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Performance Analysis of Perovskite Solar Cells Using DFT-

Extracted Parameters of Metal-Doped TiO2 Electron Transport
Layer
Sadiq Shahriyar Nishat,∥ Md. Jayed Hossain,∥ Faiyaz Elahi Mullick, Alamgir Kabir, Shaestagir Chowdhury, Sharnali
Islam, and Mainul Hossain*
Cite This: J. Phys. Chem. C 2021, 125, 13158−13166 Read Online

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ABSTRACT: The performance of perovskite solar cells (PSCs) depends heavily on the
electronic and optical properties of the electron transport layer (ETL). Density functional
theory (DFT) uses a quantum-mechanical approach to accurately predict the properties
of different layers in PSCs, including the ETL. Titanium dioxide (TiO2 ) is a widely used
material for the ETL in PSCs. In this work, we use first-principles calculations based on
DFT to obtain the electronic and optical properties of pristine rutile TiO2 and TiO2
doped with tin (Sn) and zinc (Zn). DFT-extracted carrier mobility, band gap, and the
absorption spectrum of TiO2 are used in the SCAPS-1D device simulator to evaluate
the performance of the solar cell device, with respect to dopant concentration and
thickness of TiO2 . PSCs with 3.125 mol % Sn-doped TiO2 achieve a maximum power conversion efficiency (PCE) of 17.14
versus 13.70% with undoped TiO2 . We have also compared the performance of PSCs with Sn-doped and Zn-doped TiO2 . For
the same dopant concentration, Sn-doped TiO2 offers 0.63% higher PCE than the Zn-doped counterpart. The results are in
good agreement with reported experimental findings and provide a reliable means of evaluating PSC performance by combining
first-principles (DFT) calculations with conventional device simulations.

1.INTRODUCTION

Organic−inorganic lead halide perovskite solar cells (PSCs)
have attracted a great deal of attention in recent years as a
potential candidate to replace commercial silicon solar cells.
Perovskites offer a direct band gap, a high optical absorption
coefficient, broadband absorption, a long carrier lifetime,
high carrier mobility, and easy fabrication through well-
established, low-cost, solution-processing techniques.
Developments in the perovskite technology have led to
significant improvement in the power conversion efficiency
(PCE) of PSCs, with the certified PCE increasing from 3.8% in
2009 to 25.2% in 2020,1−4 exceeding the efficiency of
existing copper−indium−gallium− selenide and
cadmium−telluride (CdTe) solar cells. Electron and hole pairs
are generated in the perovskite as it absorbs incident light
photons with energy larger than the band gap of the
perovskite. In a typical PSC, the light-absorbing perovskite is
sandwiched between an electron transport layer (ETL) and a
hole transport layer (HTL). MAPbX3 is the most commonly
used metal-halide perovskite, where MA represents
methylammonium and X is I, Cl or Br. The ETL consists of
metal oxide thin films, typically made of titanium dioxide
(TiO2 ) 5 or tin oxide (SnO2),6 while Spiro-OMeTAD (2,2′,7,7′-
tetrakis-(N,Np-di-methoxy-phenylamino)-9,9′-
spirobifluorene)7 is most commonly used as the HTL.
Depending on the PSC device architecture, the built-in,
internal electric field from the n-i-p or p-i-n heterojunction
injects electrons into the ETL and holes into the HTL from the
perovskite layer, thereby avoiding direct recombination. The
charge transport layers, therefore, plays a major role in
extracting and transporting the photogenerated charge
carriers from the perovskite absorber layer to the respective
anode and cathode electrodes. Several factors, such as the
presence of interfacial defects, thickness, doping, carrier
injection rate, absorption spectrum, and chemical stability of
the transport layers, determine the performance of the PSC
device.8,9 In addition to numerous experimental efforts,
researchers have also used electrical and optical simulations
to optimize the ETL and HTL layers for improving device
performance.10,11 Solar cell capacitance simulator one
dimension (SCAPS-1D) software has been extensively
applied to extract basic electrical characteristics and
determine the PCE of PSCs.12−14 Despite the considerable
success of SCAPS-1D in predicting PSC performance, the
accuracy, with which different transport layers are modeled,
can be compromised by using built-in absorption spectrums
in SCAPS-1D. Device simulators, like SCAPS-1D, employ a
simplified combination of power laws
Published:

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Figure 1. (a) Schematic of the simulated device structure; (b) energy band diagram of the simulated device.
to derive the absorption spectrum as a function of photon energy.
