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Magnetron sputtering NiOx for perovskite solar cells

Xiangyi Shen, Xinwu Ke, Yingdong Xia, Qingxun Guo and Yonghua Chen

+ Author Affiliations

 Corresponding author: Yingdong Xia, iamydxia@njtech.edu.cn; Qingxun Guo, iamqxguo@njtech.edu.cn; Yonghua Chen, iamyhchen@njtech.edu.cn

DOI: 10.1088/1674-4926/24100032CSTR: 32376.14.1674-4926.24100032

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Abstract: Perovskite solar cells (PSCs) have become a hot topic in the field of renewable energy due to their excellent power conversion efficiency and potential for low-cost manufacturing. The hole transport layer (HTL), as a key component of PSCs, plays a crucial role in the cell's overall performance. Magnetron sputtering NiOx has attracted widespread attention due to its high carrier mobility, excellent stability, and suitability for large-scale production. Herein, an insightful summary of the recent progress of magnetron sputtering NiOx as the HTL of PSCs is presented to promote its further development. This review summarized the basic properties of magnetron sputtering NiOx thin film, the key parameters affecting the optoelectronic properties of NiOx thin films during the magnetron-sputtering process, and the performance of the corresponding PSCs. Special attention was paid to the interfacial issues between NiOx and perovskites, and the modification strategies were systematically summarized. Finally, the challenges of sputtering NiOx technology and the possible development opportunities were concluded and discussed.

Key words: magnetron sputtering, NiOx, perovskite, solar cells



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Fig. 1.  (Color online) (a) Radar chart illustrating the key property difference between NiOx, SAMs, and PEDOT:PSS. (b) Comparison of the optoelectronic properties of NiOx, SAMs, and PEDOT: PSS[10−14].

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Fig. 2.  (Color online) The schematic diagram of the topics in this review.

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Fig. 3.  (Color online) (a) Crystal structure of NiOx[23]. (b) The conduction mechanism of NiOx, where Vc represents Ni2+ vacancies[25]. (c) Schematic diagram of the electronic structure of NiOx[26]. (d) Resistivity of Zn-doped NiOx films with different doping ratios[29]. (e) Top-view SEM images of NiOx thin films deposited on FTO[28]. (f) XRD patterns of NiOx thin films[33].

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Fig. 4.  (Color online) Schematic diagram of NiOx thin film deposition by (a) magnetron sputtering deposition, (b) spin-coating deposition[37], (c) spray pyrolysis droplet deposition[42], (d) electrochemical deposition[44], (e) pulsed laser deposition[46], and (f) ALD techniques[48].

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Fig. 5.  (Color online) (a) Schematic diagram of the sputtering under low and high sputtering pressure conditions[50]. (b) AFM images of NiOx films and bare glass deposited at different pressures. (c) Transmittance of NiOx thin films deposited by magnetron sputtering under various pressures[52]. (d) Conductivity variation with Ni3+/Ni2+ ratio, and XPS images of NiOx films at 4 mTorr (inset)[54]. (e) XRD patterns of Cu-doped NiOx films with different substrate temperatures[55]. (f) The Ni3+/Ni2+ ratio of NiOx thin films sputtered under various oxygen content[58]. (g) A chart of the energy levels of device functional layers[60]. (h) Structure diagram of aluminum-doped NiOx. (i) J−V curve of perovskite devices based on NiOx and AlyNi1−yOx[64].

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Fig. 6.  (Color online) (a) The energy levels of common perovskites used in inverted PSCs with magnetron-sputtered NiOx as the HTL[20, 52, 71, 72, 77]. (b) Efficiency evolution of PSCs based on magnetron-sputtered NiOx as HTL[20, 52, 54, 57, 65−74]. (c) Long-term stability of devices based on NiOx and MeO-4PADBC at different temperatures[18]. (d) The J−V curve of the 100 cm² minimodules based on NiOx/Me-4PACz[72]. (e) Schematic diagram of the tandem PSCs with ITO/NiOx as the connecting layer[75]. (f) Flexible perovskite solar cell devices based on NiOx[76].

