See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/369437992

Simulation study of CsPbI x Br 1-x and MAPbI 3 heterojunction solar cell using
SCAPS-1D

Article in Solar Energy · April 2023

DOI: 10.1016/j.solener.2023.02.059

CITATIONS READS

56 1,607

6 authors, including:

Vishwadeep Chakraborty Satish Kumar Yadav

University of Lucknow University of Lucknow
6 PUBLICATIONS 159 CITATIONS 28 PUBLICATIONS 576 CITATIONS

SEE PROFILE SEE PROFILE

Sujata Diwakar
University of Lucknow
3 PUBLICATIONS 56 CITATIONS

SEE PROFILE

All content following this page was uploaded by Sujata Diwakar on 22 March 2023.

The user has requested enhancement of the downloaded file.

 Solar Energy 254 (2023) 137–157

Contents lists available at ScienceDirect

Solar Energy
journal homepage: www.elsevier.com/locate/solener

Simulation study of CsPbIxBr1-x and MAPbI3 heterojunction solar cell using

SCAPS-1D
Sidra Khatoon a, Vishwadeep Chakraborty a, Satish Kumar Yadav b, *, Sujata Diwakar b,
Jyotsna Singh a, *, Rajendra Bahadur Singh a
a
Department of Physics, University of Lucknow, Lucknow, Uttar Pradesh 226007, India
b
Centre of Excellence in Renewable Energy Education and Research, Faculty of Science, University of Lucknow, Lucknow, Uttar Pradesh 226021, India

A R T I C L E I N F O A B S T R A C T

Keywords: The perovskite solar cells are attaining maximum efficiency but lagging in stability as compared with other solar
Perovskite solar cell cells. The consistent use of hybrid organic–inorganic materials in PSC poses greatest hurdle in the path of sta­
CsPbIBr2 bility. To overcome this problem the attention of research community, is diverted from methyl ammonium based
Triple layer
perovskite solar cells to cesium (Cs) based perovskite solar cell. To enhance the efficiency of PSCs further,
SCAPS-1D
effective absorption of solar-spectrum by the multi-layer will allow the maximum utilization of spectrum and in
turn it will increase the efficiency of the resulting Perovskite Solar Cell (PSC). Here, we have analyzed the ef­
ficiencies of single, double and triple absorber layers PSCs. Initially we have simulated and studied the perfor­
mance of two CsPbI2Br and CsPbIBr2 based single-junction perovskite solar cell. Then we have simulated a PSC
with CsPbI2Br and CsPbIBr2 as the two absorber layers and have optimized the performance of bilayer solar cell.
Finally, we simulated a triple layer PSC have used the combination of CsPbI2Br, CsPbIBr2 and MAPbI3 as absorber
layers. The bilayer and triple layer PSCs are optimized with respect to different variables i.e., absorber layer
thickness, defect density and interface defect density in all three PSCs. In this study we achieved a remarkable
efficiency of 29.92%, 20.62% and 7% efficiency in case of triple layer solar cell, in case of bilayer solar cell and in
case of single-junction PSC respectively. Thus, well aligned multiple absorber layers in PSC will provide the
future pathways for highly efficient PSCs.

The instability problem of PSCs can be effectively addressed by

1. Introduction substituting inorganic ions (such as Cs + ) for the organic ions at the A-
site. It has been found that switching out organic cations for inorganic
Solar energy has the greatest potential for mitigating the negative cations, like Cs, is an efficient way to get around these bottlenecks
effects of environmental change in our biosphere. New photovoltaic (Green et al., 2014; Kulbak et al., 2016). Among the Cs-based inorganic
technology, in particular perovskite solar cells, are the most emerging perovskite, CsPbBr3 has the highest resistance to heat and moisture
and efficient solar cell technology. Amongst PSC, the hybrid and lead (Chen et al., 2018; Duan et al., 2018) and is the most sought for com­
(Pb) based perovskite are the most researched which is due to their pound at present in the field of solar photovoltaic. The accumulated
exceptional optical and electrical properties, producing high efficiencies carrier mobility of a single crystal of CsPbBr3 has been found to be 2000
(Huang et al., 2017; Salado et al., 2017; Kazim et al., 2015). Due to their cm2V-1s− 1 which is more than nanosheet where mobility is roughly 77.9
exceptional photoelectric features, such as high absorption coefficients, cm2V-1s− 1 (Song et al., 2017; Yang et al., 2018). The maximum effi­
low exciton binding energies, long carrier diffusion lengths, high carrier ciency reported in literature in CsPbBr3 based PSC is approximately 11%
mobilities, and extractable bandgaps, all organic–inorganic hybrid which is lower than most of hybrid devices due to its wide bandgap as it
perovskite have received a lot of interest in recent years (Lee et al., 2012; enables to absorb upto 540 nm only (Zhu et al., 2022).
Shi et al., 2017). The thermal instability and inherent volatility of the Another candidate in Cs family is CsPbI3 which shows promising
organic material prevent the commercial viability of organic–inorganic properties for optoelectronic applications. CsPbI3 based PSC have ach­
hybrid PSCs despite the rapid progress observed in PCE (Power Con­ ieved maximum of 11.50% efficiency experimentally but theoretically it
version Efficiency) (Duan et al., 2018; Juarez-Perez et al., 2016). claimed approximately 21 % efficiency (Sebastian and Kurian, 2021).