This may often lead to unrealistic outputs, creating discrepancies
between simulation and experimental results, as discussed in the
recent work by Laali et al.15
Light absorption and charge carrier diffusion are governed by
fundamental properties like the material band gap, dielectric
constant, and effective mass of the carriers, which can be
computed, within the quantum-mechanical approach, under
various conditions (e.g., doping, temperature, and so forth) by
using density functional theory (DFT) calculations.16 Recently,
several studies have used DFT as an independent tool to study the
material properties of solar cells. Giorgi et al. used DFT analysis to
investigate the role played by the MA cation in determining the
band structure of MAPbI3. 17 Ma et al., on the other hand,
developed a set of algorithms based on DFT and time-dependent
DFT calculations to accurately predict the PCE of dye-sensitized
solar cells.18 Akbari et al. employed first principles calculations to
investigate the stability and electronic structure of perovskite/TiO2
and perovskite/Al2O3 interfaces.19 A comprehensive DFT study was
performed by Rahman et al. to extract the optical constant, energy
band gap, and effective mass of charge carriers in MAPbCl3,
MAPbBr3 and MAPbI3 perovskites under different concentrations
of halogen dopants.20 Besides, defects in perovskites were
thoroughly examined by Yin et al. using first-principles DFT
methods.21 Kumar et al. employed SCAPS 1-D software to study the
performance of lead-free double PSCs, where the band gap analysis
was done using DFT.22 Till date, most of the DFT studies have
focused on exploring the fundamental properties of the perovskite
layer. There have only been a few attempts to theoretically
investigate the structural, electronic, and optical properties of the
transport layers in PSCs through first-principles calculations.23−26
For the ETL in PSCs, TiO2 has been the primary material of choice
owing to its non-toxic nature, high chemical stability, transparency
to solar radiation, and easy fabrication. In addition, TiO 2 offers a
fast injection of photogenerated electrons from the perovskite
layer. A recent study by Zhang et al. demonstrated PSCs with
dopamine-capped TiO2 nanoparticles as the ETL, providing long-
term stability and enhanced charge-extraction efficiency at the TiO2
and perovskite interface.27 Additionally, pristine TiO2 can be doped
with a variety of dopants to enhance electron mobility and reduce
electronic trap states. The dopants for TiO2 can be alkali metals,5
non-metals,28 transition metals,29 post-transition metals,30
metalloids,31 and lanthanides.32 Among a myriad of potential
dopants, tin (Sn) and zinc (Zn) have been demonstrated as excellent
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candidates for doping TiO2. Doping with Sn significantly improves
charge carrier mobility and electrical conductivity of the pristine
TiO2. 33 Zn doped TiO2, on the other hand, is of low cost and offers
excellent transport properties along with a reduced trap-state
density.29,34 In this work, we use first-principles DFT calculations to
extract the electronic and optical properties of pristine, Sndoped,
and Zn-doped TiO2 films. First, the DFT-extracted optical absorption
spectrum, band gap, and carrier mobilities of pristine TiO2 and TiO2
doped with different concentrations of Sn are used in the SCAPS-
1D simulator to derive the electrical characteristics and PCE of the
PSCs. In addition, the influence of ETL thickness, on device
performance, has also been studied. The simulation results match
closely with the experiments, reported by Cai et al.33 Thus,
combining DFT calculations with the SCAPS-1D device simulator
provides the well-sought theoretical platform to predict PSC
performance with high accuracy. Finally, for a fixed dopant
concentration, we compare the performance of PSCs with Sn- and
Zn-doped TiO2 using the DFT-extracted parameters.
