Results in Physics 7 (2017) 2271–2276

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Results in Physics
journal homepage: www.journals.elsevier.com/results-in-physics

Fabrication and characterization of TiO2/SiO2 based Bragg reflectors

for light trapping applications
R.S. Dubey a,⇑, V. Ganesan b
a
Advanced Research Laboratory for Nanomaterials and Devices, Department of Nanotechnology, Swarnandhra College of Engineering and Technology,
Seetharampuram, Narsapur, A.P., India
b
UGC-DAE Consortium for Scientific Research, Indore Centre, University Campus, Khandwa Road, Indore, M.P., India

a r t i c l e i n f o a b s t r a c t

Article history: Distributed Bragg reflectors (DBRs) have received an intensive attention due to their increasing demand
Received 11 March 2017 in optoelectronic and photonic devices. Such reflectors are capable to prohibit the light propagation
Received in revised form 22 June 2017 within the specified wavelength range of interest. In this paper, we present the fabrication of TiO2/SiO2
Accepted 25 June 2017
stacks based Bragg reflectors by using a simple and in-expensive sol-gel spin coating technique. The pre-
Available online 30 June 2017
pared single-layer thin films of TiO2 and SiO2 onto glass substrates were characterized for their optical
constants. By tuning the process parameters, one-seven DBR stacks of TiO2/SiO2 were prepared. The cor-
Keywords:
responding shift of the Bragg reflection peak was observed with the increased number of DBR stacks and
Bragg reflector
Photonic bandgap
as much as about 90% reflectance is observed from the 7DBR stacks. The experimentally measured reflec-
Sol-gel coating tance was compared with the simulated one, which showed good in agreement. FESEM measurement has
Reflection confirmed the formation of bright and dark strips of TiO2 and SiO2 films with their thicknesses 80 and
Absorption 115 nm respectively. The simulation study was explored to a design of thin film silicon solar cell using
7DBR stacks. An enhancement in light absorption in the visible wavelength range is observed which coin-
cides with the experimental result of the reflectance. The use of DBR at the bottom of the solar cell could
felicitate the better light harvesting with the occurrence of Fabry-Perot resonances in the absorbing layer.
Ó 2017 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Introduction and cost-effective process. Several literatures have also been

Presently, multilayer thin film structures have demand in
advanced electronic, optoelectronic and photonic devices due to
their unique properties and cost-effective fabrication process by
the sol-gel method. The periodically arranged thin films of two dis-
tinct materials have the capability to deal the light waves in a dif-
ferent manner. Such multilayer thin films structures with quarter
wavelength thickness of their individual layers generate a high
reflection band in which propagation of light is prohibited. These
dielectric multilayer structures are recognized as distributed Bragg
reflectors (DBR) or one-dimensional photonic crystals (1PCs)
which work on the concept of standing wave phenomena due to
the occurrence of constructive interference of the incident and
reflected light waves. This mechanism of light manipulation has
been adopted in advanced solar cells, waveguides, vertical cavity
surface emitting diodes etc. [1–3].
Among others, the sol-gel technique is one of the demanded one
due to its simplicity, easy tuning with the deposition parameters
⇑ Corresponding author.
E-mail address: rag_pcw@yahoo.co.in (R.S. Dubey).
reported on the preparation of multilayer thin film structures of
TiO2/SiO2, a-Si/SiO2, c-Si/SiO2, ITO/a:Si:H, SiO2/Si3N4, porous silicon
layers etc. However, TiO2 and SiO2 are the most chosen materials
due to their large refractive index contrast and easy fabrication
process using combined sol-gel and spin coating method. Han
et al. have studied the properties of multilayer thin films of TiO2/
SiO2 using a cost effective sol-gel process. This investigation was
focused on the elimination of cracks/delamination originated from
the non-wettability of the solution during the deposition on
hydrophobic SiO2 film. The residual alkoxy groups onto the layer
after heat treatment was the usual cause of hydrophobic surface
therefore, the proposed heat treatment idea was found to be effec-
tive for the removal of residual alkoxy groups. Using this tech-
nique, a fine structure of TiO2/SiO2 stacks were fabricated [4].
They have also explored an energy efficient transparent window
application with the tuning of reflection band [5]. Barhoum et al.
have studied the one-dimensional photonic bandgap materials of
TiO2/SiO2 fabricated by a sol-gel and dip-coating process on planar
and curved substrates. To prevent the cracks on the film, a shock-
cooling heat-treatment was employed. The fabricated Bragg reflec-
tor of seven stacks showed the stop band centered at about 568 nm

http://dx.doi.org/10.1016/j.rinp.2017.06.041
2211-3797/Ó 2017 The Authors. Published by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
2272 R.S. Dubey, V. Ganesan / Results in Physics 7 (2017) 2271–2276

