Theoretical study of photovoltaic performance for inverted halide perovskite solar cells

Zhang Ao; Zhang Chun-Xiu; Chen Yun-Lin; Zhang Chun-Mei; Meng Tao

doi:10.7498/aps.69.20200089

Abstract

The existence of serious hysteresis effect for regular perovskite solar cells (PSCs) will affect their performances, however, the inverted PSCs can significantly suppress the hysteresis effect. To data, it has been very rarely reported to simulate the inverted planar heterojunction PSCs. In this paper, the effects of hole transport material (HTM), electron transport material (ETM), and ITO work function on performance of inverted MAPbI₃ solar cells are carefully investigated in order to design the high-performance inverted PSCs. The inverted MAPbI₃ solar cells using Cu₂O, CuSCN, or NiO_x as HTM, and PC₆₁BM, TiO₂, or ZnO as ETM are simulated with the program AMPS-1D. Simulation results reveal that i) the inverted MAPbI₃ solar cells choosing NiO_x as HTM can effectively improve the photovoltaic performance, and the excellent photovoltaic performance obtained by using TiO₂ as ETM is almost the same as by using ZnO as ETM; ii) the ITO work function increasing from 4.6 eV to 5.0 eV can significantly enhance the photovoltaic performances of Cu₂O— based and CuSCN— based inverted MAPbI₃ solar cells, and the NiO_x— based inverted MAPbI₃ solar cells have only a minor photovoltaic performance enhancement; iii) based on the reported ITO work function between 4.6 eV and 4.8 eV, the maximum power conversion efficiency (PCE) of 27.075% and 29.588% for CuSCN— based and NiO_x— based inverted MAPbI₃ solar cells are achieved when the ITO work function reaches 4.8 eV. The numerical simulation gives that the increase of hole mobility in CuSCN and NiO_x for ITO/CuSCN/MAPbI₃/TiO₂/Al and ITO/NiO_x/MAPbI₃/TiO₂/Al can greatly improve the device performance. Experimentally, the maximum hole mobility 0.1 cm²·V^–1·s^–1 in CuSCN restricts the photovoltaic performance improvement of CuSCN— based inverted MAPbI₃ solar cells, which means that there is still room for the improvement of cell performance through increasing the hole mobility in CuSCN. It is found that NiO_x with a reasonable energy-band structure and high hole mobility 120 cm²·V^–1·s^–1 is an ideal HTM in inverted MAPbI₃ solar cells. However, the increasing of electron mobility in TiO₂ cannot improve the device photovoltaic performance of inverted MAPbI₃ solar cells. These simulation results reveal the effects of ETM, HTM, and ITO work function on the photovoltaic performance of inverted MAPbI₃ solar cells. Our researches may help to design the high-performance inverted PSCs.

Keywords:

Authors and contacts

1.
Department of Science, Beijing Institute of Graphic Communication, Beijing 102600, China
2.
Institute of Applied Micro-Nano Materials, School of Science, Beijing Jiaotong University, Beijing 100044, China

Corresponding author: Chen Yun-Lin, ylchen@bjtu.edu.cn

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References

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[2]	Yin W J, Shi T T, Yan Y T 2014 Appl. Phys. Lett. 104 063903 Google Scholar
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[20]	Fonash S, Arch J, Cuiffi J, et al. A One-Dimensional Device Simulation Program for the Analysis of Microelectronic and Photonic Structures http://www.emprl.psu.edu/amps[1997-1-1]
[21]	Zhang A, Chen Y L, Yan J 2016 Ieee J. Quantum Elect. 52 1600106 Google Scholar
[22]	Onoda-Yamamuro N, Matsuo T, Suga H 1992 J. Phys. Chem. Solids. 53 935 Google Scholar
[23]	Laban W A, Etgar L 2013 Energ. Environ Sci. 6 3249 Google Scholar
[24]	Stoumpos C C, Malliakas C D, Kanatzidis M G 2013 Inorg. Chem. 52 9019 Google Scholar
[25]	Rode D L 1975 Semiconductors and Semimetals (New York: Academic) pp1–89
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[33]	Kaiser I, Ernst K, Fischer C H, Konenkamp R, Rost C, Sieber I, Lux-Steiner M C 2001 Sol. Energy Mater. Sol. Cells. 67 89 Google Scholar
[34]	Pattanasattayavong P, Ndjawa G O N, Zhao K, Chou K W, Yaacobi-Gross N, O’Regan B C, Amassian A, Anthopoulos T D 2013 Chem. Commun. 49 4154 Google Scholar
[35]	Pattanasattayavong P, Yaacobi-Gross N, Zhao K, Ndjawa G O N, Li J H, Yan F, O’Regan B C, Amassiann A, Anthopoulos T D 2013 Adv. Mater 25 1504 Google Scholar
[36]	Rao V, Smakula A 1965 J. Appl. Phys. 36 2031 Google Scholar
[37]	Ratcliff E L, Meyer J, Steirer K X, Armstrong N R, Olson D, Kahn A 2012 Org. Electron. 13 744 Google Scholar
[38]	Wu H B, Wang L S 1997 J. Chem. Phys. 107 16 Google Scholar
[39]	Liu M H, Zhou Z J, Zhang P P, Tian Q W, Zhou W H, Kou D X, Wu S X 2016 Opt. Express 24 1349 Google Scholar
[40]	Rakhshani A E 1991 J. Appl. Phys. 69 2365 Google Scholar
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[44]	Shewchun J, Dubow J, Wilmsen C W, Singh R, Burk D, Wager J F 1979 J. Appl. Phys. 50 2832 Google Scholar
[45]	Park Y, Choong V, Gao Y, Hsieh B R, Tang C W 1996 Appl. Phys. Lett. 68 2699 Google Scholar
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Cited By

