Solar Energy 77 (2004) 749–756

www.elsevier.com/locate/solener

Low cost processing of CIGS thin film solar cells

1
M. Kaelin *, D. Rudmann, A.N. Tiwari
Thin Film Physics Group, ETH Zürich, Technoparkstr. 1, CH-8005 Zürich, Switzerland

Received 19 February 2004; received in revised form 18 August 2004; accepted 23 August 2004
Available online 21 September 2004

Communicated by: Associate Editor T. M. Razykov

Abstract

A set of low cost techniques with realistic potential for direct manufacturing costs reduction were developed in the
last five years while the industrial Cu(In,Ga)Se2 (CIGS) solar cell production is based on vacuum processes, which
require high initial investment into production machines. The common properties of these low cost techniques are
the use of simple and fast non-vacuum deposition methods and the prefixing of the film-composition on a molecular
level in a precursor layer, which is chemically and thermally treated to form a high quality CIGS film. The paste coating
approaches use premixed inks which are applied by doctor-blade coating to yield solar cell efficiencies of 13.6%, with the
potential to reach 15% and more in the next years. The choice of the precursor material has to be made with respect to
the used selenization conditions to avoid detrimental impurity phases. A new precursor material is discussed, which
allows fast conversion in selenium atmosphere and was used to produce solar cells with 6.7% efficiency. The CIGS film
thickness has to be increased for complete absorption of the incident light.

2004 Elsevier Ltd. All rights reserved.

Keywords: CIGS; Thin film; Non-vacuum; Selenization

1. Introduction ment in photovoltaics. Nevertheless in recent years, the

The direct conversion of sunlight into electrical en-
ergy is a preferred method for clean and safe energy pro-
duction in future. As long as cheap traditional energy
resources are still abundant, a breakthrough of photo-
voltaics is only possible with low production costs.
Niche markets such as space and off-grid applications
have always been the motor for research and develop-
* ment required for machines, another is the shortage of
Corresponding author. Tel.: +41 1 445 14 81; fax: +41 1
445 14 99.
E-mail address: kaelin@phys.ethz.ch (M. Kaelin).
1
Also at: Department of Electronic and Electrical Engi-
neering, Loughborough University, UK.
photovoltaic market with its fast annual growth rates
of over 35% during 1996–2003 has started to attract
the attention of investors, looking for new promising
investment fields. Thin-film solar cell technologies have
raised the expectation that photovoltaics will be able
to compete with traditional energy production methods
due to expected lower processing costs. But so far with
none of the used technologies the promised potential
has been achieved and the global production volume is
still below 750 MW/Year. One reason is the high invest-
feed stock for silicon-wafer technology, which is still
dominating the market. More research and development
is necessary for the breakthrough in commercial manu-
facturing technologies for thin film photovoltaics.

