Issue

Vol. 17 (2025)

Molecular Structure Tailoring of Organic Spacers for High-Performance Ruddlesden–Popper Perovskite Solar Cells

https://doi.org/10.1007/s40820-024-01500-7
Pengyun Liu
School of Materials Science and Engineering, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, People’s Republic of China
Xuejin Li
School of Materials Science and Engineering, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, People’s Republic of China
Tonghui Cai
School of Materials Science and Engineering, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, People’s Republic of China
Wei Xing
School of Materials Science and Engineering, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, People’s Republic of China
Naitao Yang
School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, People’s Republic of China
Hamidreza Arandiyan
Centre for Applied Materials and Industrial Chemistry (CAMIC), School of Science, RMIT University, Melbourne, Vic 3000, Australia
Zongping Shao
WA School of Mines: Minerals, Energy and Chemical Engineering (WASM‑MECE), Curtin University, Perth, WA 6102, Australia
Shaobin Wang
School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
Shaomin Liu
WA School of Mines: Minerals, Energy and Chemical Engineering (WASM‑MECE), Curtin University, Perth, WA 6102, Australia

Corresponding Author: Shaomin Liu

liushaomin@gbu.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 35

Abstract

Layer-structured Ruddlesden–Popper (RP) perovskites (RPPs) with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell (PSC) technology. However, two-dimensional (2D) or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy, blocked charge transport and poor film quality, which restrict their photovoltaic performance. Fortunately, these issues can be readily resolved by rationally designing spacer cations of RPPs. This review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic applications. We firstly elucidated the important roles of organic spacers in impacting crystallization kinetics, charge transporting ability and stability of RPPs. Then we brought three aspects to attention for designing organic spacers. Finally, we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP PSCs. These proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.


Highlights:
1 Organic spacers in Ruddlesden–Popper (RP) perovskites play a vital role in tuning crystallization, charge transport and photovoltaic performance for RP perovskite solar cells (PSCs).
2 Fundamental understanding of the functions of molecular structure of organic spacers is the prerequisite to design high-performance PSCs.
3 This review proposes practical design strategies in seeking RP molecular structure to maximize its photovoltaic performance for PSCs.

Keywords

Ruddlesden–Popper perovskites Low-dimensional perovskite solar cells Organic spacers Molecular structure Design strategies
Liu, Pengyun, Xuejin Li, Tonghui Cai, Wei Xing, Naitao Yang, Hamidreza Arandiyan, Zongping Shao, Shaobin Wang, and Shaomin Liu. 2024. “Molecular Structure Tailoring of Organic Spacers for High-Performance Ruddlesden–Popper Perovskite Solar Cells”. Nano-Micro Letters 17 (October):35. https://doi.org/10.1007/s40820-024-01500-7.
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References
  1. B. Hailegnaw, S. Demchyshyn, C. Putz, L.E. Lehner, F. Mayr et al., Flexible quasi-2D perovskite solar cells with high specific power and improved stability for energy-autonomous drones. Nat. Energy 9, 677–690 (2024). https://doi.org/10.1038/s41560-024-01500-2
  2. J. Liang, Z. Zhang, Q. Xue, Y. Zheng, X. Wu et al., A finely regulated quantum well structure in quasi-2D Ruddlesden-Popper perovskite solar cells with efficiency exceeding 20%. Energy Environ. Sci. 5, 296–310 (2022). https://doi.org/10.1039/D1EE01695D
  3. X. Sheng, Y. Li, M. Xia, E. Shi, Quasi-2D halide perovskite crystals and their optoelectronic applications. J. Mater. Chem. A 10, 19169–19183 (2022). https://doi.org/10.1039/D1EE01695D
  4. X. Li, G. Wu, M. Wang, B. Yu, J. Zhou et al., Water-assisted crystal growth in quasi-2D perovskites with enhanced charge transport and photovoltaic performance. Adv. Energy Mater. 10, 2001832 (2020). https://doi.org/10.1002/aenm.202001832
  5. J.Y. Kim, J.-W. Lee, H.S. Jung, H. Shin, N.-G. Park, High-efficiency perovskite solar cells. Chem. Rev. 120, 7867–7918 (2020). https://doi.org/10.1021/acs.chemrev.0c00107
  6. J. Zhao, Z. Zhang, G. Li, M.H. Aldamasy, M. Li et al., Dimensional tuning in lead-free tin halide perovskite for solar cells. Adv. Energy Mater. 13, 2204233 (2023). https://doi.org/10.1002/aenm.202204233
  7. H. Peng, D. Li, Z. Li, Z. Xing, X. Hu et al., Ionic liquid assisted imprint for efficient and stable quasi-2D perovskite solar cells with controlled phase distribution. Nano-Micro Lett. 15, 91 (2023). https://doi.org/10.1007/s40820-023-01076-8
  8. M. Ren, S. Cao, J. Zhao, B. Zou, R. Zeng, Advances and challenges in two-dimensional organic-inorganic hybrid perovskites toward high-performance light-emitting diodes. Nano-Micro Lett. 13, 163 (2021). https://doi.org/10.1007/s40820-021-00685-5
  9. X. Zhao, T. Liu, Y.-L. Loo, Advancing 2D perovskites for efficient and stable solar cells: challenges and opportunities. Adv. Mater. 34, 2105849 (2022). https://doi.org/10.1002/adma.202105849
  10. L. Mao, C.C. Stoumpos, M.G. Kanatzidis, Two-dimensional hybrid halide perovskites: Principles and promises. J. Am. Chem. Soc. 141, 1171–1190 (2019). https://doi.org/10.1021/jacs.8b10851
  11. I. Metcalf, S. Sidhik, H. Zhang, A. Agrawal, J. Persaud et al., Synergy of 3D and 2D perovskites for durable, efficient solar cells and beyond. Chem. Rev. 123, 9565–9652 (2023). https://doi.org/10.1021/acs.chemrev.3c00214
  12. G. Bravetti, D. Altamura, B. Paci, A. Generosi, S. Carallo et al., Addressing the role of 2D domains in high-dimensionality Ruddlesden-Popper perovskite for solar cells. Sol. RRL 7, 2200860 (2023). https://doi.org/10.1002/solr.202200860