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Fig. 7.  (Color online) (a) The energy band diagram of NiOx, interlayer, and perovskites with different bandgaps. (b) The J−V curves of 1.53 eV devices with NiOx, MeO-4PADBC, and NiOx/MeO-4PADBC as HTLs[18]. (c) Schematic diagram of the redox degradation mechanism at the NiOx/perovskite interface[73]. (d) Dark and light J−V curves with excess A-site ion PSCs[80].

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Fig. 8.  (Color online) (a) Schematic diagram of molecular anchoring group of SAMs[81]. (b) Electrostatic potential of PC molecules and mechanism of co-SAMs modified interface[82]. (c) The corresponding potential histograms of ITO and ITO/NiOx films before and after the adsorption of MeO-2PACz[70]. (d) Energy level diagram for pristine NiOx and NiOx/MeO-2PACz[65]. (e) Schematic diagrams of the NaIO4-modified NiOx film experimental process and the binding of SAMs[83].

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Fig. 9.  (Color online) (a) Schematic diagram of the structure with NaCl interface introduced between NiOx and perovskite[84]. (b) XRD patterns of the perovskite layer with and without CsBr interfacial layer between NiOx and perovskite[85]. (c) Top-view SEM of NiOx/perovskite and NiOx/CsBr/perovskite. (d) UPS spectra of the work function and valence band regions for NiOx film and NiOx/CsBr film[86]. (e) Chemical structure of the N719 molecule, and the electrostatic potential diagram, and three-dimensional charge density difference diagram of the NiOx(001)/N719/PbI2-rich MAPbI3(001) interface[71]. (f) Schematic electronic structure and carrier distribution of AlOx/perovskite and SiOx/perovskite heterojunctions[89].

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Table 1.   Review summary of the device structure, VOC, JSC, and PCE of inverted PSCs using sputtered NiOx HTLs as discussed in this review.

Device structure Sputtering Parameters Jsc
(mA/cm2)		 Voc
(V)		 PCE
(%)		 Publication
date		 Ref.
FTO/NiOx/Cs0.17FA0.83Pb(I0.8Br0.2)3/C60/BCP/Cu Ar/14 sccm/1.32 W/cm2 18.79 1.05 15.71 2020 [52]
ITO/NiOx/MeO-2PACz/MAPbI3/AZO/Ag 3.5Pa 20.1 1.11 16.25 2022 [65]
FTO/NiOx/MAPbI3/PCBM/BCP/Ag Ar&O2/1.3 Pa, 100 W 20.57 1.05 16.29 2018 [66]
FTO/Cu:NiOx/CH3NH3PbI3/ZnO/Ag Ar : O2= 35 : 5 sccm/1.5 Pa, Ni : Cu = 300 : 15 W, 23.05 1.03 16.51 2020 [67]
ITO/NiOx /MAPbI3/PCBM/BCP/Ag Ar/20 sccm/0.4 Pa,
1.97 W/cm2,		 20.65 1.07 17.6 2018 [68]
ITO/Mg:NiOx/MAPbI3/PCBM/ZnMgO/Al Ar&O2/500 Pa, 80 W / / 18.5 2017 [20]
ITO/NiOx/MA0.65FA0.35PbI3/PCBM/BCP/Ag / / / 18.7 2020 [57]
ITO/NiOx/spiro-TTB/MAPbI3/PCBM/BCP/Ag 2.7 Pa, 20 W 22.3 1.08 19.5 2023 [54]
FTO/NiOx/NiyN/MAPbI3/PCBM/BCP/Ag Ar : N2=15 : 45 sccm/0.4 Pa / / 19.8 2022 [69]
ITO/NiOx/MeO-2PACz/
Cs0.05(FA0.83MA0.17)0.95Pb(I0.82Br0.18)3 /C60/BCP/Ag		 Ar : O2=20 : 2.2 sccm/0.4 Pa, 80 W 22.3 1.10 19.9 2021 [70]
ITO/NiOx/N719/
Cs0.05MA0.15FA0.80Pb(I0.85Br0.15)3/C60/BCP/Ag		 / 23.2 1.13 20.3 2021 [71]
ITO/NiOx/Me-4PACz/
Cs0.2FA0.8Pb(I0.94Br0.053)3/LiF/C60/BCP/Cu		 / 24.1 1.14 21.8 2024 [72]
ITO/NiOx/
Cs0.05MA0.16FA0.79Pb(Br0.16I0.84)3/PCBM/BCP/Ag		 Ar/100 sccm /0.37 Pa, 200 W 24.12 1.19 22.72 2024 [73]
ITO/NiOx/Me-4PACz/TEACl/
Cs0.1FA0.9PbI2.855Br0.145/TEACl/LiF/C60/BCP/Cu		 / 24.4 1.16 23.0 2023 [74]
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    Received: 24 October 2024 Revised: 12 December 2024 Online: Accepted Manuscript: 08 January 2025Uncorrected proof: 18 February 2025

