Theoretical analysis and performance optimization of Cs<sub>2</sub>AgBiI<sub>6</sub> solar cells with dual hole transport layers

WANG Jiwei; TIAN Hanmin; WANG Yuerong; CAO Rui; XU Wu

doi:10.7498/aps.74.20241361

Abstract

Double perovskite materials have received significant attention in the photovoltaic field due to their low cost, environmental friendliness, and lead-free composition, which make them ideal candidates for next-generation solar cell applications. In this work, the photovoltaic performance of solar cells using Cs₂AgBiI₆ as the light-absorbing layer is systematically investigated through simulations using Silvaco ATLAS software. Based on the previously reported single hole transport layer device architecture, namely ITO/ZnO/Cs₂AgBiI₆/HTL/Au, a new dual hole transport layer structure ITO/ZnO/Cs₂AgBiI₆/HTL1/HTL2/Au is proposed. Different dual hole transport layer combinations are explored, and their influence on the internal physical mechanism and the device performance are analyzed and optimized in detail. The simulation results show that the devices using Cu₂O/NiO and NiO/Si respectively as dual hole transport layer significantly improve charge extraction and generate a negative electric field at the interface, thereby reducing recombination losse and accelerating the transport of hole carriers. These two configurations exhibit substantially higher efficiencies than those configurations with a single hole transport layer, confirming the advantages of the dual hole transport layer structure. Additionally, devices using Cu₂O/CZTS and MoO₃/CZTS as dual hole transport layer show better performance than the reference structure using Spiro-OMeTAD/CZTS, indicating the potential for further improvement by optimizing material selection and layer properties. Of the various dual hole transport layer combinations tested, the structure utilizing Cu₂O/CZTS achieves the highest simulated power conversion efficiency (PCE) of 22.85%. By optimizing the thickness of each functional layer, the efficiency can be further increased to 25.62%, and the optimal layer thickness is determined to be 40 nm for ZnO, 850 nm for Cs₂AgBiI₆, 140 nm for Cu₂O, and 150 nm for CZTS. Furthermore, the effects of environmental and material parameters, such as temperature and hole transport layer doping concentration, on device performance are investigated. This study lays a theoretical foundation for the design and enhancement of double perovskite solar cells. By demonstrating the potential that the dual hole transport layer structures can significantly improve device efficiency, their value in advancing environmentally friendly and lead-free photovoltaic technologies becomes very prominent. The insights gained from this research pave the way for developing high-performance double perovskite solar cells with optimized architectures and material properties.

Keywords:

Authors and contacts

1.
School of Electronics and Information Engineering, Hebei University of Technology, Tianjin 300401, China
2.
Tianjin Key Laboratory of Electronic Materials and Device, Hebei University of Technology, Tianjin 300401, China

Corresponding author: TIAN Hanmin, tianhanmin@hebut.edu.cn

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References

[1]	Hasan S A U, Zahid M A, Park S, Yi J 2024 Sol. RRL 8 2300967 Google Scholar
[2]	Cheng M, Jiang J, Yan C, Lin Y, Mortazavi M, Kaul A B, Jiang Q 2024 Nanomaterials 14 391 Google Scholar
[3]	Liu H R, Zhang Z H, Yang F, Yang J E, Grace A N, Li J M, Tripathi S, Jain S M 2021 Coatings 11 1045 Google Scholar
[4]	Machin A, Marquez F 2024 Materials 17 1165 Google Scholar
[5]	万婷婷, 朱安康, 郭友敏, 汪春昌 2017 材料导报 31 16 Google Scholar Wan T T, Zhu A K, Guo Y M, Wang C C 2017 Mater. Rev. 31 16 Google Scholar
[6]	Zhai M, Chen C, Cheng M 2023 Sol. Energy 253 563 Google Scholar
[7]	Meyer E, Mutukwa D, Zingwe N, Taziwa R 2018 Metals 8 667 Google Scholar
[8]	Yuan Y, Yan G, Hong R, Liang Z, Kirchartz T 2022 Adv. Mater. 34 2108132 Google Scholar
[9]	Zhao X G, Yang J H, Fu Y, Yang D, Xu Q, Yu L, Wei S H, Zhang L 2017 J. Am. Chem. Soc. 139 2630 Google Scholar
[10]	Ji F, Boschloo G, Wang F, Gao F 2023 Sol. RRL 7 2201112 Google Scholar
[11]	chrafih Y, Al Hattab M, Rahmani K 2023 J. Alloys Compd. 960 170650 Google Scholar
[12]	Amraoui S, Feraoun A, Kerouad M 2022 Inorg. Chem. Commun. 140 109395 Google Scholar
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Cited By