  13. J. Gong, M. Hao, Y. Zhang, M. Liu, Y. Zhou, Layered 2D halide perovskites beyond the Ruddlesden-Popper phase: Tailored interlayer chemistries for high-performance solar cells. Angew. Chem. Int. Ed. 134, e202112022 (2022). https://doi.org/10.1002/ange.202112022
  14. M.A. Mahmud, T. Duong, J. Peng, Y. Wu, H. Shen et al., Origin of efficiency and stability enhancement in high-performing mixed dimensional 2D–3D perovskite solar cells: A review. Adv. Funct. Mater. 32, 2009164 (2022). https://doi.org/10.1002/adfm.202009164
  15. R. Azmi, E. Ugur, A. Seitkhan, F. Aljamaan, A.S. Subbiah et al., Damp heat–stable perovskite solar cells with tailored-dimensionality 2D/3D heterojunctions. Science 376, 73–77 (2022). https://doi.org/10.1126/science.abm5784
  16. M. Shao, T. Bie, L. Yang, Y. Gao, X. Jin et al., Over 21% efficiency stable 2D perovskite solar cells. Adv. Mater. 34, 2107211 (2022). https://doi.org/10.1002/adma.202107211
  17. A. Zhu, H. Gu, W. Li, J. Liao, J. Xia et al., Synergistic passivation with phenylpropylammonium bromide for efficient inverted perovskite solar cells. Small Methods 8, 2300428 (2024). https://doi.org/10.1002/smtd.202300428
  18. X. Chang, J.-X. Zhong, S. Li, Q. Yao, Y. Fang et al., Two-second-annealed 2D/3D perovskite films with graded energy funnels and toughened heterointerfaces for efficient and durable solar cells. Angew. Chem. Int. Ed. 62, e202309292 (2023). https://doi.org/10.1002/anie.202309292
  19. A.A. Sutanto, P. Caprioglio, N. Drigo, Y.J. Hofstetter, I. Garcia-Benito et al., 2D/3D perovskite engineering eliminates interfacial recombination losses in hybrid perovskite solar cells. Chem 7, 1903–1916 (2021). https://doi.org/10.1016/j.chempr.2021.04.002
  20. X. Jiang, J. Zhang, Y. Liu, Z. Wang, X. Liu et al., Dopant-free polymer/2D/3D perovskite solar cells with high stability. Nano Energy 90, 106521 (2021). https://doi.org/10.1016/j.nanoen.2021.106521
  21. F. Yang, P. Zhang, M.A. Kamarudin, G. Kapil, T. Ma et al., Addition effect of pyreneammonium iodide to methylammonium lead halide perovskite-2D/3D heterostructured perovskite with enhanced stability. Adv. Funct. Mater. 28, 1804856 (2018). https://doi.org/10.1002/adfm.201804856
  22. R. Azmi, D.S. Utomo, B. Vishal, S. Zhumagali, P. Dally et al., Double-side 2D/3D heterojunctions for inverted perovskite solar cells. Nature 628, 93–98 (2024). https://doi.org/10.1038/s41586-024-07189-3
  23. B. Fan, F. Lin, X. Wu, Z. Zhu, A.K.Y. Jen, Selenium-containing organic photovoltaic materials. Acc. Chem. Res. 54, 3906–3916 (2021). https://doi.org/10.1021/acs.accounts.1c00443
  24. R. Cao, K. Sun, C. Liu, Y. Mao, W. Guo et al., Structurally flexible 2D spacer for suppressing the electron–phonon coupling induced non-radiative decay in perovskite solar cells. Nano-Micro Lett. 16, 178 (2024). https://doi.org/10.1007/s40820-024-01401-9
  25. C. Tang, Y. Liu, Y. Zheng, A. Sun, J. Liang et al., Infiltrated 2D/3D heterojunction with tunable electric field landscape for robust inverted perovskite solar cells with over 24% efficiency. Small 20, 2306978 (2024). https://doi.org/10.1002/smll.202306978
  26. Y. Choi, D. Koo, G. Jeong, U. Kim, H. Kim et al., A vertically oriented two-dimensional Ruddlesden-Popper phase perovskite passivation layer for efficient and stable inverted perovskite solar cells. Energy Environ. Sci. 15, 3369–3378 (2022). https://doi.org/10.1039/D2EE00759B
  27. Q. Cheng, B. Wang, G. Huang, Y. Li, X. Li et al., Impact of strain relaxation on 2D Ruddlesden-Popper perovskite solar cells. Angew. Chem. Int. Ed. 61, e202208264 (2022). https://doi.org/10.1002/anie.202208264
  28. P. Liu, N. Han, W. Wang, R. Ran, W. Zhou et al., High-quality Ruddlesden-Popper perovskite film formation for high-performance perovskite solar cells. Adv. Mater. 33, 2002582 (2021). https://doi.org/10.1002/adma.202002582
  29. W. Kong, F. Zeng, Z. Su, T. Wang, L. Qiao et al., Oriented low-n Ruddlesden-Popper formamidinium-based perovskite for efficient and air stable solar cells. Adv. Energy Mater. 12, 2202704 (2022). https://doi.org/10.1002/aenm.202202704
  30. H.-H. Huang, T.-A. Yang, L.-Y. Su, C.-H. Chen, Y.-T. Chen et al., Thiophene-based polyelectrolyte boosts high-performance quasi-2D perovskite solar cells with ultralow energy loss. ACS Mater. Lett. 5, 1384–1394 (2023). https://doi.org/10.1021/acsmaterialslett.2c01104
  31. T. Zhang, Z. Miao, R. Zhao, F. Yuan, S. Peng et al., Optimization charge-carrier properties of 2D ruddlesden–popper perovskite for solar cells. ACS Energy Lett. 9, 2248–2256 (2024). https://doi.org/10.1021/acsenergylett.4c00724
  32. J. Lu, T. Yang, T. Niu, N. Bu, Y. Zhang et al., Formamidinium-based Ruddlesden-Popper perovskite films fabricated via two-step sequential deposition: Quantum well formation, physical properties and film-based solar cells. Energy Environ. Sci. 15, 1144–1155 (2022). https://doi.org/10.1039/D1EE02851K
  33. R. Jiang, T. Tian, B. Ke, Z. Kou, P. Müller-Buschbaum et al., Insights into the effects of oriented crystallization on the performance of quasi-two-dimensional perovskite solar cells. Next Mater. 1, 100044 (2023). https://doi.org/10.1016/j.nxmate.2023.100044
  34. X. Du, Y. Li, Z. Yu, C.M. Oh, Y. Zhang et al., Multi-functional ion-pairing additive for efficient quasi-2D perovskite light-emitting diodes and solar cells. Chem. Eng. J. 487, 150596 (2024). https://doi.org/10.1016/j.cej.2024.150596
  35. C. Xu, L. Cheng, Z. Li, X. Zheng, S. Shan et al., Fast solidification and slow growth strategy for high-performance quasi-2D perovskite solar cells. Adv. Energy Mater. 13, 2300168 (2023). https://doi.org/10.1002/aenm.202300168
  36. Q. Qu, J. Zhou, X. Xi, B. Wang, Z. Wan et al., Stable high conversion efficiency of quasi-2D perovskite solar cells via potassium iodide as additive. Chem. Eng. J. 466, 142999 (2023). https://doi.org/10.1016/j.cej.2023.142999
  37. S. Peng, Z. Miao, Y. Liang, R. Zhao, F. Yuan et al., Governing the dispersion of quasi-2D perovskite phases toward efficient and stable perovskite solar cells. Matter (2024). https://doi.org/10.1016/j.matt.2024.05.047