图 1 (a) 反式结构和(b) 正式结构平面异质结 MAPbI₃太阳能电池的工作原理示意图

Figure 1. Schematic diagram of working principle in (a) inverted and (b) regular planar heterojunction MAPbI₃ solar cells.

DownLoad: Full-Size Img PowerPoint

图 2 模拟反式钙钛矿太阳电池　(a) ITO/HTM/MAPbI₃/PC₆₁BM/Al, (b) ITO/HTM/MAPbI₃/TiO₂/Al, (c) ITO/HTM/MAPbI₃/ZnO/Al的PCE随MAPbI₃厚度的变化, 前、后电极的功函数分别是4.6 eV (ITO) 和4.3 eV (Al)

Figure 2. The PCE of inverted perovskite solar cells for (a) ITO/HTM/MAPbI₃/PC₆₁BM/Al, (b) ITO/HTM/MAPbI₃/TiO₂/Al, and (c) ITO/HTM/MAPbI₃/ZnO/Al simulated with the MAPbI₃ thickness. Front and back contact work function: 4.6 eV (ITO) and 4.3 eV (Al), respectively.

DownLoad: Full-Size Img PowerPoint

图 3 模拟反式钙钛矿太阳电池　(a) ITO/CuO₂/MAPbI₃/ETM/Al; (b) ITO/CuSCN/MAPbI₃/ETM/Al; (c) ITO/NiO_x/MAPbI₃/ETM/Al的PCE和FF随ITO功函数的变化, ETM表示PC₆₁BM, TiO₂, ZnO

Figure 3. Simulation for PCE and FF of inverted perovskite solar cells for (a) ITO/CuO₂/MAPbI₃/ETM/Al, (b) ITO/CuSCN/MAPbI₃/ETM/Al, and (c) ITO/NiO_x/MAPbI₃/ETM/Al solar cells as a function of ITO work function, here ETM is PC₆₁BM, TiO₂, or ZnO.

DownLoad: Full-Size Img PowerPoint

图 4 太阳能电池的伏安特性随CuSCN和NiO_x中空穴迁移率变化的函数, 前、后电极的功函数分别是: 4.6 eV (ITO) 和4.3 eV (Al)　(a) ITO/CuSCN/MAPbI₃/TiO₂/Al; (b) ITO/NiO_x/MAPbI₃/TiO₂/Al

Figure 4. J-V characteristics of solar cell as a function of hole mobility in CuSCN and NiO_x. Front and back contact work function is 4.6 eV (ITO) and 4.3 eV (Al), respectively: (a) ITO/CuSCN/MAPbI₃/TiO₂/Al; (b) ITO/NiO_x/MAPbI₃/TiO₂/Al.

DownLoad: Full-Size Img PowerPoint

表 1 AMPS-1D采用的MAPbI₃ 和ETM参数

Table 1. AMPS-1D parameters set for MAPbI₃ and ETM.

Parameters	MAPbI₃	ZnO	TiO₂	PC₆₁BM
Dielectric constant	23.3^[22]	8.12^[25]	100^[30]	3.9^[18]
Band gap/eV	1.51^[23]	3.40^[26]	3.2^[31]	1.9^[9]
Electron affinity/eV	3.93^[23]	4.19^[27]	4.0^[31]	3.9^[9]
Thickness/nm	40-400	90	90	90
Electron and hole mobility/cm²·V^–1·s^–1	50, 50^[24]	150, 0.0001^[28]	0.006, 0.006^[30]	0.0005, 0.0001^[18]
Acceptor concentration/cm^–3	(2.14 × 10¹⁷)^[23]	0	0	0
Donor concentration/cm^–3	0	(5 × 10¹⁹)^[29]	(5 × 10¹⁹)^[30]	5 × 10¹⁹
Effective conduction band density/cm^–3	1.66 × 10¹⁹	4.49 × 10¹⁸	1.0 × 10²¹	2.5 × 10²⁰
Effective valence band density/cm^–3	5.41 × 10¹⁸	5.39 × 10¹⁸	2.0 × 10²⁰	2.5 × 10²⁰

DownLoad: CSV

表 2 AMPS-1D采用的HTM参数

Table 2. AMPS-1D parameters set for HTM.

