Journal of Materials Science: Materials in Electronics

https://doi.org/10.1007/s10854-020-04084-1

Synthesis and characterization of ­MAPbI3 thin film and its application

in C‑Si/perovskite tandem solar cell
Shaimma M. Jassim1 · Nabeel A. Bakr1 · Falah I. Mustafa2

Received: 14 December 2019 / Accepted: 23 July 2020

© Springer Science+Business Media, LLC, part of Springer Nature 2020

Abstract
Silicon, polymer and dye sensitized have been increasing rapidly in thin film of solar cells. Recently, perovskite is proposed
as alternative material in the fabrication of solar cells. In this study, methyl ammonium lead triiodide ­(MAPbI3, ­CH3NH3PbI3)
perovskite thin film was prepared by two-step process of spin coating. The preparation process of thin film is summarized
by reaction between the methyl ammonium iodide ­(CH3NH3I) and lead iodide ­(PbI2). The absorbent layer of the prepared
perovskite solar cell is based on the ­MAPbI3 ­(CH3NH3PbI3) thin film. The conversion efficiency of p-n silicon solar cells
can be improved by preparing tandem solar cells. The X-ray diffraction result of the ­MAPbI3 perovskite film manifested that
it is polycrystalline with tetragonal system having a crystallite size of about 40 nm. The absorption spectrum of perovskite
film was recorded by Ultra Violet–Visible spectrophotometer. The energy band gap of the ­MAPbI3 film calculated by Tauc’s
formula was ~ 1.51 eV. The field emission scanning electron microscope image of the M ­ APbI3 film surface elucidated a
cubic-like crystal structure and other irregular structures also. The atomic force microscope image and the distribution chart
of the grains of the film displayed that the grain size was ~ 58.7 nm. The results demonstrated that the conversion efficiency
for silicon, perovskite and tandem (silicon/perovskite) solar cells are 3%, 4.83% and 7.42%, respectively.

1 Introduction planar hetero-junction, PSCs are, in general, based upon

the structure of (fluorine-doped tin oxide (FTO)/hole trans-
Energy is one of the essential elements of modernization. port layer (HTL)/perovskite layer/electron transport layer
The increase in energy demands entails the depletion of (ELT)/metal electrode) have attracted significant attention
world fossil fuel resources. Moreover, the consumption because of the simple processing procedure, little hyster-
of fossil energy has a detrimental side effect, which is the esis and high efficiency device design [5, 6]. A transparent
global warming that is caused by the enormous level of electrode is necessary for the solar cells as it permits the
greenhouse gas emission. Therefore, scientific research- arriving light to attain the photoactive layer. The transpar-
ers have been focusing on developing a greener and more ent conductive oxides (TCO) like FTO is used well suited
sustainable energy to alleviate environmental impacts [1]. for this purpose due to its transparent and conductive nature
Perovskite solar cells (PSCs) based upon an organic–inor- [7]. Poly(3,4 ethylenedioxythiophene): polystyrene sulfonate
ganic lead halide light harvester have taken an attracted (PEDOT: PSS) organic material has been used to as HTL
increasing interest in the world owing to its benefits of the owing to high transparency and conductivity ­(10−4 to ­10−3 s/
high power conversion efficiency (PCE), low price as well as cm), high mechanical flexibility [8] and fabrication at low
easy fabrication techniques [2, 3]. According to the order of temperature [4, 5]. While, the inorganic methyl ammonium
preparation, the planar structure can be categorized into two lead triiodide perovskite material ­(MAPbI3) was used as
types: regular (n-i-p) and inverted (p-i-n) [4]. For inverted a light-harvesting layer in solar cells owing to the unique
optoelectronic characteristics, like (proper straight bandgap,
* Shaimma M. Jassim ambipolarity [9], high mobility of charge carrier, the high
[email protected] coefficient of absorption, a steep edge of absorption, the long
length of diffusion and the unique tolerance to the struc-
1
Department of Physics, College of Science, University tural defects) [2, 10], easy synthesis, and low cost [11]. On
of Diyala, Diyala, Iraq
the other hand, organic charge transport (­ PC71BM) material
2
Ministry of Science and Technology, Renewable Energy was used as ETL in perovskite solar cells owing to its high
Directorate, Baghdad, Iraq