* Corresponding authors.
E-mail addresses: [email protected] (S.K. Yadav), [email protected] (J. Singh).

https://doi.org/10.1016/j.solener.2023.02.059
Received 16 December 2022; Received in revised form 19 February 2023; Accepted 28 February 2023
Available online 16 March 2023
0038-092X/© 2023 International Solar Energy Society. Published by Elsevier Ltd. All rights reserved.
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Nomenclature amino)-9,9′ - spirobifluorene

CuSCN Copper thinocyanate
Abbreviation Full name ZnO Zinc-oxide
PSC Perovskite solar cell Eg Bandgap
FTO Flourine doped tin oxide χ Electron affinity
ETL Electron Transport layer εr Dielectrc permittivity
HTL Hole Transport Layer Nc Effective conduction band density of states
Voc Open-circuit voltage Nv Effective valance band density of states
Jsc Short-circuit current density μn Electron mobility
FF Fill Factor μp Hole mobility
PCE Photovoltaic Conversion Efficiency ND Donor concentration
PV Photovoltaic NA Acceptor concentration
TiO2 Tindioxide Nt Bulk defect density
MAPbI3 Methylammonium lead iodide Ntf Interface defect density
Spiro-OMeTAD 2,2′ ,7,7′ - Tetrakis (N,N-di(4-methoxyphenyl) NIP n-type, intrinsic, and p-type

Fig. 1. Structure of the CsPbIBr2 solar cell.

Fig. 2. Structure of the CsPbI2Br solar cell.

However it was discovered that CsPbI3 is only stable at high tempera­
tures in the form of a-phase (a cubic perovskite), which easily changes its
(Sebastian and Kurian, 2021; Ullah et al., 2020). In order to further
structure to orthorhombic d (non-perovskite) phase (Marronnier et al.,
increase efficiency of PSCs various researchers are focusing on hetero­
2018). While CsPbI2Br is another potential candidate which offers good
junction solar cells. The research community is working on multi-layer
stability and efficiency. For CsPbI2Br based PSC, Xue et al., achieves
solar cells to enhance the absorption such that maximum part of solar
champion efficiency of 16.50%, whereas its performance is still lower
spectrum is absorbed. Bhattari et al., used novel approach with multi-
than the hybrid and CsPbI3 based PSCs. The reasons for poor perfor­
layer graded absorber layers PSC to achieve 22.3% efficiency (Bhat­
mance are interfacial recombination and energy-level misalignment in
tarai et al., 2022; Bhattarai et al., 2021). Similarly in our previous work
PSCs. The right band structure must be created in order to optimize
we have used two absorber layers and have achieved 33.54% efficiency
carrier separation and enhance transport of carriers, suppress charge
(Khatoon et al., 2022). This study focuses on simulating and optimizing
recombination, and further improve the efficiency of the cesium based
Pb- based perovskite heterojunction solar cell for further enhancement
PSCs.
in the efficiency of perovskite solar cell. With the help of simulation tool,
Device simulation is used to explore the deeper working mechanism
we have optimized the performance of double layer solar cell and triple
of solar cells (Ho-Baillie et al., 2019; Wu et al., 2016; Ma et al., 2017).
layer solar cell.
The different software available in the market to simulate the solar cell
are SCAPS-1D, AMPS-1D etc. Deepthi et al., and Ullah et al., have used
2. Material method
SCAPS-1D simulation tool to simulate and optimize CsPbI3 and CsPbBr3
based PSCs have estimated11.99% and 15.89% efficiencies respectively
This is a simulation study using SCAPS-1D simulation tool. The

138
S. Khatoon et al. Solar Energy 254 (2023) 137–157

simulation tool uses continuity equation, drift–diffusion equation of

charge-carriers to calculate IV characteristics, quantum efficiency,
capacitance–voltage characteristics etc. Here the simulation is carried at
300 K temperature, airmass 1.5G radiation. The electron and hole ve­
locity is 107 m/sec.
In the first step, we have simulated the CsPbI2Br and CsPbIBr2 based
perovskite solar cells and validated experimentally. Fig. 1 shows
CsPbIBr2 based perovskite solar cell while Fig. 2 shows CsPbI2Br based
perovskite solar cell. In the second step, we have simulated bilayer
perovskite solar cell using CsPbI2Br and CsPbIBr2 as the two absorber
layers. In the third step, we have simulated triple layer perovskite solar
cell with CsPbI2Br, CsPbIBr2 and MAPbI3 is used as the three absorber
layers. The ZnO and CuSCN are selected as ETL and HTL respectively
using optimized results from our previous work. Fig. 3 shows perovskite
bilayer solar cell while Fig. 4 shows perovskite triple layer solar cell.
Upto our knowledge the study of triple layer perovskite solar cell with
this combination of material was never been done in past. Here the Cs
based (CsPbI2Br and CsPbIBr2) inorganic materials are selected to
enhance stability while MAPbI3 is selected for high efficiency as
absorber layers of bilayer PSC and triple layer PSC. Table 1 consists of
different parameters used in our simulation study taken from different
published work. Table 2 lists the various interface parameters at
different interface of perovskite solar cell.

3. Simulation and optimization

In this work, we have used SCAPS-1D simulation tool to study

perovskite heterojunction solar cell. The simulated CsPbIBr2 based
perovskite solar cell offers 13% efficiency which is in close approxi­
mation with Han et al., experimental work as shown in Table 3. Simi­
larly the efficiency of other combination of simulated CsPbI2Br solar cell
Fig. 3. Structure of bilayer solar cell.
was estimated as 14% which is approximately similar to Valadi et al.,
experimental work as shown in Table 4.Fig. 5(a) depicts the IV curve of
CsPbI2Br while Fig. 5 (b) represents the IV curve of CsPbIBr2 based
single junction PSC (See Table 5, Table 6 and Table 7).
Further the perovskite bilayer solar cell using CsPbIBr2 and CsPbI2Br
as the two absorber layers is simulated and this type of PSC offers
a15.04% efficiency as shown in Fig. 6. By adding one more layer to the
solar cell a triple layer solar cell is simulated which is made up of three
absorber layers i.e, CsPbI2Br, CsPbIBr2 and MAPbI3 gives perovskite a
remarkable improvement in the efficiency of PSC as efficiency jumps
from 15.04% to 25.17% as shown in Fig. 6. Now the optimization of PSC
is observed by varying three parameters (i) the thickness (ii) bulk defect
density (iii) interface defect density of all absorber layers of the bilayer
and triple layer heterojunction solar cell.