  38. R. Zhang, M. Li, Z. Liang, Y. Tang, C. Han et al., Synergistic effect of 4-hydroxypyridine for the vertical orientation of quasi-2D perovskite solar cells with enhanced efficiency. J. Phys. Chem. C 127, 14098–14106 (2023). https://doi.org/10.1021/acs.jpcc.3c02626
  39. Z. Zhou, L. Li, B. Li, J. Li, T. Liu et al., N-heterocyclic olefin type ionic liquid with innate soft Lewis base character as an effective additive for hybrid quasi-2D and 3D perovskite solar cells. Small 19, 2300013 (2023). https://doi.org/10.1002/smll.202300013
  40. T. Yue, K. Li, X. Li, N. Ahmad, H. Kang et al., A binary solution strategy enables high-efficiency quasi-2D perovskite solar cells with excellent thermal stability. ACS Nano 17, 14632–14643 (2023). https://doi.org/10.1021/acsnano.3c01908
  41. A.H. Coffey, S.J. Yang, M. Gómez, B.P. Finkenauer, T. Terlier et al., Controlling crystallization of quasi-2D perovskite solar cells: Incorporating bulky conjugated ligands. Adv. Energy Mater. 13, 2201501 (2023). https://doi.org/10.1002/aenm.202201501
  42. Y. Sun, S. Ji, C. Yu, W. Liu, K. Wang et al., Regulation of phase arrangement in 2D Ruddlesden-Popper perovskite films via anti-solvent method for efficient solar cells. Sol. Energy Mater. Sol. Cells 262, 112568 (2023). https://doi.org/10.1016/j.solmat.2023.112568
  43. Z. Pan, D. Peng, X. Zhao, W. Xu, Y. Bao et al., Side-chain functionalized polymer hole-transporting materials with defect passivation effect for highly efficient inverted quasi-2D perovskite solar cells. Adv. Funct. Mater. 33, 2304881 (2023). https://doi.org/10.1002/adfm.202304881
  44. L. Chen, E.K. Tekelenburg, K. Gahlot, M. Pitaro, J. Xi et al., In situ SnSe deposition as passivation for scalable and stable quasi-2D lead–tin perovskite solar cells. Energy Environ. Sci. 16, 5315–5324 (2023). https://doi.org/10.1039/D3EE02507A
  45. H. Wang, L. Deng, Y. Pan, X. Zhang, X. Li et al., Green solvent polishing enables highly efficient quasi-2D perovskite solar cells. ACS Appl. Mater. Interfaces 15, 36447–36456 (2023). https://doi.org/10.1021/acsami.3c08182
  46. Y. Chai, L. Wu, Y. Chen, G. Zhang, X. Guo et al., Tuning hole transport properties and perovskite crystallization via pyridine-based molecules for quasi-2D perovskite solar cells. Small 20, 2311569 (2024). https://doi.org/10.1002/smll.202311569
  47. Z. Qin, M. Pols, M. Qin, J. Zhang, H. Yan et al., Over-18%-efficiency quasi-2D Ruddlesden-Popper Pb–Sn mixed perovskite solar cells by compositional engineering. ACS Energy Lett. 8, 3188–3195 (2023). https://doi.org/10.1021/acsenergylett.3c00853
  48. D. Ren, X. Li, Z. Zhang, X. Chen, Z. Liu et al., Enhanced charge transfer in quasi-2D perovskite by formamidinium cation gradient incorporation for efficient and stable solar cells. Small (2024). https://doi.org/10.1002/smll.202401831
  49. R. Liu, Y. Yu, L. Deng, M. Xu, H. Ren et al., The synergistic effect of A-site cation engineering and phase regulation enables efficient and stable Ruddlesden-Popper perovskite solar cells. Chinese Chem. Lett. (2024). https://doi.org/10.1016/j.cclet.2024.109545
  50. H. Yao, T. Wu, Y. Xiao, L. Ding, Y. Hua et al., Regulating the crystallization and carrier dynamics for high-performance quasi-2D tin perovskite solar cells. ACS Mater. Lett. 5, 3203–3211 (2023). https://doi.org/10.1021/acsmaterialslett.3c01145
  51. H. Wang, Y. Pan, X. Li, Z. Shi, X. Zhang et al., Band alignment boosts over 17% efficiency quasi-2D perovskite solar cells via bottom-side phase manipulation. ACS Energy Lett. 7, 3187–3196 (2022). https://doi.org/10.1021/acsenergylett.2c01453
  52. G. Zhang, J. Tang, C. Wang, X. Wu, J. Chen et al., Antisolvent effects in green solvent engineering of FA-based quasi-2D Ruddlesden-Popper perovskite films for efficient solar cells. Green Chem. 26, 5347–5355 (2024). https://doi.org/10.1039/D4GC00235K
  53. J.-H. Kim, C.-M. Oh, I.-W. Hwang, J. Kim, C. Lee et al., Efficient and stable quasi-2D Ruddlesden-Popper perovskite solar cells by tailoring crystal orientation and passivating surface defects. Adv. Mater. 35, 2302143 (2023). https://doi.org/10.1002/adma.202302143
  54. D. Li, Z. Xing, X. Meng, X. Hu, T. Hu et al., Selection of functional spacer cations for efficient 2D/3D perovskite solar cells. CCS Chem 5, 781–801 (2023). https://doi.org/10.31635/ccschem.023.202202409
  55. A. Caiazzo, R.A.J. Janssen, High efficiency quasi-2D Ruddlesden-Popper perovskite solar cells. Adv. Energy Mater. 12, 2202830 (2022). https://doi.org/10.1002/aenm.202202830
  56. Q. Li, L. Zhou, T. Zhou, Fluorinated quasi 2D perovskite solar cells with improved stability and over 19% efficiency. Adv. Energy Mater. 14, 2400050 (2024). https://doi.org/10.1002/aenm.202400050
  57. H. Zheng, G. Liu, Y. Wang, F. Chen, X. Dong et al., Directional management self-additive spacer cations for stable 2D Ruddlesden-Popper perovskite solar cells with efficiency over 21%. Adv. Funct. Mater. 34, 2401546 (2024). https://doi.org/10.1002/adfm.202401546
  58. H. Zhang, R. Wang, L. Yang, Z. Hu, H. Liu et al., Modulating the dipole moment of secondary ammonium spacers for efficient 2D Ruddlesden-Popper perovskite solar cells. Angew. Chem. Int. Ed. 136, e202318206 (2024). https://doi.org/10.1002/ange.202318206
  59. Y. Zhang, M. Chen, T. He, H. Chen, Z. Zhang et al., Highly efficient and stable FA-based quasi-2D Ruddlesden-Popper perovskite solar cells by the incorporation of β-fluorophenylethanamine cations. Adv. Mater. 35, 2210836 (2023). https://doi.org/10.1002/adma.202210836
  60. X. Li, J.M. Hoffman, M.G. Kanatzidis, The 2D halide perovskite rulebook: How the spacer influences everything from the structure to optoelectronic device efficiency. Chem. Rev. 121, 2230–2291 (2021). https://doi.org/10.1021/acs.chemrev.0c01006
  61. Q. Cao, P. Li, W. Chen, S. Zang, L. Han et al., Two-dimensional perovskites: Impacts of species, components, and properties of organic spacers on solar cells. Nano Today 43, 101394 (2022). https://doi.org/10.1016/j.nantod.2022.101394
