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A R T I C L E I N F O A B S T R A C T
Keywords: Recently, inorganic perovskite solar cells (PSCs) based on CsPbBr3 have triggered incredible interest due to the
CsPbBr3 demonstrated excellent stability against thermal and high humidity environmental conditions. However, the
Band offset power conversion efficiency (PCE) of the CsPbBr3-based PSCs is still lower than that of the organic-inorganic
CsPbIBr2
hybrid one, because of the large band gap and serious charge recombination at the interface or inside the de
Bilayer absorption scenario
vice. Here, the working mechanism of the devices with normal n-i-p planar structure is modeled and investigated
using SCAPS 1D simulation software. The simulation results state that the proper band structure of PSCs is crucial
to carrier separation and transport. The high interface recombination, originated from the large band offsets of
the electron transport material (ETM)/absorber and absorber/hole transport material (HTM) respectively, can be
effectively diminished with the continuous gradient junction design of the absorber, and a PCE of 11.58% is
obtained with a high open-circuit voltage (VOC) of 1.68 V. Moreover, by building a heterojunction bilayer ab
sorption scenario of CsPbIBr2/CsPbBr3 and employing ZnOS and Cu2ZnSnS4 films as the ETM and HTM
respectively, the PCE of PSCs is further increased to 15.89%, caused mainly by the enhancement in short-current
density (JSC). Moreover, reducing the interface defect density is also very important to improve the performance
of PSCs. These results will provide theoretical guidance for improving the performance of the CsPbBr3-based
PSCs.
1. Introduction CsPbBr3 shows outstanding stability against thermal and high humidity
environmental conditions (Chen et al., 2018; Duan et al., 2019; Liang
In recent years, the advances of all organic-inorganic hybrid perov et al., 2017), and is emerging as one of the most promising candidates in
skites have drawn tremendous attention in the photovoltaics community the field of photovoltaic, especially for fabricating tandem solar cells.
due to their outstanding photoelectric properties, including high ab The carrier mobility of CsPbBr3 single crystal is up to 2000 cm2V− 1s− 1,
sorption coefficients, low exciton binding energies, long carrier diffusion higher than 77.9 cm2V− 1s− 1 for nanosheet films (Song et al., 2017; Yang
lengths, high carrier mobilities, and tunable bandgaps (Lee et al., 2012; et al., 2018). Hodes et al. (Kulbak et al., 2015) first confirmed the stable
Stranks et al., 2013; Xiao et al., 2017; Shi et al., 2017, 2018). Within the fabrication of CsPbBr3 PSCs with a promising PCE of 5.95% using Spiro-
past decade, the power conversion efficiency (PCE) of the perovskite OMeTAD (2,2′ ,7,70-tetrakis(N,N-p-dimethoxy-phenylamino) − 9,90-
solar cells (PSCs) witnessed a dramatic improvement from 3.8% (Kojima spirobifl-uorene) as hole transport material (HTM). Liang et al. (Liang
et al., 2009) to 25.2% (https://www.nrel.gov/pv/insights/assets/pdfs/ et al., 2016) replaced the traditional metal electrode with carbon,
cell-pv-eff-emergingpv.pdf). Despite the rapid development in PCE, the yielding a champion PCE of 6.7% in ambient environment. Wang’s
intrinsic volatility and thermal instability of the organic components group (Wang et al., 2018) fabricated high quality CsPbBr3 films using a
hinder the commercialization of organic-inorganic hybrid PSCs (Juarez- novel SCG (solvent-controlled growth) method and obtained a high PCE
Perez et al., 2016, 2018; Shan et al., 2019). Replacing the A-site organic of 9.81%. Tang’s group (Zhao et al., 2019) performed interfacial engi
ions with inorganic ions (such as Cs+) is an effective solution to the neering on CsPbBr3-based solar cells, boosting the efficiency to 10.6%.
instability issue of PSCs. And among the Cs-based inorganic perovskites, Tong et al. (Tong et al., 2019) suggested a phase transition induced (PTI)
* Corresponding author.