3.1. Effect of absorber layer thickness on bilayer perovskite solar cell

As the light strike the absorber layer in a solar cell, the electron-hole
pairs are generated and for efficient working of solar cell these pairs
must reach their respective electrodes without recombining. As a very
thick absorber layer promotes recombination of charge carriers before
they reach their respective electrodes and on the other hand a very thin
absorber layer results in poor absorption of light and thus reduce the
current density. In both cases the efficiency of PSC is compromised. In an
attempt to achieve an optimum thickness we have varied thickness of
the two absorber layers from 100 nm to 1000 nm. Initially the thickness
of the first absorber layer i.e., CsPbIBr2 is varied in the range 100 nm to
1000 nm keeping the thickness and all other properties constant. Here
initially there is enhancement in photovoltaic (PV) parameters on
increasing thickness, the efficiency increases roughly from 13% to 14%
and then decrease to 12%, Jsc increases from 14.58 mA/cm2 to 15.08
mA/cm2 and then decreases to 14.83 mA/cm2, and FF increases from
62.60% to 68.96% and then decreases to 59.31%, Voc decreases from
Fig. 4. Structure of triple layer solar cell.
1.43 V to 1.37 V as shown in Fig. 7. Here we observed optimum per­
formance around 600 nm thickness, thus the optimized thickness of the

139
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Table 1
Different parameters of PSCs.
Parameters FTO ZnO CsPbI2Br CsPbIBr2 MAPbI3 CuSCN

Thickness/nm 500 50 100–1000 100–1000 100–1000 150

Bandgap (Eg/eV) 3.5 3.3 1.9 2.07 1.5 3.4
Electron affinity (χ /eV) 4.0 4.0 3.8 3.7 3.9 1.9
Dielectrc permittivity (εr) 9.0 9 8.6 8.00 30 10
3
Effective conduction band density of states Nc/cm− 2.2 × 1018 2.2 × 1018 2 × 1018 2 × 1018 2.5 × 1020 1.7 × 1019
Effective valence band density of states(Nv/cm− 3) 1.8 × 1019 1.8 × 1019 5 × 1018 5 × 1018 2.5 × 1020 1.8 × 1019
Electron mobility μn/(cm2/V⋅s) 20 100 20 20 50 2.0 × 10-4
Hole mobility μp/(cm2/V⋅s) 10 25 20 20 50 2.0 × 10-1
Donor concentration ND/cm¡3 1 × 1019 1.0 × 1018 0 0 0 –
Acceptor concentration NA/cm− 3 0 – 1.0 × 1015 1.0 × 1015 1.0 × 1018 1.0 × 1018
Bulk defect density Nt,bulk/cm− 3 – 1.0 × 1015 1.0 × 1011 1.0 × 1016 1 × 1015 1.0 × 1014
References (Azri et al., 2019) (Yang et al., 2021) (Yang et al., 2021) (Raoui et al., 2019) (Azri et al., 2019)

first absorber layer of the bilayer PSC is 600 nm.

Table 2 Similarly, the thickness of the second absorber layer i.e CsPbI2Br is
Interface Defect Parameters.
varied in above-mentioned range keeping the thickness of first layer
Interface defect Interface 1 Interface 2 Interface 3 constant at 600 nm. The PCE of the device has been increased from
parameters
13.72% to 15.04% Jsc increased from 12.90 mA/cm2 to 15.98 mA/cm2,
Defect type Neutral Neutral Neutral while Voc is decreased from 1.47 V to 1.34 V, and FF decreased from
Capture-cross-section 1.00E-19 1.00E-19 1.00E-19 72.09% to 68.2% as shown in Fig. 8. We have observed optimum per­
electrons(cm2)
formance at around 800 nm thickness of the second layer, therefore the
Energetic distribution 1.00E-19 1.00E-19 1.00E-19
Reference for defect single single single optimized thickness of second layer of PSC is 800 nm.
energy level Et
Energy with respect to 0.1 0.1 0.1 3.2. Effect of absorber layer thickness on triple layer solar cell
Reference (ev)
Total density (1/cm2) 1.00E + 10 to 1.00E + 10 to 1.00E + 10 to
1.00E + 20 1.00E + 20 1.00E + 20 The thickness of all three layers in triple absorber layer PSC is varied
to examine its effect on photovoltaic performance. Initially thickness of
CsPbIBr2 layer has been varied from 200 nm to 800 nm. The PCE de­
creases from 23.94% to 19.97%, Jsc decreases from 21.94 mA/cm2 to
Table 3
CsPbIBr2 based single-junction Solar cell.
Table 5
CsPbIBr2 (Han et al., 2020) Voc (V) Jsc (mA/cm2) FF (%) η (%) Factors affecting PV performance Vs. optimized results.
Experimental 1.18 8.32 75.0 7.34 Factors affecting PV Optimized results Optimized results
Simulated 1.28 8.77 65.09 7.33 performance (bilayer) (Triple layer)

Absorber layer thickness 600 nm,800 nm 200 nm,200 nm,800 nm

Bulk defect density 1 × 1013 cm− 3 1 × 1013 cm− 3.
Interface defect density 1 × 1010 cm− 3 1 × 1010 cm− 3
Table 4
CsPbI2Br based single-junction solar cell.
CsPbI2Br (Valadi et al., 2021) Voc(V) Jsc (mA/cm2) FF (%) η (%) Table 6
Experimental 1.25 15.01 79.57 14.89 Optimized results of bilayer PSC before and after optimization.
Simulated 1.21 14.15 87.17 14.91 PV parameters (bilayer solar cell) Before optimization After optimization

Voc 1.37 V 1.55 V

Jsc 14.58 mA/cm2 15.94 mA/cm2
FF 62.60% 83.24%
Efficiency 13.26% 20.62%

Fig. 5. I-V curve of (a) CsPbI2Br and (b) CsPbIBr2 based solar cell.