  62. C. Wang, X. Dong, F. Chen, G. Liu, H. Zheng, Recent progress of two-dimensional Ruddlesden-Popper perovskites in solar cells. Mater. Chem. Front. 7, 5786–5805 (2023). https://doi.org/10.1039/D3QM00547J
  63. Y. Gao, X. Dong, Y. Liu, Recent progress of layered perovskite solar cells incorporating aromatic spacers. Nano-Micro Lett. 15, 169 (2023). https://doi.org/10.1007/s40820-023-01141-2
  64. R. Stanton, D.J. Trivedi, Atomistic description of the impact of spacer selection on two-dimensional 2D perovskites: A case study of 2D Ruddlesden-Popper CsPbI3 analogues. J. Phys. Chem. Lett. 13, 12090–12098 (2022). https://doi.org/10.1021/acs.jpclett.2c03463
  65. T. Ji, T. Niu, J. Wang, R. Lu, Z. Wen et al., Crystallization regulation of solution-processed two-dimensional perovskite solar cells. J. Mater. Chem. A 10, 13625–13650 (2022). https://doi.org/10.1039/D2TA02574D
  66. N. Parikh, M.M. Tavakoli, M. Pandey, A. Kalam, D. Prochowicz et al., Role of the spacer cation in the growth and crystal orientation of two-dimensional perovskites. Sustain. Energy Fuels 5, 1255–1279 (2021). https://doi.org/10.1039/D0SE01469A
  67. N. Zhou, B. Huang, M. Sun, Y. Zhang, L. Li et al., The spacer cations interplay for efficient and stable layered 2D perovskite solar cells. Adv. Energy Mater. 10, 1901566 (2020). https://doi.org/10.1002/aenm.201901566
  68. S. Chen, N. Shen, L. Zhang, W. Kong, L. Zhang et al., Binary organic spacer-based quasi-two-dimensional perovskites with preferable vertical orientation and efficient charge transport for high-performance planar solar cells. J. Mater. Chem. A 7, 9542–9549 (2019). https://doi.org/10.1039/C8TA12476K
  69. S. Chen, N. Shen, L. Zhang, L. Zhang, S.H. Cheung et al., Understanding the interplay of binary organic spacer in Ruddlesden-Popper perovskites toward efficient and stable solar cells. Adv. Funct. Mater. 30, 1907759 (2020). https://doi.org/10.1002/adfm.201907759
  70. S. Tan, N. Zhou, Y. Chen, L. Li, G. Liu et al., Effect of high dipole moment cation on layered 2D organic–inorganic halide perovskite solar cells. Adv. Energy Mater. 9, 1803024 (2019). https://doi.org/10.1002/aenm.201803024
  71. G. Wu, T. Yang, X. Li, N. Ahmad, X. Zhang et al., Molecular engineering for two-dimensional perovskites with photovoltaic efficiency exceeding 18%. Matter 4, 582–599 (2021). https://doi.org/10.1016/j.matt.2020.11.011
  72. Y. Wang, D. Li, Z. Xing, J. Li, X. Hu et al., Quantum well growth management to smooth the energy transfer pathway for quasi-2D perovskite solar cells. Adv. Funct. (2024). https://doi.org/10.1002/adfm.202401203
  73. J. Xu, J. Chen, S. Chen, H. Gao, Y. Li et al., Organic spacer engineering of Ruddlesden-Popper perovskite materials toward efficient and stable solar cells. Chem. Eng. J. 453, 139790 (2023). https://doi.org/10.1016/j.cej.2022.139790
  74. M. Long, T. Zhang, D. Chen, M. Qin, Z. Chen et al., Interlayer interaction enhancement in Ruddlesden-Popper perovskite solar cells toward high efficiency and phase stability. ACS Energy Lett. 4, 1025–1033 (2019). https://doi.org/10.1021/acsenergylett.9b00351
  75. S. Wang, Y. Liu, J. Zou, J. Jin, Y. Jiang et al., Intermediate phase assisted sequential deposition of reverse-graded quasi-2D alternating cation perovskites for ma-free perovskite solar cells. InfoMat 5, e12396 (2023). https://doi.org/10.1002/inf2.12396
  76. A. Caiazzo, K. Datta, L. Bellini, M.M. Wienk, R.A. Janssen, Impact of alkyl chain length on the formation of regular- and reverse-graded quasi-2D perovskite thin films. ACS Mater. Lett. 6, 267–274 (2024). https://doi.org/10.1021/acsmaterialslett.3c01073
  77. X. Dong, Y. Li, X. Wang, Y. Zhou, Y. Zhao et al., Promoting Ruddlesden-Popper perovskite formation by tailoring spacer intramolecular interaction for efficient and stable solar cells. Small 40, 2309218 (2024). https://doi.org/10.1002/smll.202309218
  78. P. Li, L. Yan, Q. Cao, C. Liang, H. Zhu et al., Dredging the charge-carrier transfer pathway for efficient low-dimensional Ruddlesden-Popper perovskite solar cells. Angew. Chem. Int. Ed. 62, e202217910 (2023). https://doi.org/10.1002/anie.202217910
  79. H. Zheng, W. Wu, H. Xu, F. Zheng, G. Liu et al., Self-additive low-dimensional Ruddlesden-Popper perovskite by the incorporation of glycine hydrochloride for high-performance and stable solar cells. Adv. Funct. Mater. 30, 2000034 (2020). https://doi.org/10.1002/adfm.202000034
  80. H. Ren, S. Yu, L. Chao, Y. Xia, Y. Sun et al., Efficient and stable Ruddlesden-Popper perovskite solar cell with tailored interlayer molecular interaction. Nat. Photonics 14, 154–163 (2020). https://doi.org/10.1038/s41566-019-0572-6
  81. Y. Li, H. Cheng, K. Zhao, Z.-S. Wang, 4-(aminoethyl)pyridine as a bifunctional spacer cation for efficient and stable 2D Ruddlesden-Popper perovskite solar cells. ACS Appl. Mater. Interfaces 11, 37804–37811 (2019). https://doi.org/10.1021/acsami.9b13951
  82. H. Pan, Y. Zheng, W. He, W. Yang, X. Gong et al., Molecular interaction modulating Ruddlesden-Popper tin-based perovskite crystallization. J. Mater. Chem. A 11, 10319–10327 (2023). https://doi.org/10.1039/D3TA00873H
  83. R. Wang, X. Dong, Q. Ling, Z. Hu, Y. Gao et al., Nucleation and crystallization in 2D Ruddlesden-Popper perovskites using formamidinium-based organic semiconductor spacers for efficient solar cells. Angew. Chem. Int. Ed. 135, e202314690 (2023). https://doi.org/10.1002/ange.202314690
  84. D. Liang, C. Dong, L. Cai, Z. Su, J. Zang et al., Unveiling crystal orientation in quasi-2D perovskite films by in situ GIWAXS for high-performance photovoltaics. Small 17, 2100972 (2021). https://doi.org/10.1002/smll.202100972
  85. G. Wu, R. Liang, Z. Zhang, M. Ge, G. Xing et al., 2D hybrid halide perovskites: Structure, properties, and applications in solar cells. Small 17, 2103514 (2021). https://doi.org/10.1002/smll.202103514