E-mail address: chysh2003@zzu.edu.cn (Y. Chen).
https://doi.org/10.1016/j.solener.2020.09.003
Received 16 June 2020; Received in revised form 17 August 2020; Accepted 2 September 2020
Available online 8 September 2020
0038-092X/© 2020 International Solar Energy Society. Published by Elsevier Ltd. All rights reserved.
S. Ullah et al. Solar Energy 209 (2020) 79–84
technique by utilizing the derivative phases, to fabricate high-quality + Eg,HTM)), respectively. The band offsets at the interfaces can be
CsPbBr3 films and succeeded in boosting the recorded PCE of n-i-p adjusted by varying χ absorber of the absorber and keeping Eg constant in
structure PSCs up to 10.91%. Table S1 displays a summary of the device simulation. The impact of the χ absorber on the JSC, VOC, FF and PCE of the
architecture and performance of the previously reported CsPbBr3-based cells is depicted in Fig. 1. The enhanced performance is obtained for the
PSCs. devices with χ absorber of 3.5–3.7 eV. Fig. 2 exhibits the energy band di
However, the PCE of the CsPbBr3-based PSCs is still lower than that agrams of the PSCs under short-circuit condition with χ absorber. When
of the organic-inorganic hybrid one, because of the large band gap (2.3 low value (3.3 eV) of χ absorber is implemented, a high cliff with value of
eV) and serious charge recombination at the interface or inside the de ΔEC = 0.7 eV is formed at the ETM/absorber interface, and a low cliff is
vice. To further enhance the performance of the CsPbBr3-based PSCs, it simultaneously observed at the absorber/HTM interface. With the in
is necessary to design the proper band structure to improve carrier crease of χ absorber, ΔEC decreases and ΔEV increases, and at χ absorber =
separation and transport and reduce the charge recombination. For this 3.6 eV, ΔEC and ΔEV are comparable. The cliff does not impede photo-
purpose, device simulation is employed for providing deep insight into generated electron and hole flow toward front and back electrodes
exploring the relationship between material properties and the perfor respectively, and JSC is almost constant with increasing χ absorber as
mance of the device (Fu et al., 2015; Wu et al., 2016; Ho-Baillie et al., shown in Fig. 1. The activation energy (Ea) for carrier recombination is
2019; Ma et al., 2017; Minemoto and Murata, 2014, 2015). Here, we associated with χ absorber. Ea,front (represented by Eg,absorber-ΔEC) at ETM/
employed a Solar Cell Capacitance Simulator-one dimension (SCAPS- absorber interface increases with the increasing in χ absorber, but the Ea,
1D, ver.3.3.07), developed by the University of Gent Belgium, for the back (Eg,absorber-ΔEV) at absorber/HTM interface decreases. Both of them
modeling of PSCs. The standard AM1.5G illumination was introduced to are lower than Eg,absorber, suggesting that the interface recombination is
examine the effects of interface properties, such as the band offset and mainly responsible for the recombination mechanism of the device,
interface defect density, on the photovoltaic performance of PSCs. The which directly correlates with VOC. Fig. 3 shows the variation of
article will provide useful guidance on optimum design for processing recombination current at interface (Jinterface) and absorber bulk (Jbulk) of
high-performance CsPbBr3-based PSCs in the future. PSCs with forward bias. Jbulk caused by Shockley-Read-Hall recombi
nation mechanism is lower than Jinterface, indication that interface
2. Device simulation parameters recombination dominates the recombination process. With the increase
of the forward bias, the built-in electric field strength in absorber de
The structure and energy level diagrams of the PSCs for the simu creases, leading to a rapid increase in Jbulk and Jinterface, especially for
lation analysis is FTO/ETM/absorber/HTM/Au, as shown in Fig. S1, and the PSCs with higher ΔEC or ΔEV. Thus, VOC reaches the maximal value
the parameters of the device are summarized in Table S2. For the at χ absorber = 3.6 eV, where Ea,front approximately equals to Ea,back. In
reference PSCs, TiO2, Spiro-OMeTAD and CsPbBr3 are used as the contrast to VOC, FF decreases with increasing χ absorber, and achieves the
electron transport material (ETM), HTM and absorber, respectively. The minimum at χ absorber = 3.6 eV. Therefore, tuning the band offsets of PSCs
defects in the three layers are all set to be in the neutral single distri is essential to obtain a higher VOC.
