A new architecture for solar cells involving a metal bridge deposited

between active TiO2 particles

Sahrul Saehana, Pepen Arifin, Khairurrijal, and Mikrajuddin Abdullah
Citation: J. Appl. Phys. 111, 123109 (2012); doi: 10.1063/1.4730393
View online: http://dx.doi.org/10.1063/1.4730393
View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v111/i12
Published by the American Institute of Physics.

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JOURNAL OF APPLIED PHYSICS 111, 123109 (2012)

A new architecture for solar cells involving a metal bridge deposited between
active TiO2 particles
Sahrul Saehana, Pepen Arifin, Khairurrijal, and Mikrajuddin Abdullaha)
Department of Physics, Bandung Institute of Technology, Jalan Ganeca 10, Bandung 40132, Indonesia

(Received 1 January 2012; accepted 21 May 2012; published online 22 June 2012)
The efficiency of titanium dioxide (TiO2)-based film solar cells fabricated by combined spray and
electroplating methods was improved by forming metal bridges in the pores between TiO2
nanoparticles. The interfaces between TiO2 nanoparticles and metal bridges formed Schottky
contacts, which minimized recombination of electron-hole pairs and increased electron transfer. A
maximum efficiency of 4.38% was achieved for cells plated at 50 mA and 55  C. This efficiency is
higher than that reported for solar cells with a similar structure [Saehana et al., AIP Conf. Proc.
1284, 154 (2010); 1415, 163 (2011); IJBAS/IJENS 11, 15 (2011)]. We also identified that both
current and temperature influence the morphology of the metal bridges and efficiency of the solar
C 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4730393]
cell. V

I. INTRODUCTION

TiO2 has attracted a great deal of attention for solar

energy applications13 because of its relatively high
efficiency,24 easy fabrication,5,6 low cost,7,8 low toxicity,8
and long term stability.9 However, its large band gap
(Eg 3.2 eV) means that TiO2 requires near UV light for
photoactivation. Moreover, the high rate of electron-hole
recombination on TiO2 particles results in TiO2-based solar
cells lacking dyes showing low efficiency.
Significant effort has been devoted to enhancing the
activity of TiO2. A popular method is to minimize electronhole recombination by depositing metal on the semiconductor surface.1023 In this approach, electrons excited in TiO2
are trapped by the metal, reducing the probability of
electron-hole recombination. The process of electron trapping at the Schottky barrier of a metal (copper) in contact
with a TiO2 surface is depicted in Fig. 1.
In this paper, we report the inhibition of electron-hole
recombination by quickly capturing photoelectrons using
metallic bridges and transferring them to the main electrode.
A schematic diagram of the solar cells and the corresponding
band energy diagram are presented in Figs. 2(a) and 2(b),
respectively.
The diagram in Fig. 2(a) depicts an electron trapped at
the Schottky barrier formed at a metal/semiconductor interface, highlighting the small area of the semiconductor surface covered by the metal. The excited electron moves to the
metal and becomes trapped, reducing the probability of
electron-hole recombination. The migration of electrons to
metal particles has been confirmed by an observed reduction
in the photoconductance of the semiconductor in Cu/TiO2
devices.10 The equilibrium band diagram of a contacting
metal and semiconductor reveals that electrons flow to the
metal from the semiconductor.

a)

E-mail address: din@fi.itb.ac.id.