140
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Table 7 Similarly, thickness is varied for CsPbI2Br layer and its effect on PV
Optimized results of triple layer PSC before and after optimization. performance was observed. The efficiency decreases from 27.55% to
PV parameters (triple layer solar Before After 16.18% while Jsc decreases from 24.65 mA/cm2 to 14.69 mA/cm2,Voc
cell) optimization optimization decreases from 1.24 V to 1.23 V and FF decreases from 89.93% to
Voc 1.09 V 1.23 V 89.34% as shown in Fig. 10. The performance degrades with rise in
Jsc 14.38 mA/cm2 27.1 mA/cm2 thickness of the CsPbI2Br absorber layer. Therefore we get optimum
FF 83.36% 89.79% performance at 200 nm thickness.
Efficiency 16.18% 29.92% Finally, PV performance was further enhanced when the thickness of
MAPbI3 is varied keeping thickness of other two layers constant. The
thickness of MAPbI3 has been varied from 200 nm to 800 nm. The ef­
ficiency increases from 19.41% to 28.78% as thickness increases from
200 nm to 800 nm, Jsc increases from 16.92 mA/cm2 to 25.97 mA/cm2
while FF decreases from 90.16% to 89.88% as shown in Fig. 11. Here
there is sharp increase in performance of PV parameters up to 800 nm
after that the performance saturates, therefore the optimum thickness
for MAPbI3 absorber layer is 800 nm.
The current density increases on increasing thickness which can be
observed from Fig. 9. This increase can be attributed to increase in
number of charge carriers. The increase in Jsc results in the increase of
efficiency of the device. Whereas a decrease in Voc is observed in Fig. 9
which can be assigned to enhancement in reverse saturation current
accelerating the recombination of charge-carrier. The variation in FF is
observed from Fig. 9 where we can observe that FF decreases on
increasing the thickness, due to increase in shunt resistance.
In case of bilayer PSC performance analysis, we observe that for
optimal performance the first absorber is thin because the increase in
thickness deteriorates the performance of PSC. For second absorber
layer of bilayer PSC we observe that the optimal thickness is more than
Fig. 6. I-V curve of bilayer and triple layer solar cell. the first layer. The difference in optimal thickness of the two absorber
layers is attributed to difference in absorption of longer wavelength of
solar spectrum by the two layers respectively. The second layer with low
17.99 mA/cm2 while there is no change in FF and Voc as shown in Fig. 9. bandgap of 1.9 eV absorbs upto 650 nm and on the other hand the first
The performance of the resulting device starts decreasing with increase absorber layer with 2.05 eV bandgap absorbs upto 600 nm only.
in thickness. Hence, we get optimum performance at 200 nm thickness. Therefore, second absorber layer requires more thickness while first

Fig. 7. Effect of CsPbIBr2 thickness variation on solar cell parameters.

141
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 8. Effect of CsPbI2Br thickness variation on solar cell parameters.

Fig. 9. Effect of CsPbIBr2 thickness variation on triple layer solar cell parameters.

absorber layer requires thinner layer. thickness of the MAPbI3 absorber layer. The difference in optimal
In case of triple layer PSC performance analysis, we have observed thickness of absorber layers, is due to the difference in bandgap of all the
that the efficiency decreases with increase in thickness for the CsPbI2Br three absorber layers. As mentioned above the absorber layer with lower
and CsPbIBr2 absorber layers while efficiency enhanced upon rising bandgap absorbs longer wavelengths of solar spectrum than the

142
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 10. Effect of CsPbI2Br thickness variation on triple layer solar cell parameters.

143
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 11. Effect of MAPbI3 thickness variation on triple layer solar cell parameters.

144
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 12. Effect of bulk defect density on the performance of CsPbIBr2 solar cell.

Fig. 13. Effect on quantum efficiency of CsPbIBr2 solar cell with the variation of wavelength.

145
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 14. Effect of bulk defect density on the performance of CsPbI2Br solar cell.

Fig. 15. Quantum efficiency variation of CsPbI2Br based solar cell.

146
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 16. Effect of bulk defect density on the performance of CsPbIBr2 based triple layer solar cell.

absorber layer which has higher bandgap. Thus, lower bandgap material
requires thicker absorber layer while higher bandgap requires thinner
material.

3.3. Effect of bulk defect density on bilayer solar cell

To optimize the PSC further, we have observed the variations in the

bulk defect density of the absorber layers. Initially we have allowed the
defect density (Nt) of the first absorber layer (CsPbIBr2) of bilayer PSC to
vary from 1 × 1013 cm− 3 to 1 × 1018 cm− 3. The effect of this variation on
different parameters of PV is shown in Fig. 12. We observe that rising
defect density of the first absorber between 1 × 1013 cm− 3 to 1 × 1015
cm− 3, have a negligible effect on PV parameters but as soon as the value
of Nt rises beyond 1 × 1015 cm− 3 there is a sharp decline in the per­
formance of the bilayer solar cell. Hence we can attribute that, 1 × 1015
cm− 3 is the optimal value of Nt as we observe reasonably good perfor­
mance of bilayer PSC but if the Nt is larger than this value the parameters
of PSC deteriorates. If the value of Nt rises further, from 1 × 1015 cm− 3 to
1 × 1018 cm− 3 the efficiency of the PSC decreases from 15.27% to
4.37%, and Jsc degrades from 15.84 mA/cm2 to 8.33 mA/cm2, while the
Voc decreases from 1.382 to 1.26 V and FF decreases from 70.18% to
41.32%.
Fig. 17. Quantum efficiency variation of CsPbIBr2 based triple layer solar cell. Similarly, the Nt of the second layer (CsPbI2Br) of the bilayer PSC is
varied keeping Nt of the first layer constant at 1 × 1015 cm− 3. For second
layer we have observed that the efficiency decreases from 20.02%
to10.99 % and Jsc decreases from 15.92 to 12.54 mA/cm2 while Voc

147
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 18. Effect of bulk defect density on the performance of CsPbI2Br based triple layer solar cell.