  86. S. Shao, M.A. Loi, Advances and prospective in metal halide Ruddlesen-Popper perovskite solar cells. Adv. Energy Mater. 11, 2003907 (2021). https://doi.org/10.1002/aenm.202003907
  87. X. Dong, X. Li, X. Wang, Y. Zhao, W. Song et al., Improve the charge carrier transporting in two-dimensional Ruddlesden-Popper perovskite solar cells. Adv. Mater. 36, 2313056 (2024). https://doi.org/10.1002/adma.202313056
  88. J. Du, M. Zhang, J. Tian, Controlled crystal orientation of two-dimensional Ruddlesden-Popper halide perovskite films for solar cells. Int. J. Min. Met. Mater. 29, 49–58 (2022). https://doi.org/10.1007/s12613-021-2341-z
  89. L.E. Lehner, S. Demchyshyn, K. Frank, A. Minenkov, D.J. Kubicki et al., Elucidating the origins of high preferential crystal orientation in quasi-2D perovskite solar cells. Adv. Mater. 35, 2208061 (2023). https://doi.org/10.1002/adma.202208061
  90. Z. Lu, X. Xu, Y. Gao, Z. Wu, A. Li et al., The effect of spacer cations on optoelectronic properties of two-dimensional perovskite based on first-principles calculations. Surf. Int. 34, 102343 (2022). https://doi.org/10.1016/j.surfin.2022.102343
  91. X. Zhao, M.L. Ball, A. Kakekhani, T. Liu, A.M. Rappe et al., A charge transfer framework that describes supramolecular interactions governing structure and properties of 2D perovskites. Nat. Commun. 13, 3970 (2022). https://doi.org/10.1038/s41467-022-31567-y
  92. Q. Wei, F. Zhang, X. Li, F. Wu, Z. Yue et al., Directed assembly of ordered mixed-spacer quasi-2D halide perovskites through homomeric chains of intermolecular bonds. Small 20, 2311969 (2023). https://doi.org/10.1002/smll.202311969
  93. N. Marchal, E. Mosconi, G. García-Espejo, T.M. Almutairi, C. Quarti et al., Cation engineering for resonant energy level alignment in two-dimensional lead halide perovskites. J. Phys. Chem. Lett. 12, 2528–2535 (2021). https://doi.org/10.1021/acs.jpclett.0c03843
  94. L. Yan, J. Ma, P. Li, S. Zang, L. Han et al., Charge-carrier transport in quasi-2D Ruddlesden-Popper perovskite solar cells. Adv. Mater. 34, 2106822 (2022). https://doi.org/10.1002/adma.202106822
  95. L. Wang, B. Chang, H. Li, Y. Wu, Z. Liu et al., [PbX6]4− modulation and organic spacer construction for stable perovskite solar cells. Energy Environ. Sci. 15, 4470–4510 (2022). https://doi.org/10.1039/D2EE02218D
  96. C. Zheng, F. Zheng, Carrier transport in 2D hybrid organic-inorganic perovskites: The role of spacer molecules. J. Phys. Chem. Lett. 15, 1254–1263 (2024). https://doi.org/10.1021/acs.jpclett.3c03357
  97. L. Chao, T. Niu, Y. Xia, X. Ran, Y. Chen et al., Efficient and stable low-dimensional Ruddlesden-Popper perovskite solar cells enabled by reducing tunnel barrier. J. Phys. Chem. Lett. 10, 1173–1179 (2019). https://doi.org/10.1021/acs.jpclett.9b00276
  98. Z. Wang, F. Wang, B. Zhao, S. Qu, T. Hayat et al., Efficient two-dimensional tin halide perovskite light-emitting diodes via a spacer cation substitution strategy. J. Phys. Chem. Lett. 11, 1120–1127 (2020). https://doi.org/10.1021/acs.jpclett.9b03565
  99. G.C. Fish, A.T. Terpstra, A. Dučinskas, M. Almalki, L.C. Carbone et al., The impact of spacer size on charge transfer excitons in Dion-Jacobson and Ruddlesden-Popper layered hybrid perovskites. J. Phys. Chem. Lett. 14, 6248–6254 (2023). https://doi.org/10.1021/acs.jpclett.3c01125
  100. M. Chen, X. Dong, Y. Xin, Y. Gao, Q. Fu et al., Crystal growth regulation of Ruddlesden-Popper perovskites via self-assembly of semiconductor spacers for efficient solar cells. Angew. Chem. Int. Ed. 63, e202315943 (2024). https://doi.org/10.1002/anie.202315943
  101. J. Yang, T. He, M. Li, G. Li, H. Liu et al., π-conjugated carbazole cations enable wet-stable quasi-2D perovskite photovoltaics. ACS Energy Lett. 7, 4451–4458 (2022). https://doi.org/10.1021/acsenergylett.2c02219
  102. J. Guo, Z. Shi, J. Xia, K. Wang, Q. Wei et al., Phase tailoring of Ruddlesden-Popper perovskite at fixed large spacer cation ratio. Small 17, 2100560 (2021). https://doi.org/10.1002/smll.202100560
  103. W. Fu, T. Zhao, H. Liu, F. Lin, L. Zuo et al., High-efficiency quasi-2D perovskite solar cells incorporating 2,2’-biimidazolium cation. Sol. RRL 5, 2000700 (2021). https://doi.org/10.1002/solr.202000700
  104. H. Yao, Z. Li, C. Shi, Y. Xu, Q. Wang et al., A novel multiple-ring aromatic spacer based 2D Ruddlesden-Popper CsPbI3 solar cell with record efficiency beyond 16%. Adv. Funct. Mater. 32, 2205029 (2022). https://doi.org/10.1002/adfm.202205029
  105. Y. Zhang, M. Sun, N. Zhou, B. Huang, H. Zhou, Electronic tunability and mobility anisotropy of quasi-2D perovskite single crystals with varied spacer cations. J. Phys. Chem. Lett. 11, 7610–7616 (2020). https://doi.org/10.1021/acs.jpclett.0c02274
  106. Z. Wang, L. Liu, X. Liu, D. Song, D. Shi et al., Uncovering synergistic effect of chloride additives for efficient quasi-2D perovskite solar cells. Chem. Eng. J. 432, 134367 (2022). https://doi.org/10.1016/j.cej.2021.134367
  107. H. Di, Z. Xing, X. Xie, Y. Zhao, B.-H. Li, Effects of the phase spatial distribution on the intrinsic carrier dynamics in quasi-2D perovskite films. ACS Mater. Lett. 6, 2223–2230 (2024). https://doi.org/10.1021/acsmaterialslett.4c00038
  108. B.-H. Li, H. Di, H. Li, J.-C. Wang, W. Zeng et al., Unveiling the intrinsic photophysics in quasi-two-dimensional perovskites. J. Am. Chem. Soc. 146, 6974–6982 (2024). https://doi.org/10.1021/jacs.3c14737
  109. C. Luo, G. Zheng, F. Gao, X. Wang, Y. Zhao et al., Facet orientation tailoring via 2D-seed-induced growth enables highly efficient and stable perovskite solar cells. Joule 6, 240–257 (2022). https://doi.org/10.1016/j.joule.2021.12.006
  110. D. Wang, S.-C. Chen, Q. Zheng, Enhancing the efficiency and stability of two-dimensional Dion-Jacobson perovskite solar cells using a fluorinated diammonium spacer. J. Mater. Chem. A 9, 11778–11786 (2021). https://doi.org/10.1039/D1TA01447A
