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Received: 17 November 2021 Revised: 15 February 2022 Accepted: 18 February 2022
DOI: 10.1002/est2.331

SPECIAL ISSUE ARTICLE

Highly efficient tin oxide-based colloidal lead sulfide

quantum dot solar cell

Ajay Kumar1 | Pushkar Gahlaut1 | Neha Gupta2

1
Department of Electronics and
Communication, Jaypee Institute of
Abstract
Information Technology, Noida, India This work presents the assessment of tin oxide (SnO2) electron transport layer
2
Department of Applied Science and (ETL)-based quantum dot solar cell for improved efficiency (>20%). The pro-
Humanity, ADGITM, New Delhi, India
posed solar cell consists of a solid layer of lead sulfide (PbS) treated with PbS-
Correspondence TBAI (tetrabutylammonium iodide) as absorber layer and PbS CQD treated
Ajay Kumar, Department of Electronics with 1,2-ethanedithiol (PbS-EDT) as hole transport layer (HTL). The high level
and Communication, Jaypee Institute of
Information Technology, Noida, India.
of efficiencies is achieved by varying the doping concentration of ETL and
Email: [Link]@[Link] HTL, which affect the mobility of carriers (both electrons and holes). The opti-
Neha Gupta, Department of Applied mization is carried out with a doping concentration (for ETL and HTL) of
Science and Humanity, ADGITM, New 1  1019 cm 3. The said doping reflected >20% conversion efficiency. PCE, fill-
Delhi.
Email: [Link]@[Link]
factor (FF), Voc, and Jsc were analyzed for all the performed variations.

KEYWORDS
CQD, efficiency, ETL, HTL, SnO2, solar cell

1 | INTRODUCTION solar cells. Concerning other solar cell technologies, the

recombination of electrons and holes in a quasi-neutral
The world today looks towards renewable sources of region (where the electric field is zero) is one of the
energy to meet the ever-growing demands of the human prominent factors for the decline in the performance of
population. This need drives us towards innovative solu- colloidal QD solar cells (CQD). One method utilized by
tions and new ways of producing energy. One such scientists to reduce this is to align QDs of different sizes
renewable is solar energy which helps us convert sunlight on top of one another in a technique called graded band
into usable electricity. As a CO2 and emissions-free alignment. One of the most distinguished structures
power source, the environmental impacts of solar power prominent features of colloidal QDs has a tunable
are significantly less than other conventional power gen- bandgap according to the size of the QD.4-6 This property
eration methods.1 The only thing of note is the unique has an immense impact on the design as by changing the
materials required to produce solar panels. The search bandgap; efficiency can be improved. They can be man-
for these materials is propelled for low-cost, durable, and ufactured using solutions processing which broadens the
highly efficient elemental materials. Cost, lifetime, and scope of applications such as flexible photovoltaic
efficiency are the golden triangle elements, and various (PV) cells, LED screens, photodetectors.7 The CQDs also
technologies with different properties are traversed. utilize the solar spectrum 20% more efficiently as the tun-
To get photovoltaics to have better performance, able bandgap of CQDs allows them to use the infrared
researchers look towards quantum dots (QD).2 These photon.8 Impressive progress has been achieved, and
semiconductors are less than the exciton Bohr radius in power conversion efficiency (PCE's) exceeding 10% have
size. Its simple fabrication methods make it a desired been materialized for CQDs.
choice.3 The carrier recombination in the charge-neutral These devices suffer from a major downside: carrier
region is a major factor that hampers the efficiency of QD recombination in the charge-neutral region. On the

Energy Storage. 2022;e331. [Link]/journal/est2 © 2022 John Wiley & Sons Ltd. 1 of 8
[Link]
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2 of 8 KUMAR ET AL.

depletion layer at the interface of the electron transport Figure 1.17,18 The proposed device uses ITO as the front
layer (ETL)/absorber layer, the electric field extracts the contact upon which AM1.5G illumination of
majority of carriers.9 While in the remote region where 100 mW/cm2 is cast.10 It will allow entering the maxi-
the electric field is zero (quasi-neutral region), the collec- mum illumination in the solar cell. The extraction of
tion of carriers depends on diffusion.10 The probability of electrons is increased using SnO2 as an electron collect-
recombination of the carriers in this region is higher, lim- ing layer. ZnO is used to replace MZO and SnO2 used in
iting the device's efficiency. However, the charge collec- the published work,19 and this work is compared due to
tion simultaneously competes with charge recombination
and an effective way of increasing the charge collection is
to increase the doping densities of the transport layers. T A B L E 1 Simulation parameter for quantum dot solar cell
The QD we are working with is PbS (lead sulphide) in with SnO2 as electron transport layer (ETL)12,16,19,29,30
this work treated with tetrabutylammonium iodide.11
Parameters PbS-EDT PbS-TBAI SnO2
Lead chalcogenides (PbSe or PbS) CQDs can be tuned to
have a range of bandgap energy varying (0.5-1.6 eV) by Thickness (nm) 50 230 80
controlling particle size.12-14 The stimulation gives us Eg (eV) 1.14 1.14 3.20
insights into determining the actual physics, which will χ (eV) 3.9 4.0 3.9
help us to identify the device's efficiency. It also provides εr 20 20 9
us with accurate information regarding the carrier
Nc (cm 3) 1 1019 1  1019 2.2  1018
dynamics.15 In the proposed device, ITO is used as front
Nv (cm 3) 1  1019 1  1019 1.8  1019
contact, SnO2 as ETL, and gold as back contact.16
μn (cm2 V 1
s 1) 2.0  10 4
2.0  10 2
2.0  101
μp (cm V 2 1 1
s ) 2.0  10 4
2.  10 2
1.0  101
2 | DEVICE DESIGN, ND (cm 3) 1  1014 1  1015 1  1017
M E T H O DO L O G Y , A N D NA (cm 3) 1  1016 1  1015 0
CALIBRATION
Note: Eg, energy band gap; εr, relative permittivity; μp, hole mobility; μn,
electron mobility; NA, acceptor concentration; ND, donor concentration; Nc,
The basic structure of the proposed solar cell device is conduction band density of states; Nv, valence band density of states; χ,
stimulated on SCAPS-1D software and shown in electron affinity.