Parameters	CuSCN	NiO_x	Cu₂O
Dielectric constant	10^[32]	11.9^[36]	8.8^[40]
Band gap/eV	3.4^[33]	3.7^[37]	2.17^[41]
Electron affinity/eV	1.9^[33]	1.5^[38]	3.3^[42]
Thickness/nm	200	200	200
Electron and hole mobility/cm²·V^–1·s^–1	0.0001, 0.01—0.10^[34]	0.0001, 120^[39]	0.0001, 10^[43]
Acceptor concentration/cm^–3	(5 × 10¹⁸)^[35]	(2.66 × 10¹⁷)^[15]	(5 × 10¹⁵)^[43]
Donor concentration/cm^–3	0	0	0
Effective conduction band density/cm^–3	1.79 × 10¹⁹	2.5 × 10¹⁹	2.5 × 10¹⁹
Effective valence band density/cm^–3	2.51 × 10¹⁹	2.5 × 10¹⁹	2.5 × 10¹⁹

DownLoad: CSV

map

[1]	Zhou H P, Chen Q, Li G, Luo S, Song T B, Duan H S, Hong Z, You J B, Liu Y S, Yang Y 2014 Science 345 542 Google Scholar
[2]	Yin W J, Shi T T, Yan Y T 2014 Appl. Phys. Lett. 104 063903 Google Scholar
[3]	Boix P P, Nonomura K, Mathews N, Mhaisalkar S G 2014 Mater. Today 17 16 Google Scholar
[4]	Akihiro K, Kenjiro T, Yasuo S, Tsutomu M 2009 J. Am. Chem. Soc. 131 6050 Google Scholar
[5]	Meng L, You J B, Yang Y 2018 Nat. Commun. 9 5265 Google Scholar
[6]	Snaith H J, Abate A, Ball J M, Eperon G E, Leijtens T, Noel N K, Stranks S D, Wang J T, Wojciechowski K, Zhang W 2014 J. Phys. Chem. Lett. 5 1511 Google Scholar
[7]	Saliba M 2018 Science 359 388 Google Scholar
[8]	Yu S, Yan Y, Chen Y, Chábera P, Zheng K, Liang Z 2019 J. Mater. Chem. A 7 2015 Google Scholar
[9]	Liu T H, Chen K, Hu Q, Zhu R, Gong Q H 2016 Adv. Energy Mater. 6 1600457 Google Scholar
[10]	Jeng J Y, Chiang Y F, Lee M H, Peng S R, Guo T F, Chen P, Wen T C 2013 Adv. Mater 25 3727 Google Scholar
[11]	Li J W, Dong Q S, Li N, Wang L D 2017 Adv. Energy Mater. 7 1602922 Google Scholar
[12]	Shi J J, Zhang H Y, Xu X, Li D M, Luo Y H, Meng Q B 2016 Small 12 5288 Google Scholar
[13]	Kakavelakis G, Maksudov T, Konios D, Paradisanos I, Kioseoglou G, Stratakis E, Kymakis E 2017 Adv. Energy Mater. 7 1602120 Google Scholar
[14]	Wang K C, Shen P S, Li M H, Chen S, Lin M W, Chen P, Guo T F 2014 ACS Appl. Mater. Interfaces 6 11851 Google Scholar
[15]	Chen W, Wu Y Z, Yue Y F, Liu J, Zhang W J, Yang X D, Chen H, Bi E B, Ashraful I, Grätzel M, Han L Y 2015 Science 350 944 Google Scholar
[16]	Bi C, Wang Q, Shao Y, Yuan Y, Xiao Z, Huang J 2015 Nat. Commun. 6 8747 Google Scholar
[17]	Shao Y C, Yuan Y B, Huang J S 2016 Nat. Energy 1 15001 Google Scholar
[18]	Kuang C Y, Tang G, Jiu T G, Yang H, Liu H B, Li B R, Luo W N, Li X G, Zhang W J, Lu F S, Fang J F, Li Y L 2015 Nano Lett. 15 2756 Google Scholar
[19]	Luo D Y, Yang W Q, Wang Z P, Sadhanala A, Hu Q, Su R, Shivanna R, Trindade G F, Watts J F, Xu Z J, Liu T H, Chen K, Ye F J, Wu P, Zhao L C, Wu J, Tu Y G, Zhang Y F, Yang X Y, Zhang W, Friend R H, Gong Q H, Snaith H J, Zhu R 2018 Science 360 1442 Google Scholar