3.4. Effect of bulk defect density on triple layer solar cell

The bulk defect density (Nt) of the three absorber layers in triple
layer solar cell is varied, and its impact on PV performance is observed.
The range of variation of defect density value is between 1 × 1013 cm− 3
to 1 × 1018 cm− 3. Initially, the defect density of the first absorber layer
(CsPbIBr2) is varied keeping the defect density of other two layers
constant at 1 × 1016 cm− 3 and 1 × 1015 cm-3respectively. There is a
negligible effect of Nt on PV performance when Nt vary between 1 ×
1013 cm− 3 to 1 × 1015 cm− 3 but as soon as the Nt value increases beyond
1 × 1015 cm− 3 the efficiency decrease from 19.00% to 14.38%, Jsc de­
creases from 19.39 mA/cm2 to 14.76 mA/cm2 when Nt is 1 × 1018 cm-
3
while Voc and FF almost remain constant as observed from the Fig. 16.
Similarly the variation in Nt of the second absorber layer is observed
(CsPbI2Br) keeping the value of Nt constant for other two layers at 1 ×
1015 cm− 3. This variation in PV performance is demonstrated in Fig. 18
where we observe that there is a negligible effect on PV performance of
triple layer PSC between 1 × 1013 cm− 3 to 1 × 1015 cm− 3 but as soon as
the Nt value increases beyond 1 × 1015 cm− 3 the efficiency is decreased
from 25.41% to 12.33%, Jsc decreases from 25.72 mA/cm2 to 12.72
mA/cm2 when Nt is 1 × 1018 cm-3while Voc and FF remain same.
Fig. 19. Quantum efficiency variation of CsPbI2Br based triple layer solar cell. Finally, the bulk defect density of the third absorber layer that is
MAPbI3 is raised keeping the Nt of the other two layers fixed at 1 × 1015
reduces from 1.50 V to 1.35 V and FF from81.81% to 64.49% as depicted cm− 3. The variation in PV performance is presented in Fig. 17 where we
in Fig. 14. observe that initially there is a negligible effect on PV performance when
The rapid decline in the efficiency of bilayer PSC as the Nt of the two Nt vary between 1 × 1013 cm− 3 to 1 × 1015 cm− 3 but as soon as the Nt
absorber layers increases beyond 1 × 1015 cm− 3 is due to the rapid value increases beyond 1 × 1015 cm− 3 the efficiency decrease from
decline in the quantum efficiency of the CsPbI2Br and CsPbIBr2 absorber 19.39% to 0.29%, and the Jsc value is decreased from 20.91 mA/cm2 to
layers as shown in Fig. 13 and Fig. 15 respectively. nil when Nt is 1 × 1018 cm− 3 while Voc and FF have a negligible effect as
With the increase in the value of Nt addition of bulk defects come into observed from Fig. 20.
role. These defects create additional recombination centers for charge There is a rapid decline in the performance of triple layer PSC with
carriers. These defects allow the generated electron-hole pairs recom­ the variation in the defect density beyond 1 × 1015 cm− 3 in the three
bine before they can contribute to the external circuit. Hence the PV absorber layers. This behavior can be attributed to the rapid decline in
performance of the bilayer PSC declines with an increase in defect the quantum efficiency of the CsPbI2Br and CsPbIBr2 and MAPbI3
density of the two absorber layers beyond 1 × 1015 cm− 3. absorber layers as shown in Fig. 17, Fig. 19 and Fig. 21 respectively.

148
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 20. Effect of bulk defect density on the performance of MAPbI3 based triple layer solar cell.

peculiar behavior of the MAPbI3 absorber material is due to the fact that
it absorbs longer wavelengths of the solar spectrum than either the
CsPbI2Br or CsPbIBr2 absorber layer material. The defect density effect
efficiency and Jsc more than Voc and FF. This happens because the
defects produce recombination centers. With the addition of defects, the
charge carriers diffuse at these additional defect sites without reaching
their respective electrodes and hence reducing the Jsc. The reduced Jsc
further decreases the efficiency of triple layer PSC.

3.5. Effect of interface defect density on bilayer solar cell

To further optimize the PV performance of the bilayer PSC, the

interface defect density Ntf is varied at various interfaces of PSC. The
interface defects obstruct charge transport and therefore optimizing
interface defect density will help in better transport of charge-carriers in
the material. The Ntf has been varied at each interface of the device i.e at
ETL/absorber1, absorber1/absorber2, and absorber2/HTL interface in
the range 1 × 1010 to 1 × 1020 cm− 3.
When Ntf is varied in the above-mentioned range at ETL/absorber1
interface the Voc decrease from 1.55 V to 1.36 V, Jsc decrease from
15.94 mA/cm2 to 13.03 mA/cm2, FF reduces from 83.24% to 47.67%
Fig. 21. Quantum efficiency variation of MAPbI3 based triple layer solar cell. and efficiency decreases from 20.62% to 8.48% as observed from
Fig. 22.
Therefore the optimum defect density for triple layer PSC is in the range Similarly, Ntf has been varied in the above-mentioned range for
1 × 1013 cm− 3 to 1 × 1015. absorber1/absorber2 interface keeping the interface defect of another
We have observed that the defect density of MAPbI3 absorber ma­ interface constant at 1 × 1010 cm− 3. The variation of Ntf on different PSC
terial plays a vital role in performance analysis of triple layer PSC as it parameters are shown in Fig. 24. From where we can observe that with
make the PSC efficiency reduces rapidly such that we observe more than variation of Ntf the Voc decreased from 1.55 V to 1.36 V, Jsc decreased
90% reduction in the efficiency value for PSC when estimated for the from 15.94 mA/cm2 to 11.30 mA/cm2, FF reduces from 83.24% to
same is made at Nt = 1 × 1018 cm− 3 and Nt = 1 × 1015 cm− 3. This 70.56% and efficiency decreases from 20.62% to 10.85%.
Finally, the interface defect density is varied in the range 1 × 1010 to

149
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 22. Effect of interface defect density on PV performance at ZnO/CsPbIBr2 interface.

