sources are shown, i.e., electron
cyclotron resonance (ECR) plasma source for SiH beam production, thermal source for atomic H beam production (H-source), and a hot wire source for a-Si:H
film growth. Also shown are several of the optical diagnostics to study the radical surface interaction during plasma deposition (attenuated total reflection Fourier
transform infrared spectroscopy for the detection of surface hydrides; second harmonic generation for the detection of surface dangling bonds; and spectroscopy
ellipsometry to investigate the surface roughness evolution and surface diffusion).

creases again. This is the so called a-Si a-Si roughening transi-

tion which is caused by the fact that the surface diffusion mech-
anism is not able to stabilize roughness features at long lateral
length scales that start dominating the surface roughness. These
roughness features start growing at initial film growth but they
only become important at a certain film thickness. The condi-
tions for which the roughness at long lateral length scales are
suppressed the most, i.e., for which the “dip” lasts up to the
highest bulk thickness and for which the lowest surface rough-
ness is obtained in the dip, correspond to the conditions in which
the surface mobile species have the longest diffusion length [5].
As shown in Fig. 3, this means that the longest diffusion length is
obtained at 300 C, the temperature that also yields the highest
film smoothness for thick films. In future experiments, these ob-
servations will be interpreted in terms of the microscopic surface
diffusion process of SiH plasma radicals.

Fig. 3. Contour of the surface roughness d (in angstroms) as a function of
the bulk thickness d and the substrate temperature T , as determined with
spectroscopic ellipsometry during a-Si:H deposition. Minimum value of d at
d = 200 
 
A at T = 275 C and the most “delayed” increase in d for
large d at T 
= 325 C suggest that the surface diffusion length of the
growth precursors is at maximum at T 
= 300 C.
substrate temperatures 150 C, the surface roughness first de-
creases and this can be explained by a surface diffusion mecha-
nism which is effective on relatively short lateral length scales.
Surface mobile species are able to reach the valleys between the
nucleation sites and can smoothen out the nucleation-induced
roughness. This is not the case for temperatures 150 C for
which the surface roughness monotonically increases. For sub-
strate temperatures 150 C, a minimum (“dip”) in the sur-
face roughness is reached after which the surface roughness in-
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