F I G U R E 1 (A) Proposed
device with electron transport
layer (ETL). (B) SCAPS-1D
device structure. (C) Calibration
of J-V characteristics
experimental data19 with
simulated data
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KUMAR ET AL. 3 of 8

its high mobility, ambient stability, and low-temperature of charges. Furthermore, the calibration of experimental
endurance. A highly conductive ETL is required for effi- data19 with simulated data is performed to show the
cient charge transfer, and reducing recombination. There simulation accuracy. From Figure 1C, it is reflected that
are several efficient methods for SnO2 doping to improve the simulated data are well calibrated with
the properties of the ETL/perovskite interface.16,20,21 It is experimental work.
used to extract light-generated electrons. It is 80 nm wide. The metal work-function of contacts is 5.1 and 4.7 eV
The next layer is the absorber layer, which is 230 nm for Gold (Au) and indium tin oxide (ITO), respec-
wide and the widest to generate the maximum number of tively.26-28 Electron surface recombination velocities are
electron-hole pairs generated with the absorbed illumina- kept at 105 cm s 1 and 107 cm s 1 for the back and front
tion. It is made up of PbS QD22 crystals which is treated end, respectively. The physical parameters of the differ-
with tetrabutylammonium iodide (PbS-TBAI).23,24 A ent layers used in the suggested device are provided in
layer of PbS QD treated with PbS-EDT for the extraction Table 1. All parameters of interface defects are depicted
of holes is used.10 It creates an electric field between the in Table 2.
bulk material and the PbS-EDT to collect holes. It is
50 nm wide. Gold (Au) is used as a back contact.25 The
ETL and hole transport layer (HTL) have a significant 3 | RESULTS A ND DISCUSSION
impact on efficiency as they enhance the transportation
The actual stimulation values of the absorption coeffi-
cient of PbS are shown in Figure 2A. While Figure 2B
TABLE 2 Interface defects parameter used in simulation31 shows the value of the absorption coefficient of SnO2.
PbS-EDT/PbS- PbS-TBAI/ SnO2 has very low resistivity as compared to MZO. It is
Parameters TBAI interface ETL interface attributed to higher mobility of electrons, that is,
Type of defect Neutral Neutral
23 cm2 V 1 s 1, compared to low electron mobility
5.0 cm2 V 1 s 1 in MZO. This change of material defines
Electrons capture 1.2  10 13
1.0  10 19
the difference in results of the two devices. At the same
cross-section
(cm 2) time, the Voc and fill-factor (FF) remain to an extent the
short circuit current density and efficiency show drastic
Holes capture cross- 1.2  10 13
1.0  10 19

section (cm 2) change.

Furthermore, the entire workflow is carried out to
Energy distribution Single Single
examine the effect of donor and acceptor doping concen-
The energy level of Above Ev Above Ev
tration in ETL and HTL of the cell. The donor and accep-
the defect (Et)
tor concentrations simultaneously vary from
Energy wrt Et 0.5 0.6
1  1016 cm 3 to 1  1019 cm 3 in four parts, ensuring
reference (eV)
none of the other parameters change. The absorber layer
Effective density 1  1016 2  1014 doping is not touched during this stimulation and is kept
(cm 2)
constant 1  1015 for both acceptor and donor.

F I G U R E 2 (A) PbS
absorption coefficient, and
(B) absorption coefficient
of SnO2
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4 of 8 KUMAR ET AL.