0021-8979/2012/111(12)/123109/7/$30.00

The recombination of holes and electrons is an important electronic process in solar cells, and the rate of recombination plays a crucial role in the conversion of solar energy
into electricity. The mean lifetime of a single electron-hole
pair is approximately 30 ns,24 so electrons must be trapped
within this time to inhibit recombination. In this system,
trapping at metal-semiconductor contacts and trapping of
conduction band electrons in TiO2 particles occur very rapidly (in less than 40 ps).24 For this reason, local separation of
electron-hole pairs through the introduction of Schottky
junctions is an effective method to inhibit recombination.
We previously minimized recombination and increased
the quantum efficiency of solar cells by modifying TiO2 thin
films using a nanocomposite consisting of interconnected
metal (Cu or Zn) to improve electron transport.2527 In this
study, indium tin oxide (ITO) of varying conductivity was
used in solar cells to determine its effect on internal resistance and performance. The cells also contained polyvinyl acetate (PVA) as a polymer electrolyte and lithium ions for
ionic transport and to increase the short circuit current. Copper was deposited in the space between TiO2 particles by
electroplating. We recently reported solar cells with a similar
structure, but they were not fabricated using optimum electroplating parameters such as current source and bath temperature.26,27 Herein, we also investigated the effect of metal
particle size and electroplating parameters such as bath temperature and current density on cell performance. A subsidiary goal of the study was to demonstrate the use of simple
and low-cost methods such as electroplating to deposit metal
in the space between TiO2 particles.
II. EXPERIMENTAL

TiO2 thin films were deposited on ITO-coated glass substrates using a spray method. A suspension was prepared by
dispersing TiO2 (10 g) in water (10 ml) and mixing with a
magnetic stirrer for 45 min. The TiO2 suspension was sprayed
on the substrate at a temperature of 150  C.28 The spraying

111, 123109-1

C 2012 American Institute of Physics

V

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123109-2

Saehana et al.

FIG. 1. Photoexcitation on a copper-coated TiO2 surface.10

process was repeated 20 times. The resulting thick film of

TiO2 was heated on a hot plate at 250  C for 30 min to evaporate the water, and then sintered at 450  C for 30 min to
improve the electrical contact between the TiO2 particles and
ITO substrate. Metallic Cu was deposited on the TiO2 film

FIG. 2. (a) Architecture of TiO2 solar cells containing metal bridges, and
(b) band energy diagram of metal-semiconductor (Schottky) junction at
equilibrium.

J. Appl. Phys. 111, 123109 (2012)

using an electroplating system. The plating bath was operated

at a temperature of 25, 55, or 95  C, and the plating current
was maintained at 50, 150, or 300 mA. The plating solution
was a Watts-type bath containing copper sulfate (CuSO4,
20 ml, 0.1 M). A copper rod with a purity of 99.99% and
length of 5 cm was used as the anode and the TiO2 film was
used as the cathode. In the electroplating process, the electroplating voltage was 5 V, the deposition time was 25 s, the
anode-cathode separation was 15 cm, and the pH was 4.6.
A polymer electrolyte was prepared by dissolving LiOH
(0.5 g) in water (10 ml) and adding PVA (0.8 g, Bratachem,
Indonesia). The mixture was heated at 110  C with stirring
for 1 h to produce a gel-like electrolyte. The electrolyte was
manually applied to the Cu/TiO2 film, and then an aluminum
electrode was deposited under vacuum.
The crystal structures of the films were analyzed using
Cu Ka radiation with an X-ray diffractometer (XRD,
PW1710). A scanning electron microscope (SEM) (JEOL
JSM-6360LA) operating at 20 kV was used to investigate the
morphology of the films. Device performance was measured
using a current-voltage (I-V) meter (Keithley 617). Measurements were obtained in the dark and under xenon lamp illumination. Light intensity was measured using a luxmeter
(Lutron LX-101). Electrical conductivity measurements
were obtained by electrochemical impedance spectroscopy

FIG. 3. (a) SEM image of a bare TiO2 film on an ITO substrate, and (b) I-V
characteristics of a solar cell made from this film when illuminated at different intensities: 4.39 mW/cm2 (bottom) and 37.48 W/cm2 (top).

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123109-3

Saehana et al.

at frequencies from 20 Hz2 MHz (Agilent E4980A Precision LCR meter).