2. MODELING AND METHODS
2.1. Device Architecture. The schematic of the PSC device,
simulated in this work, is shown in Figure 1a. The planar, one-
dimensional heterostructure device has an n−i−p configuration,
where the ETL (pristine TiO2, 80 nm), perovskite (CH3NH3PbI3, 310
nm), and HTL (Spiro-OMeTAD, 160 nm) serve as the n-type (n),
intrinsic (i), and p-type (p) regions, respectively. To account for the
interface recombination, the perovskite/TiO2 interface layer (IL1)
and the perovskite/Spiro-OMeTAD interface layer (IL2) have been
considered during device simulations.35,36 The structure is
illuminated from the top at normal incidence using the standard
AM 1.5G spectrum (1 kW/m2 ) at 300 K. When irradiated with
sunlight, excitons are generated in the perovskite layer. The electric
field between the ETL (n-layer) and the HTL (p-layer) causes the
electrons to migrate to the n-layer, while the holes are transported
to the player. Figure 1b illustrates the energy band diagram of the
simulated device, clearly showing the separation and
transportation of the photogenerated charge carriers.
2.2. DFT Calculations. The electronic structure and optical
properties of many-body systems can be investigated, within the
quantum-mechanical approach, using well-established DFT
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Article

The carrier mobilities in pristine and doped TiO2 are calculated

using the BoltzTraP2 code44 with the constant relaxation time
approximation (CRTA) method. The DFTextracted band structure
calculations. In this work, we used DFT, with Hubbard-based U
is combined with the BoltzTraP2 code to calculate the carrier
correction, namely, the DFT + U method, to derive the absorption
effective mass and mobility, with a relaxation time of 10−10
spectrum, electronic band gap, carrier effective mass, and mobility of
s.45,46 The mobility calculations are discussed in detail in the
the rutile polymorph of the pristine and doped TiO2 films, which is the
Supporting Information. Table S1 of the Supporting Information
ETL of PSCs. The Hubbard U model37 was implemented to improve the
presents the computed electron and hole mobilities of undoped
accuracy in band gap calculations. The U term affects the lattice
and doped TiO2 layers. An alternative technique, which combines
parameters, expanding the cell as the U value increases. In the DFT + U
the deformation potential (DP) method47 with DFT-based
scheme, the on-site coulombic (U) and exchange (J) terms were
effective mass approximation, can be used to compute carrier
combined into a single effective U parameter (Ueff) to account for
mobilities. However, mobility values, obtained from the DP
errors in the exchange−correlation of Ti 3d and O 2p orbitals. The on-
method, do not agree well with the experimental findings. The
site Coulomb potential ofUeff = 8.0 eV on the dorbital of Ti and Ueff =
optical properties of pristine and doped TiO2 are obtained using
6.5 eV on the p-orbital of oxygen (O) have been used in this calculation.
independent particle approximation which combines occupied
The band gap of TiO2, computed using these U values, is in good
and unoccupied bands to calculate the imaginary part of the
agreement with the experimentally determined band gap found in the
dielectric function. The real part of the dielectric function is
literature. For the Sn-doped case,Ueff = 6.0 eV has been used for the d-
derived from the imaginary part using the Kramers−Kronig
orbital of Sn. The choice ofU= 6.0 eV for Sn is validated by computing
transform. The dielectric functions are then used to obtain the
the band gap of pure SnO2. The results show that the DFT + U calculated
optical absorption spectrum as described in the Supporting
band gap of 3.52 eV is in good agreement with the experimentally
Information. Different k-point mesh densities have been used to
determined band gap of 3.60 eV.38 All DFT calculations were carried
test the convergence of the absorption spectrum. The results
out using the Vienna ab initio simulation package.39,40 Projector
show that the 7 × 7 × 11, 4 × 4 × 3, 4 × 4 × 4, and 4 × 4 × 5 k-point
augmented wave (PAW) pseudopotential41 was used to account for
densities give well-converged optical spectra for pure TiO2 and
the electron-ion core interaction, with the Perdew−Burke−Ernzerhof
3.125, 4.17, and 6.25 mol % Sn-doped TiO2, respectively. For
function as generalized gradient approximation42 for the exchange−
instance, Figure S2 of the Supporting Information shows excellent
correlation term. A cutoff energy of 500 eV was used to expand the
k-point convergence in the absorption spectrum for 4.17 mol %
Kohn−Sham orbitals into plane-wave basis sets. The employed
Sn-doped TiO2. The optical absorption spectrum of each layer
pseudopotentials correspond to the configurations 3s2 3p6 3d2 4s2 for
depends on its band gap, which can be tuned by using different
Ti and 2s2 2p4 for O atoms. Reciprocal space projection was used for
dopants or by simply changing the concentration of a specific
the PAW operators, with the projection operators optimized to an
dopant. SCAPS-1D offers multiple models and sub-models15 to
accuracy of 1.0 × 10−7 eV/Å. All calculations were spin-polarized and
generate the optical absorption spectrum of each layer. In this
were geometrically optimized without symmetry or spin constraints.