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      Xiangyi Shen, Xinwu Ke, Yingdong Xia, Qingxun Guo, Yonghua Chen. Magnetron sputtering NiOx for perovskite solar cells[J]. Journal of Semiconductors, 2025, In Press. doi: 10.1088/1674-4926/24100032 ****X Y Shen, X W Ke, Y D Xia, Q X Guo, and Y H Chen, Magnetron sputtering NiOx for perovskite solar cells[J]. J. Semicond., 2025, 46(5), 051803 doi: 10.1088/1674-4926/24100032
      Citation:
      Xiangyi Shen, Xinwu Ke, Yingdong Xia, Qingxun Guo, Yonghua Chen. Magnetron sputtering NiOx for perovskite solar cells[J]. Journal of Semiconductors, 2025, In Press. doi: 10.1088/1674-4926/24100032 ****
      X Y Shen, X W Ke, Y D Xia, Q X Guo, and Y H Chen, Magnetron sputtering NiOx for perovskite solar cells[J]. J. Semicond., 2025, 46(5), 051803 doi: 10.1088/1674-4926/24100032
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      Magnetron sputtering NiOx for perovskite solar cells

      DOI: 10.1088/1674-4926/24100032
      CSTR: 32376.14.1674-4926.24100032

      • Key Laboratory of Flexible Electronics (KLoFE) & Institute of Advanced Materials (IAM), School of Flexible Electronics (Future Technologies), Nanjing Tech University (NanjingTech), Nanjing 211816, China

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      • Xiangyi Shen received her Bachelor's degree in Chemical Biology from Changzhi University in 2021. She is currently a master's student at the Institute of Advanced Materials (IAM) & School of Flexible Electronics (Future Technologies), Nanjing Tech University. Her current research focuses on perovskite solar cells with charge transport layers of metal oxides fabricated by magnetron sputtering
      • Xinwu Ke received his Bachelor's degree in Applied Chemistry from Qilu University of Technology in 2022. He is currently a master's student at the Institute of Advanced Materials (IAM) & School of Flexible Electronics (Future Technologies), Nanjing Tech University. His current research focuses on vacuum-deposited perovskite solar cells
      • Yingdong Xia received her B.E. degree in macromolecular science and engineering from Hebei University in 2006 and the Ph.D. degree in polymer chemistry and physics from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, in 2011. She then conducted her postdoc research at Georgia Institute of Technology and Wake Forest University during 2011–2013. She is now a Professor at Nanjing Tech University. Her current research interest is focused on organic light-emitting diodes, perovskite light-emitting diodes, and solar cells
      • Qingxun Guo received his Bachelor's degree from the Jilin University in 2012, and Ph.D. degree in Polymer Chemistry and Physics from the Changchun Institute of Applied Chemistry, Chinese Academy of Sciences in 2017. He engaged in OLED panel design for two years at TCL China Star Optoelectronics Technology Co., Ltd (CSOT) and then joined the Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology as a Postdoctoral Researcher in 2019. He is currently an associate professor at Nanjing Tech University. His research focuses on metal halides for light-emitting diodes and solar cells
      • Yonghua Chen received a bachelor's degree in Chemistry from Inner Mongolia University in 2006 and a Ph. D. in Polymer Chemistry and Physics at the Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, in 2011. Afterward, he spent time at Wake Forest University (2 years) and Case Western Reserve University (2 years) as a postdoctoral researcher. He is currently a full professor at Nanjing Tech University. His research interests are organic and organic/inorganic hybrid optoelectronic materials and devices for energy conversion
      • Corresponding author: iamydxia@njtech.edu.cn; iamqxguo@njtech.edu.cn; iamyhchen@njtech.edu.cn
      • Received Date: 2024-10-24
      • Revised Date: 2024-12-12
        • Available Online: 2025-01-08

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