图 1 (a) Cs₂AgBiI₆单HTL钙钛矿太阳能电池; (b) Cs₂AgBiI₆双HTL钙钛矿太阳电池结构

Figure 1. Device structure of (a) Cs₂AgBiI₆-based single HTL perovskite solar cell and (b) Cs₂AgBiI₆-based dual HTLs perovskite solar cell.

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图 2 基于Cs₂AgBiI₆的不同单空穴传输层太阳能电池的J-V参数曲线

Figure 2. J-V parameter curves for different single HTL solar cells based on Cs₂AgBiI₆.

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图 3 基于Cs₂AgBiI₆的不同双空穴传输层太阳能电池的J-V参数曲线

Figure 3. J-V parameter curves for different dual HTLs solar cells based on Cs₂AgBiI₆.

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图 4 具有不同双空穴传输层的Cs₂AgBiI₆太阳能电池界面电场　(a) Cu₂O/NiO; (b) NiO/Si; (c) MoO₃/Cu₂O; (d) MoO₃/Spiro

Figure 4. Electric fields at the interfaces of Cs₂AgBiI₆ PSCs with different HTL combinations: (a) Cu₂O/NiO; (b) NiO/Si; (c) MoO₃/Cu₂O; (d) MoO₃/Spiro.

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图 5 具有不同双空穴传输层的Cs₂AgBiI₆太阳能电池复合率　(a) Cu₂O/NiO; (b) NiO/Si; (c) MoO₃/Cu₂O, (d) MoO₃/Spiro

Figure 5. Charge recombination rate of Cs₂AgBiI₆ PSCs with different HTL combinations: (a) Cu₂O/NiO; (b) NiO/Si; (c) MoO₃/Cu₂O; (d) MoO₃/Spiro.

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图 6 具有不同双空穴传输层的Cs₂AgBiI₆太阳能电池的能带图　(a) NiO/Si; (b) Cu₂O/NiO.

Figure 6. Energy band diagram of Cs₂AgBiI₆ PSCs with different HTL combinations: (a) NiO/Si; (b) Cu₂O/NiO.

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图 7 基于Cs₂AgBiI₆的不同HTL/CZTS双空穴传输层太阳能电池的J-V参数曲线

Figure 7. J-V parameter curves for different HTL/CZTS solar cells based on Cs₂AgBiI₆.

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图 8 Cs₂AgBiI₆太阳能电池中(a) Spiro/CZTS, (b) MoO₃/CZTS, (c) Cu₂O/CZTS双空穴传输层界面上的电场, 以及(d) Spiro/CZTS, (e) MoO₃/CZTS, (f) Cu₂O/CZTS双空穴传输层的复合率

Figure 8. Electric fields at the interfaces of Cs₂AgBiI₆ PSCs with different HTL combinations: (a) Spiro/CZTS; (b) MoO₃/CZTS; (c) Cu₂O/CZTS. Charge recombination dynamics of Cs₂AgBiI₆ PSCs with different HTL combinations: (d) Spiro/CZTS; (e) MoO₃/ CZTS; (f) Cu₂O/CZTS.

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图 9 Cu₂O/CZTS双空穴传输层Cs₂AgBiI₆太阳能电池的能带图

Figure 9. Energy band diagram of Cs₂AgBiI₆ solar cell with Cu₂O/CZTS dual hole transport layer.

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图 10 (a)电子传输层ZnO、(b)钙钛矿层Cs₂AgBiI₆、双空穴传输层(c) CZTS和(d) Cu₂O厚度对钙钛矿太阳能电池V_OC, J_SC, FF和PCE的影响

Figure 10. Effects of thicknesses of (a) electron transport layer ZnO, (b) perovskite layer Cs₂AgBiI₆, (c) hole transport layer Ⅰ CZTS, (d) hole transport layer Ⅱ Cu₂O on V_OC, J_SC, FF and PCE of dual HTLs perovskite solar cell.