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 Journal of Materials Science: Materials in Electronics

electron-accepting characteristics, role as trap passivation in properties of prepared perovskite film were studied. In addi-
the perovskite film, facile synthesis, good solubility, and low tion, the inverted perovskite solar cell was prepared by using
processing [12, 13]. Finally, the metal aluminum (Al) was ­MAPbI3 thin film as an active layer. Moreover, c-Si/ inverted
chosen as perfectly suitable for the contact electrode due to perovskite tandem solar cell was designed and fabricated to
the high conduction. improve the conversion efficiency of p-n silicon solar cells.
The films quality and functionality as well as the com-
plete device vigorously rely upon the deposition method and
treating circumstances [9]. Numerous methods of deposition 2 Experimental section
are utilized to the perovskite solar cells synthesis, compris-
ing vapor deposition, one-step or two-step solution-treated, 2.1 Materials
vapor deposition, and vapor-assisted solution methods. The
two-step spin coating deposition technique has well prop- The materials used in this work are as follows: Methyl-
erties, such as the effective chemical change and a better amine ­(CH3NH2, 33 wt% in absolute ethanol, BDH-LTD),
governing above the morphology and size of crystal [11]. Hydroiodic acid (HI, 57 wt% in water, BDH-LTD), Lead
PSCs devices have exhibited a fast and clear improvement iodide ­(PbI2, 99%, Sigma Aldrich). N,N-dimethylforma-
in the energy conversion efficiency from 3.8% in 2009 to mide (DMF) (99%, BDH-LTD), Poly(3,4 ethylenedioxy-
24.2% in 2019 [14], this is attributed to the excellent advan- thiophene): polystyrene sulfonate (PEDOT: PSS, Ossila)
tages of the perovskite material. The most straight forward [6,6],-Phenyl ­C71 butyric acid methyl ester ­(PC71BM, 95.5%,
method to attain the efficiencies after such a boundary at Ossila), tin (Sn, 99.99%, India), Chlorobenzene (CB, 99.9%,
a realistic price is the combination of a silicon cell hav- BDH-LTD), Fluorine-doped tin oxide (FTO) glass substrate
ing a low-price cell with a broad-bandgap absorber mate- with a sheet resistance (8 Ω s­ q−1, TEC-8, Ossila), Diethyl
rial for forming tandem solar cells (TSCs) [15]. TSCs have ether (99%, BDH-LTD), Aluminum (Al) wire (99.9%), and
been suggested to accomplish higher change efficiency than p-n silicon wafer (5 Ω/cm2, 500 µm, from Al-Mansour com-
the single-junction solar cells. The TSCs comprises high pany, Iraq).
and low bandgap solar cells [16]. An encouraging nominee
for this a broad-bandgap top cell with the potential for low 2.2 Synthesis of methylammonium iodide (MAI)
production prices being the organic–inorganic metal halide
perovskite solar cell [15]. The advantage of TSCs is that The methylammonium iodide (MAI) was synthesized using
via the combination of solar cells appropriate for short and 24 ml of methylamine (MA) solution and 10 ml of hydroi-
long wavelength zones, every zone of wavelength can be odic acid (HI) solution. The two solutions were mixed into a
capably changed to an electric power, and a high output can round bottom flask stirred at 0 °C for 120 min in an ice bath
be reached. The bottom and top cells absorb the long and under continuous stirring to obtain a white solution. Then,
short wavelength spectra, correspondingly [17]. The highest the resultant solution was evaporated at 80 °C for 120 min
efficiency of energy change can be attained when the top cell to give white precipitate. The precipitate then was washed
bandgap equals to (1.7 eV), whereas the bottom solar cell by diethyl ether several times until it became colorless, and
bandgap equals to (1.1 eV). Therefore, the crystalline silicon a white crystalline powder was formed. The solution then
with a (1.1 eV) bandgap appears the optimum selection for was filtered and desiccated in a vacuum oven at (60 °C) for
the bottom solar cell [18]. Methyl ammonium lead triiodide (24 h).
­(MAPbI3 perovskite and crystal-silicon (c-Si are fabricated
in chiefly (2 configurations; as monolithic two-terminal 2.3 Fabrication of device
tandem (2-T, and mechanically stacked four-terminal (4-T
tandem [19]. Furthermore, the solar cells are able to make The perovskite device structure is shown in Fig. 1a. FTO
a balancing pair with the big-bandgap perovskite solar cell glass substrates were cleaned in an ultrasonic bath with de-
that functions as a top cell in charge to harvest the short ionized water, acetone and ethanol sequentially for 15 min.
wavelength photons, whereas the bottom (c-Si) solar cell is PEDOT: PSS layer was then spin coated (L2001A3, Ossila)
intended for absorbing the long-wavelength photons [20]. upon the upper FTO substrate at (1000 rpm) for (20 s), pur-
Tandem solar cells, which are encouraging outcomes, have sued via the annealing on hotplate at (120 °C) for (10 min).
been done for two-terminal tandem (2-T) and four-perovs- To prepare perovskite thin film, a two-step method was used.
kite/silicon tandem solar cells reaching the efficiencies of In the first step, ­PbI2 solution (0.4 g in 2 ml of DMF) was
(23.6%) and (26.4%), respectively [21]. then spin coated on the PEDOT: PSS film at (1000 rpm) for
In the present work, the perovskite ­MAPbI3 film was syn- (10 s), pursued via the annealing at (100 °C) for (10 min).
thesized by the use of a two-step spin coating method, in While in second step, MAI solution (0.01 g in 2 ml of DMF)
which the MAI solution was spin coated on ­PbI2 film. The was deposited on P ­ bI2 film by spin coating at (500 rpm for