  111. J. Byeon, S.H. Cho, J. Jiang, J. Jang, C. Katan et al., Structural isomer of fluorinated Ruddlesden-Popper perovskites toward efficient and stable 2D/3D perovskite solar cells. ACS Appl. Mater. Interfaces 15, 27853–27864 (2023). https://doi.org/10.1021/acsami.3c01754
  112. J. Ovčar, T.L. Leung, L. Grisanti, Ž Skoko, M. Vrankić et al., Mixed halide ordering as a tool for the stabilization of Ruddlesden-Popper structures. Chem. Mater. 34, 4286–4297 (2022). https://doi.org/10.1021/acs.chemmater.1c03815
  113. H. Yao, Z. Li, G. Peng, Y. Lei, Q. Wang et al., Novel PHA organic spacer increases interlayer interactions for high efficiency in 2D Ruddlesden-Popper CsPbI3 solar cells. ACS Appl. Mater. Interfaces 14, 35780–35788 (2022). https://doi.org/10.1021/acsami.2c09183
  114. Z. Fang, X. Hou, Y. Zheng, Z. Yang, K.-C. Chou et al., First-principles optimization of out-of-plane charge transport in Dion-Jacobson CsPbI3 perovskites with π-conjugated aromatic spacers. Adv. Funct. Mater. 31, 2102330 (2021). https://doi.org/10.1002/adfm.202102330
  115. J. Xi, I. Spanopoulos, K. Bang, J. Xu, H. Dong et al., Alternative organic spacers for more efficient perovskite solar cells containing Ruddlesden-Popper phases. J. Am. Chem. Soc. 142, 19705–19714 (2020). https://doi.org/10.1021/jacs.0c09647
  116. M. Mittal, R. Garg, A. Jana, Recent progress in the stabilization of low band-gap black-phase iodide perovskite solar cells. Dalton T. 52, 11750–11767 (2023). https://doi.org/10.1039/D3DT01581E
  117. Z. Xu, L. Li, X. Dong, D. Lu, R. Wang et al., CsPbI3-based phase-stable 2D Ruddlesden-Popper perovskites for efficient solar cells. Nano Lett. 22, 2874–2880 (2022). https://doi.org/10.1021/acs.nanolett.2c00002
  118. C. Liu, R. Liu, Z. Bi, Y. Yu, G. Xu et al., Multiple-ring aromatic spacer cation tailored interlayer interaction for efficient and air-stable Ruddlesden-Popper perovskite solar cells. Sol. RRL 5, 2100495 (2021). https://doi.org/10.1002/solr.202100495
  119. J. Wu, J. Shi, Y. Li, H. Li, H. Wu et al., Quantifying the interface defect for the stability origin of perovskite solar cells. Adv. Energy Mater. 9, 1901352 (2019). https://doi.org/10.1002/aenm.201901352
  120. A.-F. Castro-Méndez, J. Hidalgo, J.-P. Correa-Baena, The role of grain boundaries in perovskite solar cells. Adv. Energy Mater. 9, 1901489 (2019). https://doi.org/10.1002/aenm.201901489
  121. K. Li, X. Gan, R. Zheng, H. Zhang, M. Xiang et al., Comparative analysis of thiophene-based interlayer cations for enhanced performance in 2D Ruddlesden-Popper perovskite solar cells. ACS Appl. Mater. Interfaces 16, 7161–7170 (2024). https://doi.org/10.1021/acsami.3c16640
  122. B. Primera Darwich, N. Guijarro, H.-H. Cho, L. Yao, L. Monnier et al., Benzodithiophene-based spacers for layered and quasi-layered lead halide perovskite solar cells. ChemSusChem 14, 3001–3009 (2021). https://doi.org/10.1002/cssc.202100992
  123. W. Guo, J. Li, H. Cen, J. Duan, Y. Yang et al., Self-assembled molecules fostering ordered spatial heterogeneity for efficient Ruddlesden-Popper perovskite solar cells. Adv. Energy Mater. (2024). https://doi.org/10.1002/aenm.202401303
  124. B. Wang, Q. Cheng, G. Huang, Y. Yue, W. Zhang et al., Sulfonium-cations-assisted intermediate engineering for quasi-2D perovskite solar cells. Adv. Mater. 35, 2207345 (2023). https://doi.org/10.1002/adma.202207345
  125. J. Zhang, J. Wu, Y. Zhao, Y. Zou, A. Barabash et al., Revealing the crystallization and thermal-induced phase evolution in aromatic-based quasi-2D perovskites using a robot-based platform. ACS Energy Lett. 8, 3595–3603 (2023). https://doi.org/10.1021/acsenergylett.3c01508
  126. C.J. Dahlman, R.M. Kennard, P. Paluch, N.R. Venkatesan, M.L. Chabinyc et al., Dynamic motion of organic spacer cations in Ruddlesden-Popper lead iodide perovskites probed by solid-state nmr spectroscopy. Chem. Mater. 33, 642–656 (2021). https://doi.org/10.1021/acs.chemmater.0c03958
  127. Y. Miao, Y. Chen, H. Chen, X. Wang, Y. Zhao, Using steric hindrance to manipulate and stabilize metal halide perovskites for optoelectronics. Chem. Sci. 12, 7231–7247 (2021). https://doi.org/10.1039/D1SC01171E
  128. Z. Gozukara Karabag, A. Karabag, U. Gunes, X.-X. Gao, O.A. Syzgantseva et al., Tuning 2D perovskite passivation: Impact of electronic and steric effects on the performance of 3D/2D perovskite solar cells. Adv. Energy Mater. 13, 2302038 (2023). https://doi.org/10.1002/aenm.202302038
  129. L. Yang, Y. Jin, Z. Fang, J. Zhang, Z. Nan et al., Efficient semi-transparent wide-bandgap perovskite solar cells enabled by pure-chloride 2D-perovskite passivation. Nano-Micro Lett. 15, 111 (2023). https://doi.org/10.1007/s40820-023-01090-w
  130. Z. Li, N. Liu, K. Meng, Z. Liu, Y. Hu et al., A new organic interlayer spacer for stable and efficient 2D Ruddlesden-Popper perovskite solar cells. Nano Lett. 19, 5237–5245 (2019). https://doi.org/10.1021/acs.nanolett.9b01652
  131. H. Wang, Z. Dong, H. Liu, W. Li, L. Zhu et al., Roles of organic molecules in inorganic CsPbX3 perovskite solar cells. Adv. Energy Mater. 11, 2002940 (2021). https://doi.org/10.1002/aenm.202002940
  132. J. Zhang, J. Wu, S. Langner, B. Zhao, Z. Xie et al., Exploring the steric hindrance of alkylammonium cations in the structural reconfiguration of quasi-2D perovskite materials using a high-throughput experimental platform. Adv. Funct. Mater. 32, 2207101 (2022). https://doi.org/10.1002/adfm.202207101
  133. F. Li, Y. Xie, Y. Hu, M. Long, Y. Zhang et al., Effects of alkyl chain length on crystal growth and oxidation process of two-dimensional tin halide perovskites. ACS Energy Lett. 5, 1422–1429 (2020). https://doi.org/10.1021/acsenergylett.0c00286
  134. C. Chen, L. Gao, W. Gao, C. Ge, X. Du et al., Circularly polarized light detection using chiral hybrid perovskite. Nat. Commun. 10, 1927 (2019). https://doi.org/10.1038/s41467-019-09942-z
  135. L. Wang, Y. Xue, M. Cui, Y. Huang, H. Xu et al., A chiral reduced-dimension perovskite for an efficient flexible circularly polarized light photodetector. Angew. Chem. Int. Ed. 132, 6504–6512 (2020). https://doi.org/10.1002/ange.201915912