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图 11 基于Cs₂AgBiI₆的Cu₂O/CZTS钙钛矿太阳能电池优化前后J-V参数曲线

Figure 11. J-V parameter curves before and after optimization of Cu₂O/CZTS dual HTLs perovskite solar cell based on Cs₂AgBiI₆.

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图 12 空穴传输层CZTS和Cu₂O浓度对Cs₂AgBiI₆钙钛矿太阳能电池的(a) J_SC, (b) V_OC, (c) PCE和(d) FF的影响

Figure 12. Effects of the concentrations of the CZTS and Cu₂O on (a) J_SC, (b) V_OC, (c) PCE and (d) FF of the Cs₂AgBiI₆ perovskite solar cell.

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图 13 电池输出参数随HTL空穴迁移率的变化

Figure 13. Variations of solar cell output parameters with HTL hole mobility.

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图 14 温度对Cs₂AgBiI₆钙钛矿太阳能电池的(a)V_OC, (b) J_SC, (c) PCE和(d)FF的影响　　

Figure 14. Effects of the temperature on (a) J_SC, (b) V_OC, (c) PCE and (d) FF of the Cs₂AgBiI₆ perovskite solar cell.

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表 1 太阳能电池不同层材料的参数

Table 1. Device parameters for different layers of the cells.

Parameter	ZnO	Cs₂AgBiI₆	Cu₂O	MoO₃	CZTS	Spiro-OMeTAD	NiO	P3HT	Si
Thickness/nm	50	800	50	50	100	200	100	50	50
Permittivity ε_r	9	6.5	7.5	12.5	9	3	10.7	3	11.9
Band gap/eV	3.3	1.6	2.17	3	1.4	2.2	3.8	1.7	1.12
Affinity/eV	4	3.9	3.2	2.5	3.8	3	1.46	3.5	4.17
N_C/(10¹⁸ cm^–3)	3.7	10.0	2.0	2.2	2.2	2.2	28.0	2000.0	250.0
N_V/(10¹⁸ cm^–3)	18.0	10.0	11.0	18.0	1.8	250.0	10.0	2000.0	180.0
N_D(10¹⁸ cm^–3)	1	0	0	0	0	0	0	0	0
N_A/(10¹⁵ cm^–3)	0	1	1000	1000	10000	1000	1000	1000	10
μ_n/(cm²·V^–1·s^–1)	100	2	200	25	100	2×10^–4	12	1.8×10^–3	1500
μ_p/(cm²·V^–1·s^–1)	25	2	80	100	12.5	2×10^–4	2.8	1.86×10^–2	480

DownLoad: CSV

表 2 不同单空穴传输层电池的输出参数

Table 2. Performance parameters of PSCs with various HTLs.

电池结构	V_OC/V	J_SC/(mA·cm^–2)	PCE/%	FF/%
FTO/ZnO/Cs₂AgBiI₆/Cu₂O/Au	1.096	23.02	21.17	83.91
FTO/ZnO/Cs₂AgBiI₆/MoO₃/Au	1.097	23.01	21.16	83.83
FTO/ZnO/Cs₂AgBiI₆/CZTS/Au	1.088	22.07	20.00	83.29
FTO/ZnO/Cs₂AgBiI₆/Spiro/Au	1.095	23.08	20.14	79.69
FTO/ZnO/Cs₂AgBiI₆/NiO/Au	1.095	23.00	20.64	82.10
FTO/ZnO/Cs₂AgBiI₆/P3HT/Au	1.070	23.04	17.91	72.65
FTO/ZnO/Cs₂AgBiI₆/Si/Au	1.055	22.00	17.18	74.02
ITO/ZnO/Cs₂AgBiI₆/Spiro/Au^[34]	1.08	24.20	21.72	83.14
ITO/ZnO/Cs₂AgBiI₆/Spiro/Au^[33]	1.08	23.74	20.31	79.28

DownLoad: CSV

表 3 不同双空穴传输层电池的输出参数

Table 3. Performance parameters of PSCs with dual HTLs.