0038-092X/$ - see front matter
2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.solener.2004.08.015
750 M. Kaelin et al. / Solar Energy 77 (2004) 749–756
Among the investigated thin film absorber materials
polycrystalline Cu(Inx,Ga1 x)(SySe1 y)2, (CIGS) is one
of the favourites, since it has a high optical absorption
coefficient, a tuneable band gap and somewhat benign
grain boundaries (Schock and Noufi, 2000). The conven-
tional CIGS solar cell is a layer stack consisting of a
molybdenum back contact, the CIGS absorber, a thin
CdS or ZnS or In2S3 buffer layer, and a bilayer of intrin-
sic and aluminium doped zinc oxide as transparent con-
ductive oxide (TCO) front contact. Traditionally, this
layer stack is deposited on a soda-lime glass substrate,
but the recent trend includes flexible substrates such as
polymer or metal-foils. These substrate materials are
better suited for many applications including photo-
voltaic integrated buildings and space power generation
and they allow roll-to-roll manufacturing, leading to
substantial cost reductions.
This paper focuses on techniques with low initial
investment for the production equipment. Therefore,
simple deposition techniques such as spraying and paste
coating are reviewed. Electrodeposition is not covered in
detail since another article in this journal issue focuses
thereon.
2. Conventional CIGS deposition processes
Sophisticated vacuum co-evaporation techniques (Fig.
1) give the best control of composition and composi-
tional grading through the films. A maximum CIGS cell
efficiency of 19.3% has been obtained by a three-stage
co-evaporation process (Ramanathan et al., 2003). The
three-stage process has not been implemented in indus-
trial large area module production. However, other
co-evaporation process variants are used for module
production as large as 1.2 · 0.6 m2 at Global Solar and
Würth Solar (Powalla and Dimmler, 2001).
Shell Solar and Showa Shell preferred selenization
processes (also called two stage processes, Fig. 1) for
Fig. 1. Vacuum methods for CIGS deposition.
industrial module production. These processes consist
of the deposition of a precursor material with a sub-
sequent thermal annealing in controlled reactive
atmosphere. Typically, the sputter deposition of a me-
tal-alloy precursor is followed by selenization and sulfu-
rization in reactive H2Se and H2 ambient, or recently, by
evaporation of a selenium layer on the metal precursor
followed by a rapid thermal annealing (Palm et al.,
2003). A controlled band gap grading is more difficult
to achieve, but the use of a post sulfurization step led
to module efficiencies of over 14% (30 · 30 cm2) and
good process yield, showing the mature status of this
technology (Kushiya, 2003). Although low cost CIGS
solar modules can be produced by such vacuum-based
deposition techniques, high initial investment is required
for the sophisticated vacuum deposition equipment and
module costs will depend strongly on the production
volume and of course high efficiency.
3. Low cost processes
There are many criteria for characterizing low cost
processes. CIGS layer deposition remains the challeng-
ing step for low cost cell processing, since it is the most
important and complex layer of the cell. High material
utilization efficiencies close to 100% are important in
order to keep material costs and processing waste as
small as possible. These low cost techniques generally
follow the idea of the sequential techniques since a low
temperature precursor deposition step precedes a chem-
ical reaction or annealing step at higher temperature
(Fig. 2). Furthermore, they use prefixed metal ratios in
the precursor and aim for fast deposition with techno-
logically simple and reliable low cost equipment.
Although all the component layers of the cell (metal
back contact, buffer, front contact) can be grown with
non-vacuum methods, more research and development
is necessary for the application of low cost contact layers
 M. Kaelin et al. / Solar Energy 77 (2004) 749–756
Fig. 2. Low cost, non-vacuum methods for CIGS deposition.
in thin film solar cells. Some issues on non-vacuum TCO
layers from sintered nanoparticles were presented, but
the required sintering temperature for suitable low
sheet-resistances is still too high for the application in
solar cells (Ederth et al., 2003; Eberspacher et al., 2002).
4. Non-vacuum absorber formation techniques
Non-vacuum technologies use simple and low cost
equipment and enable fast processing speed. But the
lack of a high purity vacuum environment during
processing has to be compensated with a careful choice
of precursor materials and additives to avoid undesired
contamination. As shown in Fig. 2, two different ap-
proaches evolved: In one the precursor materials decom-
pose during deposition on the substrate and form the
CIGS compound directly (spray pyrolysis, electrodepo-
sition of compound layers) whereas in the second ap-
proach, the precursor material is deposited as a thin
layer that is subjected to a chemical treatment and sele-
nization thereafter (paste coating, electrodeposition of
metal layers). Even if CIGS formation during deposition
is an appealing approach, the as-produced material is of-
ten of poor quality, includes impurity phases and may be
amorphous or microcrystalline due to the low deposition
temperatures (<400 C). The quality is generally im-
proved with a second processing step, where the material
is annealed at higher temperature.
5. Chemical spray pyrolysis
Although the spray pyrolysis technique is one of the
best-investigated non-vacuum deposition processes
(mainly for CuInS2), only few results about cell perform-
751
ance were reported. To the best of our knowledge, the
efficiency record dates back to 1989 (Duchemin et al.,
1989) and is 5% for a small area cell. The spray tech-
nique to disperse and deposit a precursor solution is very
well suited for uniform large area coating. The process
consists of the decomposition and reaction of premixed
precursors, generally metal-chlorides and a chalcogen
compound (typically N,N-dimethyl selenourea or thio-
urea), on a heated substrate (300–400 C) (Pamplin
and Feigelson, 1979; Brown and Bates, 1990). Draw-
backs of this technique are impurity phases (binary
oxide and chalcogenide phases), traces from the reaction
by-products (chlorine and carbon) and the relatively
small grain-size obtained. Annealing treatments in con-
trolled atmosphere can reduce the impurity concentra-
tion and enhance crystallinity (Krunks et al., 2002;
Marsillac et al., 2003).
New precursor solutions deal with organic single
source precursors (Fig. 3). The idea behind the develop-
ment of single source precursors is to lower the CIGS
formation temperature and to avoid the formation of
impurity phases, since the synthesis is controlled on a
Fig. 3. Single source precursor molecule for CuInS2 synthesis
(Banger et al., 2002).
752 M. Kaelin et al. / Solar Energy 77 (2004) 749–756