[6]. Today, there is a demand of a special type of fabric in textile styrene sacrificial layer was employed that could also helpful to
field that gives light reflections as the indication of sign. Liu et al. avoid the penetration of the TiO2 solution in-between the nanopar-
have investigated the optical properties of TiO2/SiO2 stacks pre- ticles interstitial voids. The prepared reflectors were explored for
pared on the fabric by employing the sol-gel method. The prepared the gas sensing application and showed as much as 90% reflectance
multilayer structure was exposed to the sun for the testing and the using seven TiO2/SiO2 stacks [14].
fabric color was remained unchanged (due to light resistance) with In this work, we present the fabrication of TiO2/SiO2 stacks
the increased number of layers [7]. Chen et al. have reported the based distributed Bragg reflectors using sol-gel spin coating
fabrication of omnidirectional reflector and microcavity resonator method and characterization for their optical properties. We have
using sol-gel technique. Omnidirectional reflectors prohibit the compared the experimental results with the simulated one and
light propagation within the forbidden band gap regardless the found good in agreement. A design of thin film silicon solar cell
incident angle. A reflector of six bilayers of SiO2 and TiO2 showed using 7DBR stacks as the back reflector is also explored and dis-
an omnidirectional bandwidth of 70 nm in the infrared wavelength cussed. Section 2 describes the experimental approach used for
range at incident angle range from 0° to 80°. A microcavity res- the fabrication of TiO2/SiO2 stacks. The obtained results have been
onator with a TiO2 Fabry–Perot cavity sandwiched in-between discussed in Section 3. Finally, Section 4 presents the summary of
two reflectors of three bilayers was fabricated and showed the res- the paper.
onance at 1500 nm with quality factor value 35 [8]. Hinczewski
et al. have explored the sol-gel spin coating process for the prepa-
Experimental approach
ration of Bragg reflectors that was comprised of SiO2 and TiO2 lay-
ers on both the sides of glass substrates. Under optimized
For the fabrication of TiO2/SiO2 based DBR a combined sol-gel
condition, they have explored the fabrication of three-layer based
and spin coating processes were performed. Tetraethyl orthosili-
film structure as anti-reflective filters for near-infrared region
cate (TEOS) and titanium butoxide (TBOT) were used as the precur-
and a nine-layer based film structure as reflective filter for the
sor of silicon and titanium respectively whereas ethyl alcohol and
near-UV region. The reflective filters were characterized to study
acetic acid were preferred as the solvent and the chelating agent
the optical behavior for both transverse electric and magnetic
respectively. All the reagents were of analytical grade and used
polarizations. The fabricated multilayer film structure could act
without any further purification. The precursor solution of TiO2
as near-UV reflective filter and showed maximum reflection in
was prepared by using TBOT, acetic acid, and ethyl alcohol in the
the wavelength range from 350 to 370 nm with its center wave-
molar ratio 0.35:4:40 whereas for the SiO2 solution, the molar ratio
length at 365 nm for the case of transverse electric mode [9].
0.5:4:40 corresponding to TEOS, acetic acid and ethyl alcohol were
Yasuda et al. have proposed a novel technique to fabricate TiO2/
taken, respectively. Initially, ethyl alcohol was taken in a beaker
SiO2 stacks by using flakes for the visible light application in dye-
and mixed with the acetic acid for 10–15 min under constant stir-
sensitized solar cells without the need of substrate. The prepared
ring using magnetic stirrer. The precursor (TiO2 or SiO2) was slowly
optical interference flakes were composed of five stacks of TiO2/
added drop by drop to the above-prepared solution under vigorous
SiO2 and showed better confinement of light in the dye-
stirring condition. Further, the stirring was maintained for a few
sensitized solar cells via light scattering. Further, they have sug-
hours to get the transparent solution. The prepared solution of
gested for its application in tandem solar cells [10]. The problem
TiO2 was transparent with little yellowish in color whereas SiO2
of stress arising with the annealing of films during multilayer
solution was homogeneous and transparent. Both the solutions
deposition is a major drawback of sol-gel process which causes
were stable without any precipitation. Prior to deposition, the as-
cracks in the films. However, by giving proper heat treatment to
prepared solutions of TiO2 and SiO2 were aged for 3 and 4 h respec-
the TiO2 films, this stress could be reduced. Rabaste et al. have
tively. For the deposition of films, spin coating technique was used.
employed the sol-gel method for the preparation of TiO2/SiO2 dis-
Before the deposition process, the glass substrates were cleaned
tributed Bragg reflectors and microcavities. With proposed heating
with the soap solution and ultra-sonicated with ethanol followed
process, the seven stacks of TiO2/SiO2 Bragg reflector showed max-
by the deionized water to remove the surface impurities. The
imum reflection in the wavelength range 580–780 nm. Further, a
washed glass substrates were dried in the hot air oven at 100 °C
microcavity was fabricated by introducing the Er-doped SiO2 layer
for 15 min to avoid the weeding on the glass surface. Followed
in between the seven stacks of distributed Bragg reflector at the
by the above process, DBR stacks of high/low (TiO2/SiO2) films
top and bottom respectively. The reflectance spectra could reveal
were fabricated by dropping the precursor solution (TiO2/SiO2)
a sharp peak at around 650 nm corresponding to the microcavity
onto the glass substrates while the spin rate was maintained at
resonance peak [11]. Fuertes et al. have demonstrated the fabrica-
3000 RPM for the time 30 s. Several samples were prepared by
tion of ordered mesoporous thin films stacks of TiO2/SiO2 using
varying number of DBR stacks and characterized for the measure-
chemical dip-coating process. By controlling the film composition,
ments of thickness and refractive index using Filmetrics (F20, USA),