  136. Y. Qin, F.-F. Gao, S. Qian, T.-M. Guo, Y.-J. Gong et al., Multifunctional chiral 2D lead halide perovskites with circularly polarized photoluminescence and piezoelectric energy harvesting properties. ACS Nano 16, 3221–3230 (2022). https://doi.org/10.1021/acsnano.1c11101
  137. T. Liu, W. Shi, W. Tang, Z. Liu, B.C. Schroeder et al., High responsivity circular polarized light detectors based on quasi two-dimensional chiral perovskite films. ACS Nano 16, 2682–2689 (2022). https://doi.org/10.1021/acsnano.1c09521
  138. J. Son, S. Ma, Y.-K. Jung, J. Tan, G. Jang et al., Unraveling chirality transfer mechanism by structural isomer-derived hydrogen bonding interaction in 2D chiral perovskite. Nat. Commun. 14, 3124 (2023). https://doi.org/10.1038/s41467-023-38927-2
  139. A. Shpatz Dayan, M. Wierzbowska, L. Etgar, Ruddlesden-Popper 2D chiral perovskite-based solar cells. Small Struct. 3, 2200051 (2022). https://doi.org/10.1002/sstr.202200051
  140. L. Scalon, Y. Vaynzof, A.F. Nogueira, C.C. Oliveira, How organic chemistry can affect perovskite photovoltaics. Cell Rep. Phys. Sci. 4, 1010358 (2023). https://doi.org/10.1016/j.xcrp.2023.101358
  141. Z. Wang, Q. Wei, X. Liu, L. Liu, X. Tang et al., Spacer cation tuning enables vertically oriented and graded quasi-2D perovskites for efficient solar cells. Adv. Funct. Mater. 31, 2008404 (2021). https://doi.org/10.1002/adfm.202008404
  142. Q. Fu, M. Chen, Q. Li, H. Liu, R. Wang et al., Selenophene-based 2D Ruddlesden-Popper perovskite solar cells with an efficiency exceeding 19%. J. Am. Chem. Soc. 145, 21687–21695 (2023). https://doi.org/10.1021/jacs.3c08604
  143. G. Li, Z. Su, L. Canil, D. Hughes, M.H. Aldamasy et al., Highly efficient p-i-n perovskite solar cells that endure temperature variations. Science 379, 399–403 (2023). https://doi.org/10.1126/science.add7331
  144. S. Zhao, J. Xie, G. Cheng, Y. Xiang, H. Zhu et al., General nondestructive passivation by 4-fluoroaniline for perovskite solar cells with improved performance and stability. Small 14, 1803350 (2018). https://doi.org/10.1002/smll.201803350
  145. H. Pan, X. Zhao, X. Gong, Y. Shen, M. Wang, Atomic-scale tailoring of organic cation of layered Ruddlesden-Popper perovskite compounds. J. Phys. Chem. Lett. 10, 1813–1819 (2019). https://doi.org/10.1021/acs.jpclett.9b00479
  146. H. Su, L. Zhang, Y. Liu, Y. Hu, B. Zhang et al., Polarity regulation for stable 2D-perovskite-encapsulated high-efficiency 3D-perovskite solar cells. Nano Energy 95, 106965 (2022). https://doi.org/10.1016/j.nanoen.2022.106965
  147. Y. Zeng, R. Wang, K. Chen, X. Gao, X. Liu et al., Molecular engineering of 2D spacer cations to achieve efficient and stable 2D/3D perovskite solar cells. Sol. RRL 8, 2301077 (2024). https://doi.org/10.1002/solr.202301077
  148. C. Shi, Z. Li, K. Kang, X. Zhou, H. Wang et al., Fluorosubstitution boosting 2D Ruddlesden-Popper CsPbI3 with high stability and efficiency. Sol. RRL 6, 2200694 (2022). https://doi.org/10.1002/solr.202200694
  149. Y. Yan, S. Yu, A. Honarfar, T. Pullerits, K. Zheng et al., Benefiting from spontaneously generated 2D/3D bulk-heterojunctions in Ruddlesden−Popper perovskite by incorporation of S-bearing spacer cation. Adv. Sci. 6, 1900548 (2019). https://doi.org/10.1002/advs.201900548
  150. Q. Zhou, Q. Xiong, Z. Zhang, J. Hu, F. Lin et al., Fluoroaromatic cation-assisted planar junction perovskite solar cells with improved VOC and stability: The role of fluorination position. Sol. RRL 4, 2000107 (2020). https://doi.org/10.1002/solr.202000107
  151. Y. Liu, S. Han, J. Wang, Y. Ma, W. Guo et al., Spacer cation alloying of a homoconformational carboxylate trans isomer to boost in-plane ferroelectricity in a 2D hybrid perovskite. J. Am. Chem. Soc. 143, 2130–2137 (2021). https://doi.org/10.1021/jacs.0c12513
  152. M.A. Hope, T. Nakamura, P. Ahlawat, A. Mishra, M. Cordova et al., Nanoscale phase segregation in supramolecular π-templating for hybrid perovskite photovoltaics from nmr crystallography. J. Am. Chem. Soc. 143, 1529–1538 (2021). https://doi.org/10.1021/jacs.0c11563
  153. A.M. Najarian, M. Vafaie, R. Sabatini, S. Wang, P. Li et al., 2D hybrid perovskites employing an organic cation paired with a neutral molecule. J. Am. Chem. Soc. 145, 27242–27247 (2023). https://doi.org/10.1021/jacs.3c12172
  154. A. Morteza Najarian, F. Dinic, H. Chen, R. Sabatini, C. Zheng et al., Homomeric chains of intermolecular bonds scaffold octahedral germanium perovskites. Nature 620, 328–335 (2023). https://doi.org/10.1038/s41586-023-06209-y
  155. W. Yu, Y. Zou, H. Wang, S. Qi, C. Wu et al., Breaking the bottleneck of lead-free perovskite solar cells through dimensionality modulation. Chem. Soc. Rev. 53, 1769–1788 (2024). https://doi.org/10.1039/D3CS00728F
  156. W. Fu, H. Liu, X. Shi, L. Zuo, X. Li et al., Tailoring the functionality of organic spacer cations for efficient and stable quasi-2D perovskite solar cells. Adv. Funct. Mater. 29, 1900221 (2019). https://doi.org/10.1002/adfm.201900221
  157. Y. Dong, D. Lu, Z. Xu, H. Lai, Y. Liu, 2-Thiopheneformamidinium-based 2D Ruddlesden-Popper perovskite solar cells with efficiency of 16.72% and negligible hysteresis. Adv. Energy Mater. 10, 2000694 (2020). https://doi.org/10.1002/aenm.202000694
  158. M. Kundar, S. Bhandari, S. Chung, K. Cho, S.K. Sharma et al., Surface passivation by sulfur-based 2D (TEA)2PbI4 for stable and efficient perovskite solar cells. ACS Omega 8, 12842–12852 (2023). https://doi.org/10.1021/acsomega.2c08126
  159. C. Chen, J. Liang, J. Zhang, X. Liu, X. Yin et al., Interfacial engineering of a thiophene-based 2D/3D perovskite heterojunction for efficient and stable inverted wide-bandgap perovskite solar cells. Nano Energy 90, 106608 (2021). https://doi.org/10.1016/j.nanoen.2021.106608
  160. Y. Xu, K.-J. Jiang, P. Wang, W.-M. Gu, G.-H. Yu et al., Highly oriented quasi-2D layered tin halide perovskites with 2-thiopheneethylammonium iodide for efficient and stable tin perovskite solar cells. New J. Chem. 46, 2259–2265 (2022). https://doi.org/10.1039/D1NJ05178D