work, the absorption spectra of undoped and doped TiO2 (ETL)
The structures converged when the forces on all atoms were less than
are extracted from the DFT calculations. For CH3NH3PbI3
0.005 eV/ Å. For the relaxation of the rutile TiO2 unit cell, the 7 × 7 × 11
(perovskite) and SpiroOMeTAD (HTL), the absorption spectra,
Monkhorst−Pack scheme43 and the Gaussian smearing model, with σ
used in the device simulations, are obtained from those reported
= 0.05, were used to integrate the Brillouin zone. High accuracy in
by Phillips et al.48 and Filipičet al., 49 respectively.
energy and density of state (DOS) calculations originate from a denser
mesh with a 11 × 11 × 17 k-point grid. For modeling rutile TiO2 doped 2.3. Device Modeling. The current−voltage characteristics of the
with Sn, 4 × 2 × 2, 3 × 2 × 2, and 2 × 2 × 2 TiO 2 supercells are created, PSC are obtained using SCAPS-1D software by solving the
which correspond to 3.125, 4.17, and 6.25 mol % Sn-doped TiO2, following semiconductor equations under steady-state
respectively. conditions as a function of the position coordinate x 10

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observed that the valence band region is constructed by Ti 3d, O
2p, and Sn 4d orbitals, occupying the energy bands between 2.2
and 6 eV. The conduction band, on the other hand, consists of
contributions from Ti 3d, O 2p, and Sn 5s orbitals occupying the
energy bands between 0 and 5.8 eV. Therefore, depending on the
concentration, the 4d and 5s orbitals of Sn modulate the
conduction band minima (CBM) and the valence band maxima
(VBM), resulting in changes in band gap. For pristine rutile TiO2,
the DFT-calculated band gap is 3.00 eV. When doped with Sn, the
Sn 5s defect orbitals push the conduction band toward a higher
energy, slightly changing the energy band gap from 2.98 eV
(3.125 mol % Sn) to 2.99 eV (4.17 mol % Sn). The results are in
good agreement with previously reported studies.33,50,51 At
higher Sn concentrations (6.25 mol % Sn), the band gap decreases
to 2.83 eV because of the larger number of valence electrons of
Sn compared to Ti.
3.2. Optical Properties of TiO2. The performance of the solar cell
heavily depends on the absorption coefficient of the TiO2 layer.
Figure 3 shows a significant difference between the
Figure 3. Absorption spectrum of pristine rutile TiO2 obtained from DFT
and SCAPS
DFT-calculated absorption spectrum of pristine rutile TiO2 and
the default, analytical optical absorption spectrum, obtained
from SCAPS. In the traditional SCAPS model, the optical
absorption, α(λ), as a function of wavelength (λ) is given by
where hν is the incident photon energy, Eg is the material
band gap, and A (in cm−1 eV−1/2) and B (in cm−1 eV1/2) are the
model parameters.52 From Figure 3, it is clear that in
comparison with SCAPS, the DFT calculations yield a more
realistic absorption profile for pristine rutile TiO2, with
significantly stronger absorption in the shorter, ultraviolet
(UV) wavelength regions.33 The default SCAPS spectrum, on
the other hand, shows a considerably lower absorption
profile throughout the entire wavelength
Figure 4. DFT-extracted (a) absorption and (b) transmittance spectra of pristine and Sn-doped TiO2; (c) Tauc plots, showing optical band gaps
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range, which leads to an overestimation of the number of photons
reaching the perovskite layer. Hence, the DFT-derived optical spectra
more accurately predict the device performance, as discussed in the
subsequent sections.