thickness and disposition in the space, the tuning of the Bragg
reflectance using UV–vis spectrophotometer with a specular reflec-
mirrors were discussed. They have explored the tuning of Bragg
tance attachment (UV1800 Shimadzu, Japan) and surface morphol-
reflectors using the selective introduction of functional groups
ogy by field emission scanning electron microscopy (ZIESS,
in one-type of the building blocks of these structures [12].
Germany).
Colodrero et al. have discussed the hydrothermal fabrication of
nanoparticles-based 1D photonic crystal of two distinct refractive
index materials with the controlled porosity of an individual layer. Results and discussion
Due to the created defect states, high transmission windows were
noticed in the photonic band gap region. Further, the applicability To estimate the refractive indices and thicknesses of TiO2 and
of this material was demonstrated for the sensing with the expo- SiO2 films, each single-layer was prepared and characterized. The
sure of solvents and showed variations in its optical behavior obtained refractive index values are found to be 2.2 and 1.4 with
[13]. Anaya et al. have demonstrated a high refractive index con- thicknesses 80 and 115 nm corresponding to the TiO2 and SiO2
trast distributed Bragg reflectors (DBRs) which needs less number films respectively. To observe the behavior of the incident light
of stacks to a targeted spectral range. The approach was to prepare onto the prepared DBRs, the reflectance measurements were done
a porous films of SiO2 nanoparticles and TiO2 films processed by using UV–vis spectrophotometer attached with a specular reflec-
sol-gel technique. To preserve the porosity of the SiO2 film, a poly- tance accessory. The modulated deposition of n-number of TiO2/
 R.S. Dubey, V. Ganesan / Results in Physics 7 (2017) 2271–2276
SiO2 stacks pairs was performed in one-dimension of the space.
With an increment of the number of DBR stacks, the reflectance
is found to be increased with the shift towards higher wavelength
range as depicted in Fig. 1.
The emergence of the strong interference of light can be
observed in the optical images of the three-, five- and seven-DBR
stacks as shown in the inset of Fig. 1. This interference effect is
found to be dominant in the visible-region as can be seen with
bright color onto the samples by the naked eye. The brightness
of the samples is in accordance with the increased number of
TiO2/SiO2 stacks.
The obtained parametrical values of the individual TiO2 and
SiO2 films were used for the simulation using rigorous coupled-
wave analysis (RCWA) method that is employed to analyze the
optical behavior of the light through the layered media. RCWA is
a computational method, which deals with the scattering of elec-
tromagnetic waves through a periodic dielectric film structures.
Typically, this approach is based on the Floquet’s theorem meaning
that the solutions of periodic differential equations is expanded
with the Floquet functions. For the calculation, the proposed device
is needed to be discretized uniformly into layers along a direction
and the staircase approximation is considered for the curved
Fig. 1. Reflectance spectra of one-, three-, five- and seven-DBR stacks with their
optical images.
Fig. 2. Optical behavior of light through one-, three-, five- and seven-DBR stacks using RCWA method.
2273
devices with their properties. With this, electromagnetic waves
propagating through each layer are analytically calculated. Using
scattering matrices, the matching boundary conditions are applied
at each interface between the layers. RCWA has been demanded for
the reflectometry measurement in semiconductor industry which
helps to get the profile of trench structures. In thin film solar cell
design, RCWA is used to optimize the diffractive structures in order
to achieve the optimal performance of the solar cell. Here, we have
performed the two-dimensional simulations using rigorously cou-
pled wave analysis. Fig. 2 depicts the electric field distribution
within the one-, three-, five- and seven-DBR stacks. The black lines
shown here in Fig. 2(a)–(d) symbolizes the interface of the films.
As shown in Fig. 2(a), the maximum portion of the incident light
is observed to be passed out in the air region (bottom) due to an
inefficient reflector, which is composed of only one-DBR stack
and yields minimal reflectance about 0.3%. A distinct effect of light
propagation can be observed in Fig. 2(b) that the partial light is
reflected back and transmitted through the three-DBR stacks with
its reflectance about 53%. In a similar way, the reflection and trans-
mission of light is observable from the five-DBR stacks as depicts in
Fig. 2(c) however, the propagation of light towards the bottom is
reduced with the enhancement in reflectance up to 81%. The prop-
agation of light is more affected for the case of seven-DBR stacks as
depicted in Fig. 2(d) which shows 90% reflectance.
With the above interesting electric field analysis, we have
extended the simulation work to obtain the photonic band gap of
the 7DBR stacks for the matching with the experimental result.
For this simulation, plane wave method was employed which is
demanded for the photonic band gap analysis of metamaterials.
Fig. 3(a) shows the refractive index profile of the Bragg reflector/
one-dimensional photonic crystal, which is composed of seven-
stacks of TiO2 and SiO2 layers in a periodic manner. The photonic
band structure of the Bragg reflector is depicted in Fig. 3(b) and
it is noted that the experimentally obtained optical values were
used in this simulation at center wavelength 617 nm correspond-
ing to the highest Bragg reflection peak.
The photonic band diagram shows the forbidden gap in the fre-
quency range from 0.27 to 0.34 (in the units of xa/2pc) or wave-
length from 573 to 722 nm which represents the maximum
reflectance for the perpendicular polarization (TE) case. Similarly,
photonic band gap for the parallel polarization (TM) is also
observed but with a reduced width due to a limitation of Brewster
angle. The shaded region in red color represents the omnidirec-
tional reflection band from 629-573 nm, which indicates the
2274 R.S. Dubey, V. Ganesan / Results in Physics 7 (2017) 2271–2276