Device structures	V_OC/V	J_SC/(mA·cm^–2)	PCE/%	FF/%
FTO/ZnO/Cs₂AgBiI₆/Cu₂O/NiO/Au	1.098	23.19	21.39	83.46
FTO/ZnO/Cs₂AgBiI₆/NiO/Si/Au	1.093	23.05	20.71	82.21
FTO/ZnO/Cs₂AgBiI₆/MoO₃/Cu₂O/Au	1.097	22.9	21.13	83.44
FTO/ZnO/Cs₂AgBiI₆/MoO₃/Spiro/Au	1.097	23.96	21.12	83.77

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表 4 不同HTL/CZTS双空穴传输层电池的输出参数

Table 4. Performance parameters of PSCs with HTL/CZTS.

Device structures	V_OC/V	J_SC/(mA·cm^–2)	PCE/%	FF/%
FTO/ZnO/Cs₂AgBiI₆/Spiro/CZTS/Au	1.1	24.73	22.62	83.15
FTO/ZnO/Cs₂AgBiI₆/Cu₂O/CZTS/Au	1.1	24.89	22.85	83.46
FTO/ZnO/Cs₂AgBiI₆/MoO₃/CZTS/Au	1.1	24.83	22.79	83.44

DownLoad: CSV

表 5 正交实验中Cu₂O和CZTS作为HTL的太阳能电池性能参数

Table 5. Performance parameters of PSCs with Cu₂O and CZTS as HTL in orthogonal experiments.

Experiment No.	Thickness/nm				V_OC/V	J_SC/(mA·cm^–2)	PCE/%	FF/%
Experiment No.	ZnO	Cs₂AgBiI₆	CZTS	Cu₂O	V_OC/V	J_SC/(mA·cm^–2)	PCE/%	FF/%
1	40	850	150	140	1.103	28.31	25.62	82.05
2	40	900	170	150	1.100	28.36	25.46	81.61
3	40	950	160	160	1.098	28.37	25.25	81.06
4	50	850	170	160	1.102	27.92	25.26	82.10
5	50	900	160	140	1.101	28.10	25.21	81.49
6	50	950	150	150	1.098	28.09	25.01	81.09
7	60	850	160	150	1.103	27.80	25.15	82.02
8	60	900	150	160	1.100	27.56	24.75	81.64
9	60	950	170	140	1.098	28.30	25.15	80.94