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Journal of Materials Science: Materials in Electronics

Fig. 1  Device structure of the

­MAPbI3 based on: a Perovskite
solar cell, b Schematic diagram
of the mask, and c Tandem (Si/
Ps) solar cell

5 s, 1000 rpm for 10 s) and then annealed at (100 °C) for and Al electrodes were connected electrically to Keithley
(10 min). The color of the perovskite film changed from light source by wires to an efficiency test, as displayed in Fig. 1c.
yellow to dark brown. Beyond the cooling down to the room
temperature, ­PC71BM solution (20 mg in 1 ml of chloroben-
zene) thin film was spin coated at (500 rpm for 5 s). The 2.4 Characterization
mask shown in Fig. 1b was used to deposit the aluminum
as an electrode which fixed over the prepared films. The The crystalline phase and crystallite size of perovskite film
aluminum electrode was deposited by thermal evaporation were characterized via X-ray Diffractometer, type Shimadzu
under the pressure of ­10–5 mbr. 6000type (Japan) utilizing CuKα radiation (λ = 1.5406 Å)
The conversion efficiency of p-n silicon cell can be scan from 10° to 60°. The morphology of the perovskite
improved via preparing a tandem solar cell. Silicon cell film surface was examined via a Field Emission Scanning
used here was purchased from Al-Mansour factory (Bagh- Electron Microscope (FE-SEM, Zeiss, SUPRA 55) type.
dad/Iraq). The cells were cleaned with HF: DI water (5:1 Optical absorbance for perovskite layer was obtained at the
v/v) in an ultrasonic bath for 10 min to remove the ­SiO2 room temperature via (UV–VIS-NIR) spectrophotometer
layer that covers the front face of the silicon cell and then (type Shimadzu, UV-1800). The characteristics of the Cur-
cleaned with DI water in an ultrasonic bath for 10 min also. rent–Voltage (I-V) of silicon, perovskite as well as tandem
Tin oxide (­ SnO2) thin film was deposited on silicon cells solar cells were tested using a Keithley 2400 source meter
by the thermal evaporation method at the room temperature under a standard simulated light source of AM 1.5 G condi-
under vacuum of the order of 1­ 0–5 mbar using high purity tin tions (1000 W/cm2). Depending upon the (I–V) curve, the
as the source material, here ­SnO2 film employed as an anti- fill factor (FF) was computed by the following equation [23]:
reflection layer [22]. Following, the annealing of deposited
Pmax
film was conducted at (400 °C) for (1 h). Aluminum layer FF(%) = × 100 (1)
was deposited by thermal evaporation technique on the back- JSC .VOC
side of silicon cells. To form a two-terminal tandem solar where: Pmax: The maximum power, Jsc: The density of
cell, the two cells (PS and Si) were mechanically stacked the short-circuit photocurrent, Voc : The open-circuit
on the top of each other. Then, the electrolyte solution was photovoltage.
injected by a syringe between the two cells. Finally, FTO