maximum reflection band within the region regardless the angle of
incidence. We have compared the experimental reflectance of the
prepared seven-stacks based Bragg reflector and observed that
the reflection peak falls within the photonic band gap.
The experimental and simulated reflectance spectra are plotted
in Fig. 4(a). One can observe the maximum reflectance 90% from
the 7DBR stacks at wavelength 617, which falls within the reflec-
tion band of the simulated result. However, a slight deviation can
also be observed between the reflection bands that might be
related to the disturbed interfaces of TiO2/SiO2 as can be seen in
the cross-section FESEM image of 7DBR stacks in the inset of
Fig. 4(a). The resolution of the interfaces is not so clear which
might be associated with the improper cutting of the sample dur-
ing the FESEM measurement. The combination of high and low
refractive index layers exhibit intense Bragg reflection peak cen-
tered at wavelength 617 nm. The fabricated films of TiO2 and
SiO2 can be identified with their bright and dark strips in the
FESEM image, which represents the high and low density of the
elections. The formation of periodic layers of TiO2 and SiO2 is visi-
ble along the normal direction of the glass substrate. The estimated
thicknesses of TiO2 and SiO2 films were found to be 80 and 115 nm
with a deviation of 10–12 nm as compared to the result obtained
by the filmetric measurement.
Bragg reflectors have their potential applications in optoelec-
tronics, photonics, sensors etc. and presently demanded in thin
film silicon and dye-sensitized solar cells. Thin film silicon solar
cells are having the weak absorption of sunlight due to its thin
active-layer region. This optical loss can be prevented by using
advanced optical engineering so that optimal light harvesting can
be attained. To achieve this, Bragg reflectors are the promising
one that has the capability to fold the light back towards the absor-
ber layer via Bragg reflections. In simple words, light absorption