1 × 1020 cm− 3 at absorber2/HTL interface keeping the interface defect

at other interfaces constant at 1 × 1010 cm− 3. The variation of Ntf on
different PSC parameters are shown in Fig. 26 from where we can
observe that with variation of Ntf the Jsc degrades from 15.94 mA/cm2
to 15.54 mA/cm2, Voc decrease from 1.55 V to 1.32 V, FF degrades from
83.24% to 76.08% and efficiency decreases from 20.62% to 15.62%.
An important characteristic of PSC can be observed from Fig. 22, 24,
26. It shows that a decrease in PV performance of the solar cell on in­
crease in the interface defect density. This is because defect creates
recombination centres decreasing charge carrier density. Hence there is
a major decline in Jsc values than in Voc values. Also, it can be observed
from the Fig. 22, 24, 26 that there is a sharp decline in PV performance
after 1 × 1012 cm− 3. Such a decline in PV performance can be justified by
the quantum efficiency curve shown in Fig. 23, 25, 27 that beyond 1 ×
1013 cm− 3 value of Ntf the absorption of photons reduces sharply
(Khatoon et al., 2022). Also, the PV performance of the PSC is more
affected by variation in Ntf at ETL/Absorber1 interface than at HTL/
absorber2 interface as observed from Fig. 23 and Fig. 27 respectively.
This happens because we are simulating NIP solar cells with electrons as
majority carriers.

Fig. 23. Quantum efficiency with variable interface defect density at ZnO/
CsPbIBr2 interface. 3.6. Effect of interface defect density on triple layer solar cell

The interface defect density is varied in the range of 1 × 1010 cm− 3

to

150
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 24. Effect of interface defect density on PV performance at CsPbIBr2/CsPbIBr2 interface.

1 × 1018 cm− 3 to observe its effect on PV performance of triple layer

PSC. The Ntf is optimized at all four interfaces i.e at the ETL/absorber1
interface, absorber1/absorber2 interface, absorber2/absorber3 and
absorber3/HTL interface. At the ETL/absorber1 interface, the Ntf is
varied in the above-mentioned range keeping Ntf of all other layers
constant at 1 × 1010 cm− 3. The variation of Ntf on different PSC pa­
rameters are shown in Fig. 28 from where we can observe that with
variation of Ntf the efficiency is decreases from 29.96% to 19.88%, Jsc is
decreases from 27.11 mA/cm2 to 18.15 mA/cm2 while Voc and FF
remain almost constant.
Similarly at the second interface i.e at CsPbI2Br/CsPbIBr2, Ntf is
raised in the range 1 × 1010 cm− 3 to 1 × 1018 cm− 3 and its impact on PV
performance is observed on triple layer PSC. The variation of Ntf on
different PSC parameters are shown in Fig. 30 from where we can
observe that with variation of Ntf the efficiency is decreased from
29.96% to 16.5%, Jsc is decreased from 27.11 mA/cm2 to 15.13 mA/
cm2, while Voc and FF remain almost constant.
The Ntf at the third interface that is CsPbI2Br /MAPbI3 is varied from
1 × 1010 cm− 3 to 1 × 1018 cm− 3 to observe its effect on PV performance
of triple layer PSC. The variation of Ntf on different PSC parameters are
shown in Fig. 32 from where we can observe that with variation of Ntf
Fig. 25. Quantum efficiency with variable interface defect density at CsPbIBr2/ the PCE is decreased from 29.96% to 3.22%, Jsc is decreased from 27.11
CsPbIBr2 interface. mA/cm2 to 3.7 mA/cm2 while Voc and FF remain almost constant.
Finally, the Ntf is varied at CuSCN/MAPbI3 interface to see its effect

151
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 26. Effect of interface defect density on PV performance at CsPbI2Br/CuSCN interface.

Fig. 27. Quantum efficiency with variable interface defect density at CsPbI2Br/CuSCN interface.

152
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 28. Interface defect density variation at CsPbIBr2/ZnO interface.

to 10.67 mA/cm3 while there is slight variation in FF and Voc.

An important characteristic of PSC can be observed from Fig. 28, 30,
32, 34. It shows that PV performance of the solar cell degrades on in­
crease in the interface defect density. It happens because defect creates
recombination centers for charge carrier decreasing current density and
efficiency. Hence there is a greater decline in Jsc and efficiency values
than in Voc and FF values. Also, it can be observed from the Fig. 28, 30,
32, 34 that there is a sharp decline in PV performance after 1 × 1012
cm− 3. Such a decline in PV performance can be justified by the quantum
efficiency curve demonstrated in Fig. 29, 31, 33, 35 that beyond 1 ×
1012 cm− 3 value of Ntf the absorption of photons reduces sharply
(Khatoon et al., 2022). Also, the PV performance of the PSC is more
affected by variation in Ntf at ETL/Absorber1 interface than at
absorber3/HTL interface as observed from Fig. 29 and Fig. 35. This
happens because we are simulating NIP solar cells with electrons as
majority carriers.