III. RESULTS AND DISCUSSION
A. Solar cells from bare TiO2

An SEM image of a bare TiO2 film made by the spray

method on an ITO substrate is shown in Fig. 3(a). The thickness of the film was about 5 lm and it contained pores with
diameters of 50300 nm. Good interconnection was observed
between TiO2 particles and between TiO2 particles and the
ITO surface. Such interconnection facilitates electron transport from TiO2 to the ITO electrode.
The I-V characteristics of a solar cell made from the bare
TiO2 film are shown in Fig. 3(b). A mixture of poly(ethylene
glycol) and sodium fluoride (PEGNaF) was used as an electrolyte. Measurements were performed at two different
illumination intensities: 4.39 and 37.48 mW/cm2. The lower
intensity replicates dark conditions. Conversion efficiencies
(g) were very low under both conditions: 0.05% in the dark
and 0.04% under high illumination. The efficiencies reported
in this work are the apparent efficiencies obtained by directly
comparing the incident photon energies and electricity produced. Other mechanisms such as scattering of light by TiO2

FIG. 4. I-V curves of solar cells containing PVALiOH (red) and PEGNaF
(blue) electrolytes at intensities of (a) 4.39 mW/cm2 and (b) 37.48 mW/cm2.

J. Appl. Phys. 111, 123109 (2012)

particles that might occur in this type of solar cell were not
measured.29 The low efficiencies of this device were caused
by rapid recombination of the produced electron and hole
pairs because of the absence of a mechanism to separate
them.15,21 In addition, the high resistance of ITO (100 X/cm2)
also reduced the fill factor (FF), as described by Joshi et al.8
The effect of the type of electrolyte on g was also determined. Some authors reported that the performance of TiO2based solar cells does not only depend on metal contact but
also on the ionic conductivity of the electrolyte.1,9,30 We
tested two types of polymer electrolytes, PEGNaF and
PVALiOH. These electrolytes possess different ion carrier
masses, which affects their conductivity. The electrical
conductivities at room temperature for PVALiOH and
PEGNaF were 0.16 and 0.0014 S/cm, respectively. The electrolytes used here were gel-like polymer electrolytes rather
than solids, which is why their electrical conductivity was
higher than that of solid polymer electrolytes.
The I-V curves of the TiO2-based solar cells at intensities of 4.39 mW/cm2 and 37.48 mW/cm2 are shown in Fig. 4.
The solar cells containing PVALiOH electrolyte showed
higher g than the cell containing PEGNaF electrolyte at both
illumination intensities.
The FF of the solar cell containing PEGNaF was
slightly lower than that of the solar cell containing PVALiOH,
possibly because of the lower ionic conductivity of PEGNaF.

FIG. 5. SEM images of TIO2 films containing (a) Cu and (b) Fe bridges.

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123109-4

Saehana et al.

Wang et al. reported that Li ions create new trapping states

that contribute to electron injection into the TiO2 conduction
band.30 Increasing the electrolyte conductivity might increase
the short-circuit current. However, we did not optimize the
conductivity in this study.

B. TiO2 solar cells with metal bridges

From the above results, it was concluded that it is very

difficult to obtain high g using bare TiO2 films. In an attempt
to improve g, metal bridges were inserted in the spaces
between TiO2 particles. The insertion of metal bridges was
expected to improve the separation of electrons and holes.
Photogenerated electrons should flow quickly to the metal
bridge, which prevents recombination with a hole.
Two kinds of metal, Fe and Cu, were tested as bridges.
SEM images of TiO2 films containing Cu and Fe bridges are
presented in Fig. 5. The morphologies of Fe and Cu were very
different. Cu formed pyramidal particles with a size of around
0.5 lm, while Fe formed fiber-like structures. The presence of
two different shapes was also demonstrated by direct electroplating of Cu and Fe on ITO substrates for 15 min. After electroplating, one ITO surface was fully covered with pyramidal

FIG. 6. Morphologies of (a) Cu and (b) Fe particles deposited on the surface

of ITO electrodes.

J. Appl. Phys. 111, 123109 (2012)

Cu particles and the other was fully covered with Fe fibers, as

shown in Fig. 6.
I-V characteristics of TiO2 solar cells containing Cu and
Fe bridges are shown in Fig. 7. Measurements were performed both at low and high illumination intensities. Compared with the solar cell containing TiO2 alone, the presence
of Fe bridges improved g. However, a substantial increase of
g by more than one order of magnitude was observed for the
solar cell containing Cu bridges because of the different electron affinities of Cu and Fe. Although the work functions of
these two metals are similar (4.65 and 4.67 eV for Cu and
Fe, respectively), the electron affinity of Cu (119.24 kJ/mol)
is significantly larger than that of Fe (15.70 kJ/mol).
The efficiency of TiO2-based solar cells depends not
only on metal particles with a capacity for collecting electrons (electron affinity), but also on the ability of electrons to
migrate from the interior to the surface of a metal (the work
function).3033 Higher electron affinity indicates a stronger
ability to accept electrons from a semiconductor, while a
lower work function indicates that electrons can migrate
more easily from the interior to the surface. Therefore, it is
intuitive that Cu produces a solar cell with higher g that that

FIG. 7. Comparison of the I-V performance of solar cells containing (a) Cu

and (b) Fe bridges.