Fig. 3. Refractive index profile (a) and photonic band structure (b) of 7DBR based Bragg reflector using plane wave method.

Fig. 4. Reflectance spectra with inset FESEM image (a) and light absorption spectra (b) with inset schematic diagrams of the proposed solar cells SC1 and SC2.
 R.S. Dubey, V. Ganesan / Results in Physics 7 (2017) 2271–2276 2275

Fig. 5. Electric field distribution in the reference cell (a) and DBR based solar cell (b) with their and quantum efficiency (c).

can be enhanced in the thin film silicon solar cells with the use of region in which reflectance was observed to be dominant as seen
Bragg reflectors/one-dimensional photonic crystals that reprocess in Fig. 4(a). In this way, the desired wavelength range of the Bragg
the unabsorbed light coming from the active layer and enforces reflection or photonic band gap can be tailored to achieve the cor-
back to the same region. By doing so, the mean residing time of responding improvement in the photovoltaic performance.
the photons within the active region gets prolonged which is useful
for the prevention of recombination of charge carriers. With this
Conclusions
concept, we have designed two types of solar cells: SC1 as refer-
ence solar cell without a DBR/back reflector and SC2 with a DBR/
In this work, we have presented the fabrication and characteri-
back reflector. The schematic diagrams of SC1 and SC2 are shown
zation of TiO2/SiO2 stacks based Bragg reflectors using a simple and
in the inset of Fig. 4(b). The designed solar cells consist of a
cost-effective sol-gel spin coating method. The prepared films of
70 nm thick Si3N4 film as anti-reflection coating layer, 200 nm
TiO2 and SiO2 showed refractive indices 2.2 and 1.2 respectively.
amorphous-silicon (a-Si) layer as active region and a DBR of seven
As a result of constructive interference caused by the incident
TiO2/SiO2 stacks as a back reflector with their thicknesses
and reflected light waves, a bright color is observed onto the pre-
80/115 nm in the case of SC2. The light absorption from both the
pared DBR samples in accordance with the increased number of
solar cells is plotted in Fig. 4(b). The reference solar cell without
TiO2/SiO2 stacks. The seven-DBR stacks showed the maximum
DBR shows less light absorption as compared to the solar cells
reflectance 90% at wavelength 617 nm and this result is found good
based on three-, five- and seven-DBR pairs. In addition, one can
in agreement with the simulated results of the photonic band gap
observe the enhancement in the light absorption beyond 560 nm
and reflectance. By FESEM measurement, the formation of alter-
range in the visible wavelength range. This result coincides with
nate layers of TiO2 and SiO2 as bright and dark strips with their
the experimental reflectance shown in Fig. 3(a). Interestingly, the
periodicity in one-direction and thicknesses 80 and 115 nm
obtained Bragg reflection peak at wavelength 617 nm reveals the
respectively is observed. Further, we have explored a design of thin
corresponding absorption enhancement in Fig. 4(b) through the
film silicon solar cell by using seven-stacks of DBR as back reflector
7DBR stacks based solar cell (SC2).
and an enhancement in light absorption is noticed in the visible
Finally, we have compared the electric field profiles of reference
spectrum, which agrees with our experimental reflectance result.
(SC1) and DBR based (SC2) solar cells, which is plotted in Fig. 5
(a) and (b). The electric field distribution shown in Fig. 5(a) repre-
sents the partial absorption and transmission of light through the Acknowledgements
active region of SC1 as shown in the dotted red box. The intensity
of the light can be evaluated with the help of color bar, which is The authors gratefully acknowledge financial support from the
depicted beside the Fig. 5(b). Here, transmitted portion of the light UGC-DAE Consortium for Scientific Research, Indore, (M. P.), India.
is the loss, which generally occurs in thin film silicon solar cell. We thank Prof. K. Ramaji, Center for Nanotechnology for the access
A distinct behavior of light propagation is observed in Fig. 5(b) of characterization facilities. RSD express thanks to Mr. Ajay Kumar
for the SC2 where the use of Bragg reflector is dominating the for the partial help in experimental work.
transmission of light towards the bottom. One can see the typical
Fabry-Perot resonances (dashed box) within the active region, References
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