Figure 4a,b compares the absorption spectrum and transmittance
between undoped and Sn-doped TiO2 layers. Doping with Sn
increases the optical band gap of TiO2, causing the absorption edge
to be blue-shifted, as shown in Figure 4a. Maximum absorption
occurs in the UV region, below 400 nm, for both doped and undoped
TiO2. Doped TiO2 samples exhibit enhanced transmittance,
compared to the undoped counterpart. Figure 4b confirms that in the
visible range, 3.125 mol % Sndoped TiO2 provides the highest
transmittance, allowing a larger number of incident photons to pass
through the ETL and reach the perovskite layer.
The indirect band gap, Eg, of pristine and doped TiO2 can be
derived from the absorption spectrum using the Kubelka−Munk
formula33,53
where C is the proportionality constant. Figure 4c shows the optical
band gaps derived from the Tauc plots, where Sn-doped TiO2 films
exhibit higher optical band gaps than the pristine TiO2. As the Sn
doping concentration is increased above 3.125 mol %, the optical
band gap decreases from 3.196 eV (3.125 mol % Sn) and 3.146 eV
(4.17 mol % Sn) to 3.088 eV (6.25 mol % Sn). This is consistent with
the experimental findings by Cai et al., 33 where the decrease in the
optical band gap at high doping concentrations is attributed to the
structural defects caused by the overdose of Sn dopants. The optical
absorption spectrum and the corresponding band gaps obtained
from the Tauc plots have been used as input parameters in the
subsequent SCAPS1D simulations to obtain the electrical
characteristics of the PSC device.
3.3. Solar Cell Device Characteristics. The current− density
versus voltage (J−V) graphs of pristine and Sn-doped rutile TiO2 are
shown in Figure 5a. For the undoped TiO2, the simulated results are
obtained using the DFT-extracted absorption spectrum as well as the
default, built-in spectrum used in the SCAPS simulator. For the same
input parameters, the J−V curve, corresponding to the DFT-extracted
absorption spectrum, matches more closely with the experimental
results, reported by Cai et al.33 Also, PSC with Sn-doped TiO2 yields
a higher PCE than the one with undoped TiO2. Doping with Sn causes
a positive shift in Fermi energy of pristine TiO2, which
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improves the efficiency of electron injection.33,54
Moreover, Sndoped TiO2 has a higher conductivity
than the undoped counterpart, leading to more
efficient electron extraction at the TiO2/perovskite
interface. Both these factors contribute to higher
values of short-circuit current density (Jsc) and fill
factor (FF) in PSCs with Sn-doped TiO2. Also, reduced
carrier recombination and improved charge
collection and separation enhance the open-circuit
voltage (Voc) in Sn-doped TiO2 PSCs. Table S2 of the
Supporting Information summarizes the output
photovoltaic parameters of PSCs with undoped and
doped TiO2. The PCE of the proposed device, with
pristine rutile TiO2 is 13.70%, whereas the PCEs for
the Sn-doped TiO2 devices are 17.14% (3.125 mol %
Sn), 17.07% (4.17 mol % Sn), and 15.42% (6.25 mol %
Sn), respectively. At a higher dose of Sn, electron
trapping sites are introduced, which deteriorate the
charge transport properties and increase absorption
by the TiO2 layer. The physical origin of decreased
electron mobility at a high Sn content can also
bejustified based on the electronic structural changes
obtained from the DFT calculations. Since the
relaxation time is fixed, the mobility depends on the
effective mass of the charge carriers which, in turn,
relies on the VBM and CBM of the E−k diagram. From
the DOS, shown in Figure 2, it is clear that the
contribution of the 5s orbital of Sn near CBM is flat
compared to the contributions made by the 3d orbital
of Ti and the 2p orbital of O. As the Sn concentration
increases, it flattens the CBM even
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more, thereby increasing the effective mass of the
electrons and decreasing the mobility. Consequently,
the PCE decreases when the Sn content exceeds
3.125 mol %.33 The corresponding incident-photon-
to-electron conversion efficiency (IPCE) spectra are
shown in Figure 5b, where the Sn-doped TiO2 devices
exhibit a higher IPCE for the wavelengths between
300 and 900 nm. Toward the short wavelength
region, a majority of the incoming photons are
absorbed by TiO2 and the thick glass/FTO (fluorine-
doped tin oxide), which forms the front contact,
without reaching the perovskite layer. At
wavelengths above 800 nm, the energy of the
incident photons is less than the band gap of the
perovskite and therefore cannot generate excitons.