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123109-5

Saehana et al.

containing Fe because Cu possesses both a higher electron

affinity and slightly lower work function than Fe. In addition,
the charge transfer resistance was much lower in the solar
cell containing Cu bridges rather than that containing Fe
bridges.
C. Effect of internal resistance

An efficiency of less than 1% is insufficient to be economically viable, so the search to improve the efficiency of
these solar cells was continued. The internal resistance of solar cells affects the charge transport at interfaces and ion diffusion in the electrolyte. According to Han et al.,3436 an
increase in the efficiency of solar cells will be obtained by
reducing the internal resistance. The sheet resistance of the
ITO glass substrate is one of factor that influences the internal
resistance of solar cells, so the efficiency of the solar cells
should increasing as the resistance of the ITO substrate is
decreased. To determine the effect of the resistance of ITO on
the performance of solar cells, the performances of devices
containing ITO with specific resistances of 10 and 100 X/cm2
were compared.

FIG. 8. IV curves of TiO2-based solar cells with ITO resistances of 10 and

100 X/cm2 under light intensities of 4.39 and 37.48 mW/cm2.

J. Appl. Phys. 111, 123109 (2012)

I-V characteristics of solar cells containing ITO with different specific resistances of 10 and 100 X/cm2 are shown in
Fig. 8. Both cells contained Cu bridges and PVALiOH electrolyte. Measurements were performed at both low and high
illumination (4.39 and 37.48 mW/cm2, respectively). It is
clear that the resistance of ITO played a significant role in
the efficiency of these solar cells. Under low illumination,
the efficiency of the solar cell containing ITO with a sheet
resistance of 10 X/cm2 was five times that containing ITO
with a sheet resistance of 100 X/cm2. Under high illumination, the efficiency of the solar cell containing ITO with a
sheet resistance of 10 X/cm2 was 4.16%, which was more
than ten times higher than that containing ITO with a sheet
resistance of 100 X/cm2. It was concluded that the use of
ITO with a low sheet resistance reduces internal resistance
and improves the performance of solar cells.
The presence of metal on the TiO2 films was confirmed
using XRD and energy-dispersive x-ray (EDX) measurements. XRD patterns of a TiO2 film and TiO2 films containing Cu bridges deposited using different bath temperatures
(25, 55, and 95  C) and electroplating currents (50, 150, and
300 mA) are shown in Fig. 9. The primary peaks of TiO2 in
the anatase phase appeared at 25 , 38 , 49 , and 83 . Cu diffraction peaks were also observed at 2h 43.34 and 52 .
Inspection of SEM images of the TiO2 films containing
Cu bridges revealed that the average size of Cu crystals
depends on the bath temperature. The average crystal size

FIG. 9. XRD patterns of (a) a bare TiO2 film, and TiO2 films electroplated
using various bath temperatures (b: 25, c: 55, and d: 95  C) and currents
(e: 50, f: 150, and g: 300 mA).

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123109-6

Saehana et al.