DownLoad: CSV

map

[1]	Hasan S A U, Zahid M A, Park S, Yi J 2024 Sol. RRL 8 2300967 Google Scholar
[2]	Cheng M, Jiang J, Yan C, Lin Y, Mortazavi M, Kaul A B, Jiang Q 2024 Nanomaterials 14 391 Google Scholar
[3]	Liu H R, Zhang Z H, Yang F, Yang J E, Grace A N, Li J M, Tripathi S, Jain S M 2021 Coatings 11 1045 Google Scholar
[4]	Machin A, Marquez F 2024 Materials 17 1165 Google Scholar
[5]	万婷婷, 朱安康, 郭友敏, 汪春昌 2017 材料导报 31 16 Google Scholar Wan T T, Zhu A K, Guo Y M, Wang C C 2017 Mater. Rev. 31 16 Google Scholar
[6]	Zhai M, Chen C, Cheng M 2023 Sol. Energy 253 563 Google Scholar
[7]	Meyer E, Mutukwa D, Zingwe N, Taziwa R 2018 Metals 8 667 Google Scholar
[8]	Yuan Y, Yan G, Hong R, Liang Z, Kirchartz T 2022 Adv. Mater. 34 2108132 Google Scholar
[9]	Zhao X G, Yang J H, Fu Y, Yang D, Xu Q, Yu L, Wei S H, Zhang L 2017 J. Am. Chem. Soc. 139 2630 Google Scholar
[10]	Ji F, Boschloo G, Wang F, Gao F 2023 Sol. RRL 7 2201112 Google Scholar
[11]	chrafih Y, Al Hattab M, Rahmani K 2023 J. Alloys Compd. 960 170650 Google Scholar
[12]	Amraoui S, Feraoun A, Kerouad M 2022 Inorg. Chem. Commun. 140 109395 Google Scholar
[13]	Slavney A H, Hu T, Lindenberg A M, Karunadasa H I 2016 J. Am. Chem. Soc. 138 2138 Google Scholar
[14]	Huang Q, Liu J, Qi F, Pu Y, Zhang N, Yang J, Liang Z, Tian C 2023 J. Environ. Chem. Eng. 11 109960 Google Scholar
[15]	Creutz S E, Crites E N, De Siena M C, Gamelin D R 2018 Nano Lett. 18 1118 Google Scholar
[16]	Rehman M A, Ur Rehman J, Tahir M B 2023 J. Phys. Chem. Solids. 181 111443 Google Scholar
[17]	Yadav S C, Srivastava A, Manjunath V, Kanwade A, Devan R S, Shirage P M 2022 Mater. Today Phys. 26 100731 Google Scholar
[18]	Volonakis G, Filip M R, Haghighirad A A, Sakai N, Wenger B, Snaith H J, Giustino F 2016 J. Phys. Chem. Lett. 7 1254 Google Scholar
[19]	Igbari F, Wang R, Wang Z K, Ma X J, Wang Q, Wang K L, Zhang Y, Liao L S, Yang Y 2019 Nano Lett. 19 2066 Google Scholar
[20]	Hossain M K, Samajdar D P, Das R C, Arnab A A, Rahman M F, Rubel M H K, Islam M R, Bencherif H, Pandey R, Madan J, Mohammed M K A 2023 Energy Fuels 37 3957 Google Scholar
[21]	Alla M, Manjunath V, Choudhary E, Samtham M, Sharma S, Shaikh P A, Rouchdi M, Fares B 2023 Phys. Status Solidi A 220 2200642 Google Scholar
[22]	Zarabinia N, Rasuli R 2021 Energy Sources Part A 43 2443 Google Scholar
[23]	Chen Q M, Ni Y, Dou X M, Yoshinori Y 2022 Crystals 12 68 Google Scholar
[24]	Azadinia M, Ameri M, Ghahrizjani R T, Fathollahi M 2021 Mater. Today Energy 20 100647 Google Scholar
[25]	Yoon S, Kim H, Shin E Y, Bae I G, Park B, Noh Y Y, Hwang I 2016 Org. Electron. 32 200 Google Scholar
[26]	Chen G S, Chen Y C, Lee C T, Lee H Y 2018 Sol. Energy 174 897 Google Scholar
[27]	Dahal B, Rezaee M D, Gotame R C, Li W 2023 Mater. Today Commun. 36 106846 Google Scholar
[28]	Kim D I, Lee J W, Jeong R H, Nam S H, Hwang K H, Boo J H 2019 Surf. Coat. Technol. 357 189 Google Scholar
[29]	Chen Y, Zhang M, Li F Q, Yang Z Y 2023 Coatings 13 644 Google Scholar
[30]	Islam T, Jani R, Amin S M A, Shorowordi K M, Nishat S S, Kabir A, Taufique M F N, Chowdhury S, Banerjee S, Ahmed S 2020 Comput. Mater. Sci. 184 109865 Google Scholar
[31]	Anoop K M, Ahipa T N 2023 Sol. Energy 263 111937 Google Scholar
[32]	Kumar A 2021 Superlattices Microstructure. 153 106872 Google Scholar
[33]	Hossain M K, Arnab A A, Das R C, Hossain K M, Rubel M H K, Rahman M F, Bencherif H, Emetere M E, Mohammed M K A, Pandey R 2022 RSC Adv. 12 34850 Google Scholar
[34]	Bhattarai S, Hossain M K, Pandey R, Madan J, Samajdar D P, Rahman M F, Ansari M Z, Amami M 2023 Energy Fuels 37 10631 Google Scholar

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Vol. 74, Issue 3 - 2025-02-05

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Theoretical analysis and performance optimization of Cs₂AgBiI₆ solar cells with dual hole transport layers

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Corresponding author: TIAN Hanmin, tianhanmin@hebut.edu.cn

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Theoretical analysis and performance optimization of Cs2AgBiI6 solar cells with dual hole transport layers

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Theoretical analysis and performance optimization of Cs₂AgBiI₆ solar cells with dual hole transport layers