4. Conclusion

In this study, the performance of bilayer PSC and triple layer PSC is
optimized using SCAPS-1D simulation tool. The optimization is achieved
Fig. 29. Quantum efficiency curve variation for CsPbIBr2/ZnO interface. by varying three important characteristics of the materials (i) absorber
layer thickness (ii) bulk defect density (iii) interface defect density of
bilayer and triple layer PSC. Firstly we have simulated inorganic
on PV performance keeping Ntf constant at 1 × 1012 cm− 3 of all other
perovskite solar cell i.e CsPbI2Br and CsPbIBr2 based perovskite solar
layers. The variation of Ntf on different PSC parameters are shown in
cell. The simulated results for performance studies of single junction PSC
Fig. 34 from where we can observe that with variation of Ntf the effi­
are approximately similar to experimental results but the FF needs to be
ciency decreases from 29.96 to 7.43%, Jsc decreases from 27.1 mA/cm2
redefined with better clarity.

153
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 30. Solar cell performance at CsPbIBr2/CsPbI2Br interface for defect density variation.

Fig. 31. Quantum efficiency curve variation for CsPbIBr2/CsPbI2Br interface.

Further, for bilayer solar cell the absorber layer materials are second absorber layers respectively while for triple layer PSC it is 200
CsPbI2Br and CsPbIBr2 whereas for triple layer solar cell the absorber nm,200 nm and 800 nm for first, second and third absorber layers
layers are CsPbI2Br, CsPbIBr2 and MAPbI3. The optimum thickness for respectively. Then we worked on the defect density in bulk material and
the two layers of bilayer solar cell are 600 and 800 nm for first and it has been found that the optimum range of defect density for CsPbI2Br,

154
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 32. Interface defect density variation at MAPbI3/CsPbI2Br interface.

Fig. 33. Quantum efficiency curve variation for MAPbI3/CsPbI2Br interface.

CsPbIBr2 and MAPbI3 is 1 × 1015 cm− 3 to 1 × 1013 cm− 3 but both bilayer 1 × 1010 cm− 3. Also we have observed that ETL interface plays an
and triple layer PSC shows best performance at 1 × 1013 cm− 3. Similarly, important role than the HTL interface. We found that as the number of
we have optimized interface defect density at the interface of ETL, HTL absorber layers increases the current density increases increasing effi­
and absorber layers of bilayer PSC and triple layer PSC and found that ciency. It is clear from Fig. 36 and Fig. 37 that both quantum efficiency
the optimum interface defect density range is 1 × 1012 cm− 3 to 1 × 1010 and photovoltaic conversion efficiency increases with an increase in the
cm− 3 but both bilayer PSC and triple layer PSC show best performance at number of absorber layer. In our study, we found that a single junction

155
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Fig. 34. Interface defect density variation at MAPbI3/CuSCN interface.

Fig. 35. Quantum efficiency curve variation for MAPbI3/CuSCN interface. Fig. 36. I-V curves of all type of perovskite solar cells.

perovskite solar cell gives 7% efficiency, bilayer solar cell gives 20.62% optimization with respect to various parameters of the PSCs results in an
efficiency and triple layer solar cell gives 29.92% efficiency. enhancement of efficiency of approximately 13%–21% in the case of a
As we have observed in this study, heterojunction PSC provides bilayer and 16%–30% in the case of a triple layer PSC. Therefore,
better efficiency with respect to single junction PSC. Further, the providing the researchers with more profound insights to enhance