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 Journal of Materials Science: Materials in Electronics

The efficiency (ɳ) of photoelectric conversion was com- [25]. Consequently, the XRD results revealed that the film
puted by this formula [24]: obtained in this study consisted of a pure S­ nO2 phase with-
out any secondary phases.
JSC ⋅ VOC ⋅ FF
𝜂(%) = × 100 (2) The crystal structure, crystallite size, and the prepared
Pin perovskite thin film phase were obtained utilizing XRD. The
where, ­Pinp is the incident power. X-ray diffraction patterns of M
­ APbI3 thin film deposited on
the glass substrate by spin coating method are displayed
in Fig. 2b. A set of pronounced peaks at 2θ with 14.09°,
3 Results and analysis 19.96°, 23.48°, 24.47°, 28.42°, 31.77°, 34.99°, 40.43°,
43.07° and 50.20° corresponding to the (110), (112), (211),
3.1 X‑ray diffraction (XRD) analysis (202), (220), (222), (312), (224), (314) and (404) planes of
the ­MAPbI3 tetragonal phase, correspondingly, which is in a
The crystalline phase and the preferred orientation of ­SnO2 good agreement with other documented researches [26–28].
film deposited via the process of thermal evaporation upon From the figure, no peaks associated with remaining ­PbI2
a glass substrate were obtained by the XRD technique. The and other phases of perovskite were observed, signifying
X-ray diffraction patterns of the ­SnO2 thin film are shown that the deposited thin films are in pure phase and crystal-
in Fig. 2a. The patterns indicate well-defined XRD peaks line in nature [29]. The presence of the higher number of
of crystallized S­ nO2 which were indexed to the tetrago- diffraction peaks indicates the successful conversion into
nal phase, which is consistent with the JCPDS card no. the perovskite structure. Similar results were obtained in ear-
41-1445, and such result agrees with those documented by lier reports [30–33]. Also from the figure, it was noted that
(110) is the main preferred direction in the crystal growth of
perovskite. The perovskite film with the oriented crystalline
domains thus ensures the high charge mobility necessary
(a) for the high-performance solar cells [34]. Consequently,
(110)

enhancing the crystal orientation and the perovskite film

crystallinity are good for the performance of optoelectronic
(101)

devices.
Intensity (a.u)

The crystallite size (D) was estimated by Scherrer’s for-

mula [35]:
(211)
(200)

K𝜆
D= (3)
(220)

𝛽COS𝜃
(112)
(310)

(301)
(202)

(321)

where, (K) is constant, (λ) is the wavelength of x-ray, which

is equal to 0.15406 nm, (β) is the full-width at half-max-
15 20 25 30 35 40 45 50 55 60 65 70 75 80 imum, and (θ) is Bragg angle [36]. The perovskite film
2θ ° lattice parameters were estimated as a = b = 8.8762 Å and
c = 12.6383 Å. The average crystallite size of the synthesized
perovskite film was obtained to be (40 nm).
(110)

(b)
(220)

3.2 Field emission scanning electron microscopy

(FE‑SEM) analysis
Intensity (a.u.)