FIG. 10. Relationship between Cu grain size and bath temperature.

was determined from the XRD peaks using the Scherrer

approximation.37 A plot of crystal size as a function of bath
temperature is shown in Fig. 10. The crystal size initially
decreased with increasing bath temperature, and then
increased at higher temperature. A minimum size of 67 nm
was observed at 55  C. The results obtained for bath temperatures above 55  C are in agreement with those of Rashidi
and Amadeh.38
The trend of crystal size with temperature did not reflect
the amount of Cu deposited on the TiO2 film. EDX measurements showed that the amount of Cu deposited on the TiO2
film increased with bath temperature: 13.12 wt. % at 25  C,
33.49 wt. % at 55  C, and 42.03 wt. % at 95  C.
In addition, we identified from the SEM images that a
low bath temperature (25  C) resulted in particles with a
globular morphology, while bath temperatures of 55 and
95  C resulted predominantly pyramidal morphology. The
Cu particles formed at a bath temperature of 55  C were
smaller pyramids than those grown at 95  C. It was assumed

FIG. 11. Relationship between Cu crystal size and electroplating current.

J. Appl. Phys. 111, 123109 (2012)

that a pyramidal morphology leads to better cell efficiency

than a globular morphology because it contains sharp edges
that can produce a large electric field to attract electrons
from TiO2 more strongly.
The effect of electroplating current on the crystal size of
Cu is shown in Fig. 11. In contrast to the effect of bath temperature, the crystal size initially increased with current and then
decreased at higher current. The largest crystal size, about
59 nm, was observed using a deposition current of 150 mA.
This result originated from competition between the nucleation rate, which tends to increase crystal size, and the number
of growth sites, which tends to reduce the crystal size as the
current is increased. EDX analysis indicated that the Cu
contents of the films were 14.17, 36.34, and 34.43 wt. % for
applied currents of 50, 150, and 300 mA, respectively.
As mentioned above, deposition temperatures of 55 and
95  C produced pyramidal Cu particles, as did a deposition
current of 50 mA. Because of their sharp edges, this shape
will produce a high electric field. By approximating this
shape as a cone, the electric field (E) around the tip can be
expressed as,39

FIG. 12. Photocurrent and voltage characteristics of cells electroplated at (a)

different temperatures (25, 55, and 95  C), and (b) different currents (50, 150,
and 300 mA). The illumination intensity was maintained at 37.48 mW/cm2.

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123109-7

Saehana et al.



r r
H
1  p ;
E ln
e0 R
R2 H 2

J. Appl. Phys. 111, 123109 (2012)

3

(1)

where r is the cone radius at a specific position, R is the radius of the cone base, H is the cone height, r is the charge
density, and e is the electrical permittivity. It is clear that
near the sharp edge, r ! 0, so E becomes very large. This
large E will strongly attract electrons photoinduced in TiO2,
allowing them to be quickly separated from holes so that the
efficiency of solar cells containing pyramidal bridging Cu
particles is improved.
The I-V characteristics of solar cells fabricated by
depositing Cu using different bath temperatures and currents
are shown in Fig. 12. For different bath temperatures, the
highest efficiency of 3.88% was obtained for the cell fabricated at a bath temperature of 55  C (small pyramidal crystals). For different bath currents, the highest efficiency of
4.38% was recorded for the cell produced under an electroplating current of 50 mA (pyramidal). These results confirm
the hypothesis that pyramidal Cu crystals with sharp edges
improve device efficiency because they facilitate electron
capture from the TiO2 particles.
The efficiencies of the solar cells achieved here are
greater than those reported in our previous studies of around
3.73%.2527 Under intense irradiation, efficiencies ranged
from 3.74% to 4.11%, while under lower intensity illumination, efficiencies were between 1.39 and 2.70%. The
improved performance of the devices produced in this study
was because of decreased electron-hole recombination and
their low internal resistance.3436
IV. CONCLUSION

TiO2-based solar cells with a power conversion efficiency of 4.38% were fabricated by spray deposition of TiO2
and electroplating Cu bridges in the spaces between TiO2
nanoparticles. The semiconductor-metal contacts provided a
significant photovoltaic response, and show potential for use
as electron traps in solar cells to minimize electron-hole
recombination. Such structures may reduce the cost and
allow environmentally friendly processing of TiO2-based solar cells, which might revolutionize the field of photovoltaics. Further improvement may be achieved by replacing
copper with a noble metal such as gold.
ACKNOWLEDGMENTS

This work was supported by research grants from Asahi

Glass Foundation 2010, Hibah Strategis Nasional DIPA-ITB
(Bandung Institute of Technology) 2010, and Hibah Doktor
2010.
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