molecular level (Hirpo et al., 1993; Banger et al., 2002).
These organic precursors decompose and form CIGS at
temperatures below 400 C. Given the lack of commer-
cial availability of these precursors efficient synthesis
reactions which allow compositional tuning are re-
quired. Research and development is going on in this
direction (Banger et al., 2003).
6. Electrodeposition
Electrodeposition has been successfully used to de-
posit quaternary CIGS films with a small area efficiency
of over 10% after a subsequent thermal annealing
(Guimard et al., 2003). By applying additional In and
Ga and a high temperature annealing in vacuum, an effi-
ciency of 15.4% was obtained (Bhattacharya et al.,
2000). The stability of the chemical solution, large area
uniformity and high deposition rates are still a challenge.
Electrodeposition of an elemental-layer stack which was
subjected to a selenization treatment led to 7–10% effi-
cient devices (Kapur et al., 1987; Kampmann et al.,
2003).
soft and reactive metals resulted in mechanically alloyed
CIS powder, which requires sintering temperatures higher
than pure metal powder. A solution to this problem was
presented by using copper-indium-alloyed powder pro-
duced by gas atomization (Basol, 2000). The alloy is more
brittle than pure In and therefore allows ball milling to
produce finer powder. CIS devices produced by seleniza-
tion in diluted H2Se gas yielded efficiencies in the range of
10–11%, although some porosity remained in the film,
which was attributed to the randomly shaped precursor
particles (Fig. 4a).
Layers of metal-oxide nanoparticles allowed an
apparently higher packing density due to smaller particle
size and uniformly round shape (Fig. 4b). Furthermore,
gallium could be introduced into the precursor material,
which led to a higher open-circuit voltage and devices
with maximum efficiencies of 11.7% (Eberspacher
et al., 2002) and 13.6% (Kapur et al., 2003b). Still higher
efficiencies above 15% may be reached if a better control
of the Ga grading is achieved. The chemical conversion
of the stable oxides to CIGS requires well optimized
reactions. Such a two stage process includes a reduction
step in diluted hydrogen prior to selenization with
diluted H2Se (Kapur et al., 2003b).

7. Paste coating

Typical paste coating techniques are screen printing,

doctor-blade coating and curtain coating. Paste coating
is a fast process and can be applied in continuous roll-to-
roll deposition. The paste is prepared with the precursor
materials (e.g. nanoparticles) in the desired stoichiome-
try and a liquid binder, used as a transfer media. Paste
rheology can be tailored with material load and addi-
tives, which affect the final film thickness and homogene-
ity (Kapur et al., 2003a). In contrast to liquid
atomization (spraying), where valuable portions of the
precursor material are wasted, paste coating allows a
very efficient use of the material and exhibits higher
packing densities (Eberspacher et al., 2003). Material
loss minimization is very desirable for precursors con-
taining expensive elements like indium and gallium.
After deposition, the precursor layer is sintered and
converted to the CIGS layer in controlled atmosphere
(Fig. 2).
After some preliminary work on high temperature
sintering (780 C) of CuInSe2 (CIS) pellets from a pow-
dered CIS ingot (Gombia et al., 1983), it was quite a
challenge to produce homogenous thin layers by sinter-
ing of ground material (Arita et al., 1988; Vervaet et al.,
1991). The motivation for the approach was the success-
ful development of screenprinted and sintered CdTe/
CdS solar cells. Nevertheless, in the case of CIS, the pre-
cursor powders used to formulate screen printable pastes Fig. 4. Cross-sections of particulate precursor layers: (a)
had too big particle size (5–50 lm) and did not lead to sprayed Cu–In alloy precursor layer, and (b) doctor-blade
compact single-phase thin layers. Ball-mill grinding of coated Cu–In compound precursor layer (Basol, 2000).
 M. Kaelin et al. / Solar Energy 77 (2004) 749–756
It is an ongoing discussion if the highly toxic H2Se gas,
though diluted to a small concentration in N2, or the less
hazardous selenium vapour should be used for seleniza-
tion in industrial production. An experimental compari-
son study concluded that H2Se selenization gives more
uniform layers with better control, especially at moderate
selenization temperatures of 400–500 C (Alberts, 2002).
Nevertheless, there are some restrictions on the use of
H2Se in many European countries and costly security
measures are required in industrial production.
In an effort to get rid of the H2Se gas, various nano-
sized precursor materials, metal-oxides, metal-selenides
and pure metals, were tested for their conversion poten-
tial in selenium vapour (Kaelin et al., 2003). Fig. 5 shows
the morphology and cross-section of selenized nanopar-
ticle precursor layers. Selenization was done in a two-
temperature-zone quartz reactor where the substrate
temperature was typically at 500–550 C and the sele-
nium source at 300–450 C. The reaction time was be-
tween 10 and 30 min. Metal precursor layers formed a
dense CIS top layer of about 1 lm grain size on a small
grained underlayer. The sintering reaction starts from
top and proceeds through the film. The top layer thus
formed may slow down the sintering process for thicker
layers and may prevent the complete conversion of the
precursor. As a result, impurities (mainly oxygen) intro-
duced during precursor deposition may remain in the
Fig. 5. Morphology and cross-sections of selenized precursor layers from metal (a), metal selenide (b) and metal-oxide precursor
particles (c).
753
layer (Kaelin et al., 2004). Even if coarsening was ob-
served for selenide precursor layers, no densification oc-
curred and the layers were cracked after selenization.
Similar problems were observed with oxide precursors.
The selenium content in the layer was measured with
EDX (Energy dispersive X-ray analysis) and should be
50% for a complete reaction. Resulting layers from
oxide precursors showed typical selenium contents of
30–40%, whereas for selenide and metal precursors typ-
ically 47–51% were obtained. By using higher pressures
of selenium vapour it was possible to increase the sele-
nium content to nearly 50%, but the problem of cracking
persisted for oxides and selenides. Only solar cells made
from metal precursors showed a photovoltaic behaviour,
even though efficiencies were poor (1%), mainly be-
cause of not fully converted underlayers, still containing
In2O3 as an impurity phase. Precursor materials that can
be used for direct conversion to the CIGS compound by
reaction with selenium should therefore prevent the for-
mation of In and Ga oxide phases, which are difficult to
convert into selenide.
Recently we tested a new precursor material for paste
coating and selenization. In Fig. 6 the X-ray diffraction
pattern shows the absence of Cu-, In- and Ga related
binary impurity phases. A compact submicron CIGS
layer with large grains is formed (Fig. 7). Devices made
with this proprietary process show AM1.5 efficiencies up
754 M. Kaelin et al. / Solar Energy 77 (2004) 749–756