The surface morphology of perovskite thin film depos-

ited on FTO substrate was examined by field emission
(202)

(224)
(222)

scanning electron microscopy. The top-view FE-SEM

(211)
(112)

(314)

image of the film is manifested in Fig. 3 revealing that

(404)
(312)

the film has a polycrystalline nature in the nano-scale. As

10 15 20 25 30 35 40 45 50 55 60 observed from the FE-SEM image, cuboid-like crystals
2θ ° and other irregular ones are formed [37]. The top view of
a perovskite film prepared depicts that the FTO substrate
Fig. 2  XRD patterns of: a ­SnO2 thin film and b ­MAPbI3 perovskite is not fully covered by the perovskite layer, and the per-
film on glass ovskite aggregates, which led to the formation of islands,

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Journal of Materials Science: Materials in Electronics

3.3 Atomic force microscope (AFM) analysis

Atomic force microscopy measurement was performed to

investigate the surface topography of the perovskite film
made via the spin-coated technique upon the FTO glass.
Figure 4a and b display the 3D image of AFM and the chart
of the granularity cumulative distribution of the film of per-
ovskite. The grain size, the average roughness and the root
mean square of the thin film was about 58.7 nm, 1.51 nm and
1.81 nm, respectively. From the results (AFM image), the
film containing a large grain size was noted. Some studies
indicated that a larger perovskite crystal size favors the light
absorbance [42]. The large grain size leads to decrease the
grain boundary with the carrier trapping sites and suppresses
Fig. 3  FE-SEM image of top-view of perovskite film the charge recombination, which makes for increasing the
carrier transport mobility in M
­ APbI3 film and the electrons
injection to the PEDOT: PSS layer from the perovskite layer
were observed [38]. From the image, the large grain size [43], which is an important reason for the increase of conver-
of perovskite crystal and the presence of some voids or sion efficiency of the perovskite device.
pinholes among the perovskite grains were noted [39].
The few pinholes present in the perovskite layer may be 3.4 Ultraviolet–Visible‑infrared spectrophotometer
attributed to the subsequent growth [40]. The pinholes (UV–Vis‑NIR) analysis
can produce direct contacts of a hole transporting layer
and an electron transporting layer, which causes poorer Figure 5 elucidates the UV–Vis absorption spectra of the
performance and big hysteresis in the perovskite solar perovskite thin film cast on the glass substrate. As explained
cells current density–voltage (J-V) curve [30]. Addi- in Fig. 5a, the perovskite film absorption spectra cover the
tionally, the large grains size presence in the film has a light’s broad range from the visible region to the near-IR
large vitality for the perovskite film-based optoelectronic region, depicting the M­ APbI3 perovskite formation during
apparatuses, since the decreased charge recombination at reaction [44] and also the improved crystallinity, which is
the grain boundaries as well as the carrier of charge can in a good agreement with previously reported works [33]. In
transport and be efficiently gathered in the big grains of addition, the spectra of the film show the absorption onsets
crystal [41]. at 800 nm nearly [45], suggesting the strong light absorption
for the perovskite film, which works as the solar cells active
layer, and causing the higher short-circuit current density

Fig. 4  a Perovskite thin film 3D (AFM) image and b Chart of the granularity Cumulative Distribution of perovskite film

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 Journal of Materials Science: Materials in Electronics

0.26

0.24

0.22
Absorbance (a.u.)

0.20

0.18

0.16

0.14

0.12

0.10

0.08
350 400 450 500 550 600 650 700 750 800 850 900 950

λ (nm)

Fig. 5  UV–Vis-NIR absorption spectra of perovskite film Fig. 6  Tauc’s plot of perovskite film