[20]	Fonash S, Arch J, Cuiffi J, et al. A One-Dimensional Device Simulation Program for the Analysis of Microelectronic and Photonic Structures http://www.emprl.psu.edu/amps[1997-1-1]
[21]	Zhang A, Chen Y L, Yan J 2016 Ieee J. Quantum Elect. 52 1600106 Google Scholar
[22]	Onoda-Yamamuro N, Matsuo T, Suga H 1992 J. Phys. Chem. Solids. 53 935 Google Scholar
[23]	Laban W A, Etgar L 2013 Energ. Environ Sci. 6 3249 Google Scholar
[24]	Stoumpos C C, Malliakas C D, Kanatzidis M G 2013 Inorg. Chem. 52 9019 Google Scholar
[25]	Rode D L 1975 Semiconductors and Semimetals (New York: Academic) pp1–89
[26]	Muth J F, Kolbas R M, Sharma A K, Oktabrsky S, Narayan J 1999 J. Appl. Phys. 85 7884 Google Scholar
[27]	Moormann H, Kohl D, Heiland G 1980 Surf. Sci. 100 302 Google Scholar
[28]	Hagemark K J, Chacka L C 1975 J. Solid State Chem. 15 261 Google Scholar
[29]	Kim K J, Park Y R 2001 Appl. Phys. Lett. 78 475 Google Scholar
[30]	Wojciechowski K, Saliba M, Leijtens T, Abate A, Snaith H J 2014 Energ. Environ. Sci. 7 1142 Google Scholar
[31]	Liu F, Zhu J, Wei J F, Li Y, Lv M, Yang S F, Zhang B, Yao J X, Dai S Y 2014 Appl. Phys. Lett. 104 253508 Google Scholar
[32]	Jaffe J E, Kaspar T C, Droubay T C, Varga T, Bowden M E, Exarhos G J 2010 J. Phys. Chem. C 114 9111 Google Scholar
[33]	Kaiser I, Ernst K, Fischer C H, Konenkamp R, Rost C, Sieber I, Lux-Steiner M C 2001 Sol. Energy Mater. Sol. Cells. 67 89 Google Scholar
[34]	Pattanasattayavong P, Ndjawa G O N, Zhao K, Chou K W, Yaacobi-Gross N, O’Regan B C, Amassian A, Anthopoulos T D 2013 Chem. Commun. 49 4154 Google Scholar
[35]	Pattanasattayavong P, Yaacobi-Gross N, Zhao K, Ndjawa G O N, Li J H, Yan F, O’Regan B C, Amassiann A, Anthopoulos T D 2013 Adv. Mater 25 1504 Google Scholar
[36]	Rao V, Smakula A 1965 J. Appl. Phys. 36 2031 Google Scholar
[37]	Ratcliff E L, Meyer J, Steirer K X, Armstrong N R, Olson D, Kahn A 2012 Org. Electron. 13 744 Google Scholar
[38]	Wu H B, Wang L S 1997 J. Chem. Phys. 107 16 Google Scholar
[39]	Liu M H, Zhou Z J, Zhang P P, Tian Q W, Zhou W H, Kou D X, Wu S X 2016 Opt. Express 24 1349 Google Scholar
[40]	Rakhshani A E 1991 J. Appl. Phys. 69 2365 Google Scholar
[41]	Ghijsen J, Tjeng L H, van Elp J, Eskes H, Westerink J, Sawatzky G A 1988 Phys. Rev. B 38 11322 Google Scholar
[42]	Zuo C T, Ding L M 2015 Small 11 5528 Google Scholar
[43]	Matsumura H, Fujii A, Kitatani T 1996 Jpn. J. Appl. Phys. 35 5631 Google Scholar
[44]	Shewchun J, Dubow J, Wilmsen C W, Singh R, Burk D, Wager J F 1979 J. Appl. Phys. 50 2832 Google Scholar
[45]	Park Y, Choong V, Gao Y, Hsieh B R, Tang C W 1996 Appl. Phys. Lett. 68 2699 Google Scholar
[46]	Balasubramanian N, Subrahmanyam A 1991 J. Electrochem. Soc. 138 322 Google Scholar
[47]	Nehate S D, Prakash A, DossMani P, Sundaram, K B 2018 ECS J. Solid State Sc. 7 87

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