8. Conclusions and future prospects

The promising results from paste coating and seleni-

Fig. 6. XRD pattern of selenized precursor layer.
Fig. 7. Cross-section of selenized precursor layer.
to 6.7% (VOC: 404 mV, JSC: 27.2 mA/cm2, FF: 61%).
Given the thin absorber of 0.5–1 lm, shunting and insuf-
ficient absorption of incident photons may be responsi-
ble for the low efficiency. Therefore the process
parameters have to be optimized to obtain 1.5–2 lm
thick and smooth absorbers with suitable composition
(higher Ga content), which would improve the cell
efficiency.
Table 1 summarizes the process parameters of recent
paste coating processes.
zation methods as well as electrodeposition have shown
that non-vacuum deposition processes can be used for
high quality CIGS absorber formation. After unsuccess-
ful initial attempts with paste coating, the breakthrough
followed only five years ago when non-vacuum proc-
esses with efficiencies above 10% were announced. In
the mean time the maximum efficiency on soda-lime
glass was increased to 13.6% and the process was suc-
cessfully applied to flexible substrates (Kapur et al.,
2003b), while flexible cells have somewhat low efficiency.
Still there is some room left for optimization, especially
the layer thickness and band gap grading need better
control to reach to a realistic potential of 15–16% with
these methods.
Simple and fast processing techniques with high
(nearly 100%) material utilization yield will have a ben-
eficial influence on the manufacturing costs of CIGS
solar cells. Zweibel (Zweibel, 1999) has investigated
issues to achieve manufacturing costs of 50$/m2, con-
cluding that present capital and maintenance costs for
thin film semiconductor processes are too high, leading
to poor product cost-competitiveness. Paste coating
does not require expensive vacuum equipment which
keeps initial investments and maintenance costs on a
low level. Therefore the direct manufacturing cost per
square meter is significantly lower compared to vacuum
deposited absorber layers and the ambitious energy cost
target of 1$/Wp can already be reached with module
efficiencies between 6% and 8%. Low cost processes do
not primarily need to be tuned for highest efficiencies
but for high process yield.
Acknowledgments
The funding by the Swiss Federal Commission for
technology and Innovation is gratefully acknowledged.
Further, the authors would like to thank Dr. V.K.
Kapur from ISET for valuable discussions and also to

Table 1
Process parameters and efficiencies of recent paste coating processes
Institution Precursor deposition Reaction conditions g max (%) Substrate, Area (cm2) Reference
a
ISET Doctor-blade H2, H2Se, 475–550 C 13.6 Glass, 0.08 Kapur et al. (2003b)
11.7 Mo foil
8.9 Upilex
8 65 (mini-module)
Unisunb Doctor-blade/spray H2, H2Se, 400–600 C 11.7 not indicated Eberspacher et al. (2002)
ETHZc Doctor blade Se, 550 C 6.7 Glass, 0.08 Kaelin et al. (in press)
a
International Solar Electric Technology (California, USA).
b
Unisun (California, USA).
c
Swiss Federal Institute of Technology (Zürich, Switzerland).
 M. Kaelin et al. / Solar Energy 77 (2004) 749–756
Dr. Banger and Dr. Hepp from the NASA Glenn Re-
search Center for allowing to use their illustration mate-
rial in this paper.
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