bution, and the defect energy level is located in the center of the The ideal situation for the optimization of photovoltaic performance
bandgap. The defect density (Nt,bulk) of CsPbBr3 is calculated using the is to completely remove the cliff formed at the interface, in other words,
following relation, to maintain Ea = Eg,absorber. Previous reports in this field suggest that the
band levels of CsPbBr3 film can be tuned slightly with the homogeneous
Nt,bulk = 1/(τσ Vth )
doping of foreign ions (Li et al., 2018; Duan et al., 2018; Tang et al.,
2019; Zhao et al., 2019). So, a continuous gradient junction design
Where τ is charge carrier lifetime, σ (10− 15 cm2) is capture cross-section
originated from the inhomogeneous doping is an effective way to reduce
of electron/hole, and Vth (107 cm/s) is the thermal velocity of electron/
the interface recombination. Qiao et al. (Qiao et al., 2019) evaluated
hole respectively. The value of τ is set to 10 ns, and the mobility of
several guest ions in a Cs0.1FA0.9PbI3 crystal and found that the In3+ and
electron and hole is 10 cm2V− 1s− 1, following the literatures (Liu et al.,
Sb3+ cations may be inhomogeneously doped into the perovskite, and an
2019; Li et al., 2017; Haruta et al., 2019). The values used for the
optimized band alignment and a best PCE of 21.04% are achieved. Here,
interface defects are as follows: Defect type is neutral and density (Nt,
13 three continuous gradient junction cases of absorber are investigated
interface) is 1 × 10 cm− 3, energetic distribution is Gaussian, charac
and compared to the reference cell, where χ absorber changes linearity to
teristic energy is 0.1 eV, located above the top of valence band EV at 0.6
separately or simultaneously eliminate the band offsets of ETM/perov
eV. We have taken a constant illumination of 1000 W/m2 at AM 1.5G
skite and HTM/perovskite. Fig. 4a displays the energy band diagrams of
and a constant temperature at 300 K to run the simulation. The ab
PSCs with and without continuous gradient design. For the reference
sorption coefficient (α) calculated using the following equation,
cell, χ absorber is fixed at 3.3 eV. For the PSC with the gradient design of
( )1/2
α = Aα hν⋅Eg case 1, χ absorber decreases linearly from 3.3 eV to 3.15 eV along the
thickness direction of the absorber, and ΔEV = 0.0 eV (χ absorber + Eg,
Where the pre-factor value Aα is 105 for both TiO2, ZnOS, Spiro-
OMeTAD and Cu2ZnSnS4, and 3 × 105 for CsPbIBr2 and CsPbBr3.
Using SCAPS-1D, we have calculated short-circuit current density (JSC), 8.10 1.25
76 6.7
VOC, Fill Factor (FF) and PCE.
8.08 1.20
JSC (mA/cm 2)/V OC (V)
74 6.6
3. Results and discussion
FF (%) /PCE (%)
8.06 1.15
72 6.5
The band offset between ETM/absorber and absorber/HTM layers
8.04 1.10
plays a vital role in the carrier recombination at the interface, which 70 6.4
affects the value of VOC (Minemoto and Murata, 2015; Zhou et al.,
8.02 1.05
2016). Electron affinity (χ ) refers to the energy difference between the 68 6.3
free electron energy level of vacuum and the bottom energy level of
8.00 1.00 66 6.2
conduction band (EC). The band offsets of EC and EV (valence band) at 3.3 3.4 3.5 3.6 3.7 3.8 3.9
ETM/absorber and absorber/HTM interfaces are defined using ΔEC Electron affinity (eV)
(ΔEC = χ ETM − χ absorber) and ΔEV (ΔEV = (χ absorber + Eg,absorber) − (χ HTM
Fig. 1. Impact of χ absorber on the performance of solar cells.
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S. Ullah et al. Solar Energy 209 (2020) 79–84
81
S. Ullah et al. Solar Energy 209 (2020) 79–84
4. Conclusions
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S. Ullah et al. Solar Energy 209 (2020) 79–84
Acknowledgments
This work was supported by the Program for the Innovation Team of
Science and Technology in University of Henan of China (No.
20IRTSTHN014).
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