Although in practice, TiO2 with less than 3.125 mol %
Sn doping can yield a higher PCE, as demonstrated by
Cai et al.33 and Liao et al., 55 the DFT calculations at
low doping concentrations are currently limited by
our available computational resources. For example,
2 mol % Sn doping in TiO2 results in a supercell with
150 atoms by replacing 1 Ti atom, out of 50 Ti atoms,
with a single Sn atom. The computational resources
used in this work can however handle a maximum of
only 100 atoms.
The performance of PSCs also depends on the
thickness of the TiO2 layer, as displayed in Figure
6a−d. A thinner ETL facilitates electron extraction
from the perovskite/TiO2 interface and enhances the
PCE by yielding higher Jsc. The open-circuit
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voltage (Voc) remains nearly constant, indicating that

there is no leakage of the charge carriers as the thickness
of TiO2 is increased.56 Moreover, the thinner TiO2 layer is
more transparent to incoming solar radiation and offers
lower series resistance and defect densities, contributing
to the enhanced performance of the PSC device.
3.4. Doping TiO2 with Zn. Zinc (Zn), when used as a dopant,
modifies the electronic structure of TiO2, enhancing its
electrical conductivity. This leads to higher Jsc and PCE in
PSCs with Zn-doped TiO2 when compared to PSCs with
pristine TiO2. 34 The widespread use of Zn as a dopant
material for TiO2 is attributed to the low cost of Zn
precursors. Moreover, Zn doped TiO2 is found to have a
lower number of trap states when compared to undoped
TiO2 films.29 Here, for a given doping concentration, we
have compared the performance of PSCs with Sn-doped and Table S2 of the Supporting Information compare the
and Zn-doped TiO2 using DFT-extracted energy band gaps, current−voltage characteristics of PSCs with 4.17 mol % Sn-
carrier mobilities, and absorption spectra. Figure 7 shows and Zn-doped TiO2 films, having pristine TiO2 as the a PSC
the supercell (3 × 2 × 2), energy band diagram, and PDOS with 4.17 mol % Sn-doped TiO2 is 0.63% higher than that
of TiO2, doped with 4.17 mol % Zn, where Ueff = 10.8 eV obtained from a PSC with 4.17 mol % Zn-doped TiO2. The
has been used for the d-orbital of Zn. Choosing the U value corresponding IPCE plots are shown in Figure 8d.