156
S. Khatoon et al. Solar Energy 254 (2023) 137–157

Duan, J., Zhao, Y., He, B., Tang, Q., 2018. High-purity inorganic perovskite films for
solar cells with 9.72% efficiency. Angew. Chemie. 130, 3849–3853.
Duan, J., Zhao, Y., Yang, X., Wang, Y., He, B., Tang, Q., 2018. Lanthanide ions doped
CsPbBr 3 halides for HTM-free 10.14%-efficiency inorganic perovskite solar cell with
an ultrahigh open-circuit voltage of 1.594 V. Adv. Energy Mater. 8, 1802346.
Green, M.A., Ho-Baillie, A., Snaith, H.J., 2014. The emergence of perovskite solar cells.
Nat. Photonics. 8, 506–514.
Han, Y., Zhao, H., Duan, C., Yang, S., Yang, Z., Liu, Z., Liu, S., 2020. Controlled n-doping
in air-stable CsPbI2Br perovskite solar cells with a record efficiency of 16.79%. Adv.
Funct. Mater. 30, 1909972.
Ho-Baillie, A., Zhang, M., Lau, C.F.J., Ma, F.-J., Huang, S., 2019. Untapped potentials of
inorganic metal halide perovskite solar cells. Joule. 3, 938–955.
Huang, J., Yuan, Y., Shao, Y., Yan, Y., 2017. Understanding the physical properties of
hybrid perovskites for photovoltaic applications. Nat. Rev. Mater. 2, 1–19.
Juarez-Perez, E.J., Hawash, Z., Raga, S.R., Ono, L.K., Qi, Y., 2016. Thermal degradation
of CH 3 NH 3 PbI 3 perovskite into NH 3 and CH 3 I gases observed by coupled
thermogravimetry–mass spectrometry analysis. Energy Environ. Sci. 9, 3406–3410.
Kazim, S., Ramos, F.J., Gao, P., Nazeeruddin, M.K., Grätzel, M., Ahmad, S., 2015.
A dopant free linear acene derivative as a hole transport material for perovskite
pigmented solar cells. Energy Environ. Sci. 8, 1816–1823.
Khatoon, S., Yadav, S.K., Singh, J., Singh, R.B., 2022. Design of a CH3NH3PbI3/CsPbI3-
based bilayer solar cell using device simulation. Heliyon. 8, e09941.
Kulbak, M., Gupta, S., Kedem, N., Levine, I., Bendikov, T., Hodes, G., Cahen, D., 2016.
Cesium enhances long-term stability of lead bromide perovskite-based solar cells.
J. Phys. Chem. Lett. 7, 167–172.
Fig. 37. Quantum efficiency curves of all type of perovskite solar cells. Lee, M.M., Teuscher, J., Miyasaka, T., Murakami, T.N., Snaith, H.J., 2012. Efficient
hybrid solar cells based on meso-superstructured organometal halide perovskites,
Science (80-.), 338, 643–647.
efficiency experimentally. Also, the study is conducted using inorganic Ma, L., Liu, P., Wu, X., Li, H., Jiang, Y., Tu, L., Chen, Y., Lu, J., Yang, S., 2017.
materials for each layer of the solar cell as they are more stable than Investigation of organic–inorganic hybrid perovskite solar cells based on Al2O3
organic materials. As a result, our optimization study paves the way for nanorods. Sol. Energy. 153, 77–82.
Marronnier, A., Roma, G., Boyer-Richard, S., Pedesseau, L., Jancu, J.-M.,
the fabrication of highly efficient and stable all-inorganic PSCs in the Bonnassieux, Y., Katan, C., Stoumpos, C.C., Kanatzidis, M.G., Even, J., 2018.
future. Anharmonicity and disorder in the black phases of cesium lead iodide used for stable
inorganic perovskite solar cells. ACS Nano. 12, 3477–3486.
Raoui, Y., Ez-Zahraouy, H., Tahiri, N., El Bounagui, O., Ahmad, S., Kazim, S., 2019.
Declaration of Competing Interest Performance analysis of MAPbI3 based perovskite solar cells employing diverse
charge selective contacts: Simulation study. Sol. Energy. 193, 948–955.
Salado, M., Kokal, R.K., Calio, L., Kazim, S., Deepa, M., Ahmad, S., 2017. Identifying the
The authors declare that they have no known competing financial charge generation dynamics in Cs+-based triple cation mixed perovskite solar cells.
interests or personal relationships that could have appeared to influence Phys. Chem. Chem. Phys. 19, 22905–22914.
the work reported in this paper. Sebastian, V., Kurian, J., 2021. Simulation and optimization studies on CsPbI3 based
inorganic perovskite solar cells. Sol. Energy. 221, 99–108.
Shi, Z., Li, Y., Zhang, Y., Chen, Y., Li, X., Wu, D., Xu, T., Shan, C., Du, G., 2017. High-
Acknowledgement efficiency and air-stable perovskite quantum dots light-emitting diodes with an all-
inorganic heterostructure. Nano Lett. 17, 313–321.
Song, J., Cui, Q., Li, J., Xu, J., Wang, Y., Xu, L., Xue, J., Dong, Y., Tian, T., Sun, H., 2017.
The authors are thankful to Dr Marc Burgelman (Department of Ultralarge all-inorganic perovskite bulk single crystal for high-performance
Electronics and information systems (ELIS) of the University of Gent, visible–infrared dual-modal photodetectors. Adv. Opt. Mater. 5, 1700157.
Ullah, S., Liu, P., Wang, J., Yang, P., Liu, L., Yang, S.-E., Guo, H., Xia, T., Chen, Y., 2020.
Belgium) for providing SCAPS-1D software. Sidra Khatoon is thankful to
Optimizing the working mechanism of the CsPbBr 3-based inorganic perovskite solar
University Grant Commission, India for providing the fellowship (UGC- cells for enhanced efficiency. Sol. Energy. 209, 79–84.
JRF). Valadi, K., Gharibi, S., Taheri-Ledari, R., Akin, S., Maleki, A., Shalan, A.E., 2021. Metal
oxide electron transport materials for perovskite solar cells: a review. Environ.
Chem. Lett. 19, 2185–2207. https://doi.org/10.1007/s10311-020-01171-x.
References Wu, X., Liu, P., Ma, L., Zhou, Q., Chen, Y., Lu, J., Yang, S., 2016. Two-dimensional
modeling of TiO2 nanowire based organic–inorganic hybrid perovskite solar cells.
Azri, F., Meftah, A., Sengouga, N., Meftah, A., 2019. Electron and hole transport layers Sol. Energy Mater. Sol. Cells. 152, 111–117.
optimization by numerical simulation of a perovskite solar cell. Sol. Energy. 181, Yang, P., Liu, P., Ullah, S., Wang, J., Liu, L., Yang, S.-E., Guo, H., Wang, L., Chen, Y.,
372–378. 2021. The investigation of CsPb (I1− xBrx) 3/crystalline silicon two-and four-
Bhattarai, S., Sharma, A., Muchahary, D., Gogoi, D., Das, T.D., 2021. Numerical terminal tandem solar cells. Sol. Energy. 216, 145–150.
simulation study for efficiency enhancement of doubly graded perovskite solar cell. Yang, Z., Wang, M., Qiu, H., Yao, X., Lao, X., Xu, S., Lin, Z., Sun, L., Shao, J., 2018.
Opt. Mater. (Amst). 118, 111285. Engineering the exciton dissociation in quantum-confined 2D CsPbBr 3 nanosheet
Bhattarai, S., Pandey, R., Madan, J., Muchahary, D., Gogoi, D., 2022. A novel graded films. Adv. Funct. Mater. 28, 1705908.
approach for improving the efficiency of Lead-Free perovskite solar cells. Sol. Zhu, J., Liu, Y., He, B., Zhang, W., Cui, L., Wang, S., Chen, H., Duan, Y., Tang, Q., 2022.
Energy. 244, 255–263. Efficient interface engineering of N, N’-Dicyclohexylcarbodiimide for stable HTMs-
Chen, H., Xiang, S., Li, W., Liu, H., Zhu, L., Yang, S., 2018. Inorganic perovskite solar free CsPbBr 3 perovskite solar cells with 10.16%-efficiency. Chem. Eng. J. 428,
cells: a rapidly growing field. Sol. Rrl. 2, 1700188. 131950.

157

View publication stats