F I G U R E 3 (A-D) The energy band diagrams of all four batches of hole transport layer (HTL) doping densities (cm 3) under AM1.5G
100 mW/cm2 illumination.19

The energy band diagrams (EBD) are obtained at

thermal equilibrium. The carrier dynamics for all four
steps are reflected in Figure 3A-D. The left side section of
each graph from 0-0.05 μm is PbS-EDT, the middle from
0.05 to 0.28 μm is PbS-TBAI, and the right side from 0.28
to 0.36 μm is SnO2. As evident by observation the
maximum energy increases from 0.96, 1.02, and 1.08 eV
and finally to 1.14 eV for PbS-EDT (HTL) as we increase
the doping density32 from 1  1016 cm 3 to 1  1019
cm 3, respectively. Also, in negative energy value (mag-
nitude) increases from 3.06 , 3.12, 3.18 to 3.24 eV
as the doping density is increased. The energy line (top-
most black) at SnO2 flattens vs the distance as we
increase the density. From EBD, it is depicted that, at the
PbS-TBAI/SnO2 interface, an offset is observed in the
conduction band.
The quantum efficiency (QE) of all four batches is
evaluated and plotted against wavelength as shown in FIGURE 4 The quantum efficiency of all four batches w.r.t
Figure 4. The graph consequently shifts upwards with the wavelength
gradual shift in doping values in the QE values. As seen
for the 1  1019 cm 3 doping density device performs the
improvement (95%) owing to high electron mobility of decline in QE (%) of all the devices regardless of the dop-
SnO2 as ETL layer and slightly besting out the ing density as the wavelength of light increases from
1  1018 cm 3 device in terms of QE. There is a steady 400 to 900 nm and then decreases till 1000 nm and then
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KUMAR ET AL. 5 of 8

sharply reduces due to the QE cut-off at (1.24/Eg), that is, donor density of HTL and ETL, as evident from the
1.08 μm (1080 nm) for a PbS CQD solar cell. increase in the Voc value. It reflects when increasing the
Figure 5A depicts the Jsc as a function of voltage. The density, the electric field is strengthening, leading to
point where the current crosses the zero axis in extraction of more charge carriers (electrons in case of
Figure 5A of the J-V curve gives us the Voc (open circuit ETL, and conversely for HTL, holes). The highest poten-
voltage). Beyond this voltage, the absence of the PV effect tial divided by electric field value is with the doping of
can be observed. Below Voc point, the magnitude of the 1  019 cm 3 and the higher slope of the graph validates
external electric field of different semiconducting inter- it. The Jsc value increases from 30.24 to 31.71 mA/cm2.
faces is lower than the internal electric field. This field Figure 5B reflects the change in mobility w.r.t doping
helps in the collection of carriers from electron-hole concentration in HTL. From Figure 5B, it is observed that
pairs. The enhanced built-in potential and an increased with the doping concentration mobility is increases
electric field result from an increase in acceptor and which leads to performance of the solar cell.

F I G U R E 5 (A) Short
circuit current density (Jsc) as a
function of open-circuit voltage
for different doping densities.
(B) Variation of mobility as a
function of different doping
densities for hole transport
layer (HTL)

F I G U R E 6 Solar cell
performance metrics; (A) Voc,
(B) Jsc, (C) fill-factor (FF), and
(D) PCE; for different doping
densities
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6 of 8 KUMAR ET AL.

Furthermore, the four plots of Figure 6A-D signify shown in Figure 6C. The lower value of FF signifies low
that all the PV performance parameters improve signifi- conductivity, resulting in reduced conduction of carriers.
cantly with the variation in density. As previously dis- The result validates that the devices outperform the lower
cussed, the strong electric field at high doping levels doped devices significantly at higher doping densities as
leads to higher performance of Voc, Voc increases with higher PV performance is observed at high doping levels.
doping density for the proposed solar cell as shown in PCE measures the fraction of incident power that is
Figure 6A. Thus, a higher value of Voc leads to the high converted into electricity. The PCE value starts at 12.35%
performance of the PV device. Figure 6B reflects the solar for the calibrated device. Whereas for the 1  1016 doping
cell performance in terms of short circuit current density density, the efficiency is 11.07%. After varying the values
(Jsc). From Figure 6A, it is observed that its value is of densities, the final efficiency comes out 9.34% higher
higher for a higher value of doping density. However, Jsc than the initial steps. The best performance is attained
performance is improved (30.24 [mA/cm2]) for lower with the doping concentration of 1  1019 cm 3, while
doping density (1  1016 cm 3) as compared to other PV very difficult in fabricating such a device would give
devices. FF measures the squareness of the current- 20.41% efficiency as reflected in Figure 6D.
voltage curve. The total series resistance is derived by the All the stimulated device performance parameters
sum of individual resistivities of the semiconducting (illustrated in Table 3) of the proposed device (SnO2-
layers. The FF value increases from 57.33% to 81.54% at based ETL device) are calculated in terms of Jsc, FF, Voc,
the minimum and maximum value of doping density, as and PCE and simultaneously compared and calibrated

T A B L E 3 Proposed solar cell

Doping density
(both ETL and HTL) Voc (V) Jsc (mA/cm )
2
FF (%) PCE (%) performance matrix

1  10 16 cm 3
0.638 30.24 57.33 11.07
1  10 17 cm 3
0.702 31.006 68.63 14.94
1  10 18
cm 3
0.752 31.5 77.46 18.37
1  10 19
cm 3
0.789 31.71 81.54 20.41

F I G U R E 7 Performance
matrix of SnO2-based ETL
device comparison with existing
work19
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KUMAR ET AL. 7 of 8

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