as 10.8 eV yielded a band gap of 3.24 eV for pure ZnO,
which matched very closely with the experimentally 4. CONCLUSIONS
determined band gap of 3.25 eV, as demonstrated in our
In summary, we have accurately derived the device
previous study.57 The PDOS of Zn-doped TiO2 shows the characteristics of PSCs with pristine, Sn-doped, and Zn-
contribution of the 3dorbital of Zn, hybridized with the 2p- doped TiO2 as the ETL using the DFT-extracted absorption
orbital of O, to form the VBM. This pushes the VBM toward
spectrum, band gap, and carrier mobility of TiO2. The DFT
the higher energy, reducing the band gap to 2.89 eV for
calculations take into consideration the quantum-
4.17 mol % Zn-doped TiO2. The carrier mobilities are
mechanical properties of the ETL and provide a more
calculated using the CRTA method, with a relaxation time realistic absorption spectrum than the builtin spectrum in
of 10−10 s, and are listed in Table S1 of the Supporting
the SCAPS simulator. The current−voltage characteristics
Information. From Figure
of the PSC with pristine TiO2 showed that the absorption
8a,b, it is clear that for any given wavelength, the 4.17 mol
spectrum of TiO2, obtained from SCAPS, clearly
% Sn-doped TiO2 is less absorbing, with higher overestimates the solar cell performance. The DFT
transmittance than the Zn-doped counterpart. The Jsc, extracted spectrum, on the other hand, yields electrical
Voc, FF, and PCE of the PSC with Zndoped TiO2 are 20.15
characteristics that are in very good agreement with
mA/cm2 , 1.12 V, 0.73, and 16.44%, respectively. Figure 8c
experimental results reported in

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the literature. The excellent matching between the simulation
and experimental results can be attributed to the appropriate
choice of U values and relaxation time for the DFT-computed
absorption spectrum and carrier mobilities. A maximum PCE of
17.14% is achieved for 3.125 mol % Sn-doped TiO2, which is
3.44% higher than that of the PCE obtained with pristine TiO2
films. A higher concentration of Sn degrades the device
performance due to increased defect levels. The performance
ofthe solar cell, with varying thicknesses of pristine and Sndoped
TiO2, has also been investigated, with thinner TiO2 layers (∼20
nm) yielding the highest Jsc and PCE. Comparing the PCE between
4.17 mol % Sn- and Zn-doped TiO2 layers, it is clear that PSCs with
the Sn-doped ETL are slightly more efficient than those with the
Zn-doped ones. The combination of DFT calculations and device
simulations, as demonstrated in this study, can be further
extended to include other layers, organic molecular additives,
and metal dopants, paving the way for predicting the
performance of PSCs with quantum-mechanical accuracy.
■ ASSOCIATED CONTENT
Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.jpcc.1c02302.
Macrscopic charge carrier mobility calculations in TiO2 using
DFT; carrier mobilities of undoped and doped TiO2 calculated
with the CRTA method; calculation of optical properties of TiO 2
using DFT; PSC output characteristics obtained from SCAPS-1D
using DFT-extracted parameters of undoped and doped TiO2
(PDF)
■ AUTHOR INFORMATION
Corresponding Author
Mainul Hossain − Department of Electrical and
Electronic Engineering, University of Dhaka, Dhaka
1000, Bangladesh; orcid.org/0000-0001-9011-9029;
Email: mainul.eee@ du.ac.bd
Authors
Sadiq Shahriyar Nishat − Department of Physics, University of
Dhaka, Dhaka 1000, Bangladesh; orcid.org/0000-0003- 4236-
346X
Md. Jayed Hossain − Department of Electrical and Electronic
Engineering, University of Dhaka, Dhaka 1000, Bangladesh;
orcid.org/0000-0002-6685-7627
Faiyaz Elahi Mullick − Department of Electrical and Electronic
Engineering, University of Dhaka, Dhaka 1000, Bangladesh
Alamgir Kabir − Department of Physics, University of Dhaka,
Dhaka 1000, Bangladesh
Shaestagir Chowdhury − Department of Mechanical and
Materials Engineering, Portland State University, Portland,
Oregon 97201, United States
Sharnali Islam − Department of Electrical and Electronic
Engineering, University of Dhaka, Dhaka 1000, Bangladesh;
orcid.org/0000-0002-0218-7337 Complete contact information is
available at: https://pubs.acs.org/10.1021/acs.jpcc.1c02302
Author Contributions
∥S.S.N and M.J.H contributed equally to this work.
Notes
The authors declare no competing financial interest
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pubs.acs.org/JPCC Article
■ ACKNOWLEDGMENTS
No funding was received for this work. The authors thankfully
acknowledge the technical support from Fab Lab DU at the
University of Dhaka and the Bangladesh Research and Education
Network (BdREN) for providing the necessary computational
resources for this simulation study.
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