­(JSC) [15]. The spectra exhibit three distinct peaks located the higher efficiency compared to the silicon and perovskite
at ~ 420 nm, 520 nm and 756 nm, respectively [46]. The devices due to the absorption of photons with different wave
first peak of absorption at (756 nm) matches to the straight lengths. Table 1 summarizes the photovoltaic parameters of
bandgap shift from the initial valence band ­(VB1) to the the whole solar cells arranged in the present study (Fig. 7).
conduction band (CB) demonstrating that the material’s
photogeneration initiates at that wavelength, while the other 3.6 Comparison of the tandem solar cells
peaks at (520 nm) and (420 nm) attributed to the shift from performance
the second ­(VB2) and the third valence band ­(VB3) to (CB)
[44]. From the figure, it was observed that the reduction in A comparison between the conversion efficiency of the pre-
the absorbance is in the region (550–725 nm) which is the sent study and the efficiency of previous studies based on
feature of the M­ APbI3 film deposited using DMF solvent different parameters is shown in Table 2. The tandem device
[47]. prepared in this study recorded less efficiency compared to
Tauc’s model is employed to quantify the optical bandgap the references [35, 36, 51], this attributed to several reasons,
of ­MAPbI3 film using the following equation [48]: including the large active area and the use of an inverted
structure to prepare the device. In addition, the reason for
𝛼h𝜈 = A (h𝜈 − Eg )n (4) the emergence of pinholes in the perovskite film led to a
where, (α) is the coefficient of absorption, (hν) is the energy decrease in the performance of the device.
of photon, (A) is a constant that doesn’t relies upon energy
of photon, (Eg) is the optical bandgap and (n) possesses four
numeric values (1/2 for allowed direct, (2) for allowed indi- 4 Conclusions
rect, (3) for forbidden direct and (3/2) for forbidden indirect
optical shifts) [49]. Figure 6 displays the Tauc’s plot, where In this study, the perovskite solar cell was successfully
the allowed direct band gap of the ­MAPbI3 film can be esti- fabricated. The XRD analysis manifested that the M ­ APbI3
mated by the intercept of the extrapolation of the straight thin film prepared by spin coating method is appeared to be
line portion of the plot at (αhν)2 = 0. From the Tauc’s plot, it polycrystalline with nanostructure. According to the absorp-
was observed that the direct optical bandgap value of perovs- tion spectra, the ­MAPbI3 film is characterized by a wide
kite film is approximately 1.51 eV, which is in good agree- range of absorption, which extends from the visible region
ment with the previously reported articles [50].
Table 1  The photovoltaic parameters of the prepared devices
3.5 Photovoltaic performance analysis Solar cell type Jsc (mA/cm2) VOC (v) FF ɳ (%)

Perovskite 3.65 0.4 0.278 4.83

Figure 7 illustrates the characteristics of the current den-
Silicon 3.2 0.2 0.464 3
sity–voltage (J-V) curves for silicon, perovskite and tan-
Tandem 3.87 0.35 0.513 7.42
dem solar cells. In this figure, the tandem device evinces

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Journal of Materials Science: Materials in Electronics

Fig. 7  J-V curves characteris- 4.5

tics for silicon, perovskite and Si
tandem devices 4
Perovskite (MAPbI3)
3.5
Tandem
3

J (mA/cm²)
2.5
2
1.5
1
0.5
0
0 0.1 0.2 0.3 0.4 0.5

V (volt)

Table 2  Comparison between the efficiency of the tandem device and previous studies
References Structure of tandem solar cells Active area ­(cm2) ɳ (%)

Kanda et al. [51] Al/C-Silicon/ITO/Spiro-OMeTAD/MAPbI3 /TiO2/FTO glass 0.09 12.7

Albrecht et al. [35] Ag/AZO/C-Silicon/SnO2/MAPbI3/Spiro-OMeTAD/MoO3/ITO glass 0.25 16.1
Kanda et al. [36] Al/C-Silicon/ITO/IZO/MoO3/Spiro-OMeTAD/MAPbI3/m-TiO2/C-TiO2/FTO 0.09 13.9
glass
Present study Al/p-n Silicon/SnO2/PCBM/MAPbI3/PEDOT:PSS/FTO glass 1 7.42

to the infrared region and is therefore used as an absorbent perovskite solar cell using PEDOT: PSS for hole transport layer.
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