  161. Y. Zheng, S.-C. Chen, Y. Ma, Q. Zheng, Furfurylammonium as a spacer for efficient 2D Ruddlesden-Popper perovskite solar cells. Sol. RRL 6, 2200221 (2022). https://doi.org/10.1002/solr.202200221
  162. H. Tsuji, E. Nakamura, Design and functions of semiconducting fused polycyclic furans for optoelectronic applications. Acc. Chem. Res. 50, 396–406 (2017). https://doi.org/10.1021/acs.accounts.6b00595
  163. L.A. Illicachi, J. Urieta-Mora, C. Momblona, A. Molina-Ontoria, J. Calbo et al., Selenophene-based hole-transporting materials for perovskite solar cells. ChemPlusChem 86, 1006–1013 (2021). https://doi.org/10.1002/cplu.202100208
  164. R. Wang, X. Dong, Q. Ling, Q. Fu, Z. Hu et al., Spacer engineering for 2D Ruddlesden-Popper perovskites with an ultralong carrier lifetime of over 18 μs enable efficient solar cells. ACS Energy Lett. 7, 3656–3665 (2022). https://doi.org/10.1021/acsenergylett.2c01800
  165. M.-H. Jung, Highly stable thiophene perovskite enabled by an oxygen-containing moiety for efficient photovoltaics. J. Phys. Chem. C 125, 25430–25445 (2021). https://doi.org/10.1021/acs.jpcc.1c08095
  166. Y. Guo, M. Sun, W. Yang, S. Yuan, H. Xiong et al., Enhanced charge transport by regulating the electronic structure in 2D tin-based perovskite solar cells. J. Phys. Chem. C 126, 9425–9436 (2022). https://doi.org/10.1021/acs.jpcc.2c02830
  167. D. Fu, Z. Hou, Y. He, H. Wu, S. Wu et al., Formamidinium perovskitizers and aromatic spacers synergistically building bilayer Dion-Jacobson perovskite photoelectric bulk crystals. ACS Appl. Mater. Interfaces 14, 11690–11698 (2022). https://doi.org/10.1021/acsami.2c00806
  168. X. Li, W. Ke, B. Traoré, P. Guo, I. Hadar et al., Two-dimensional Dion-Jacobson hybrid lead iodide perovskites with aromatic diammonium cations. J. Am. Chem. Soc. 141, 12880–12890 (2019). https://doi.org/10.1021/jacs.9b06398
  169. S. Ahmad, M. Guan, J. Kim, X. He, Z. Ren et al., High-quality pure-phase MA-free formamdinium Dion-Jacobson 2D perovskites for stable unencapsulated photovoltaics. Adv. Energy Mater. 14, 2302774 (2024). https://doi.org/10.1002/aenm.202302774
  170. T. He, S. Li, Y. Jiang, C. Qin, M. Cui et al., Reduced-dimensional perovskite photovoltaics with homogeneous energy landscape. Nat. Commun. 11, 1672 (2020). https://doi.org/10.1038/s41467-020-15451-1
  171. E. Mahal, S.C. Mandal, B. Pathak, Band edge engineering of 2D perovskite structures through spacer cation engineering for solar cell applications. J. Phys. Chem. C 126, 9937–9947 (2022). https://doi.org/10.1021/acs.jpcc.2c01840
  172. C. Liu, Z. Fang, J. Sun, Q. Lou, J. Ge et al., Imidazolium ionic liquid as organic spacer for tuning the excitonic structure of 2D perovskite materials. ACS Energy Lett. 5, 3617–3627 (2020). https://doi.org/10.1021/acsenergylett.0c01784
  173. Y. Lao, S. Yang, W. Yu, H. Guo, Y. Zou et al., Multifunctional π-conjugated additives for halide perovskite. Adv. Sci. 9, 2105307 (2022). https://doi.org/10.1002/advs.202105307
  174. Z. Xu, D. Lu, F. Liu, H. Lai, X. Wan et al., Phase distribution and carrier dynamics in multiple-ring aromatic spacer-based two-dimensional Ruddlesden-Popper perovskite solar cells. ACS Nano 14, 4871–4881 (2020). https://doi.org/10.1021/acsnano.0c00875
  175. W. Yang, Y. Zhan, F. Yang, Y. Li, Hot-casting and anti-solvent free fabrication of efficient and stable two-dimensional Ruddlesden-Popper perovskite solar cells. ACS Appl. Mater. Interfaces 13, 61039–61046 (2021). https://doi.org/10.1021/acsami.1c17169
  176. X. Dong, M. Chen, R. Wang, Q. Ling, Z. Hu et al., Quantum confinement breaking: Orbital coupling in 2D Ruddlesden-Popper perovskites enables efficient solar cells. Adv. Energy Mater. 13, 2301006 (2023). https://doi.org/10.1002/aenm.202301006
  177. R. Yang, R. Li, Y. Cao, Y. Wei, Y. Miao et al., Oriented quasi-2D perovskites for high performance optoelectronic devices. Adv. Mater. 30, 1804771 (2018). https://doi.org/10.1002/adma.201804771
  178. T. Liu, J. Guo, D. Lu, Z. Xu, Q. Fu et al., Spacer engineering using aromatic formamidinium in 2D/3D hybrid perovskites for highly efficient solar cells. ACS Nano 15, 7811–7820 (2021). https://doi.org/10.1021/acsnano.1c02191
  179. X. Li, W. Hu, Y. Shang, X. Yu, X. Wang et al., Phenylformamidinium-enabled quasi-2D Ruddlesden-Popper perovskite solar cells with improved stability. J. Energy Chem. 66, 680–688 (2022). https://doi.org/10.1016/j.jechem.2021.09.026
  180. Z. Wang, X. Liu, H. Ren, L. Liu, X. Tang et al., Insight into the enhanced charge transport in quasi-2D perovskite via fluorination of ammonium cations for photovoltaic applications. ACS Appl. Mater. Interfaces 14, 7917–7925 (2022). https://doi.org/10.1021/acsami.1c21715
  181. H. Zhang, Z. Wang, H. Wang, X. Yao, F. Wang et al., Strain relaxation and phase regulation in quasi-2D perovskites for efficient solar cells. J. Mater. Chem. A 11, 15301–15310 (2023). https://doi.org/10.1039/D3TA01935G
  182. X. Lai, W. Li, X. Gu, H. Chen, Y. Zhang et al., High-performance quasi-2D perovskite solar cells with power conversion efficiency over 20% fabricated in humidity-controlled ambient air. Chem. Eng. J. 427, 130949 (2022). https://doi.org/10.1016/j.cej.2021.130949
  183. G. Liu, X.-X. Xu, S. Xu, L. Zhang, H. Xu et al., Passivation effect of halogenated benzylammonium as a second spacer cation for improved photovoltaic performance of quasi-2D perovskite solar cells. J. Mater. Chem. A 8, 5900–5906 (2020). https://doi.org/10.1039/C9TA14139A
  184. J. Shi, Y. Gao, X. Gao, Y. Zhang, J. Zhang et al., Fluorinated low-dimensional Ruddlesden-Popper perovskite solar cells with over 17% power conversion efficiency and improved stability. Adv. Mater. 31, 1901673 (2019). https://doi.org/10.1002/adma.201901673
  185. S. Lu, K. Li, R. Zhen, M. Xiang, X. Gan et al., Incorporating formamidinium into 4-fluoro-phenethylammonium based quasi-2D perovskite films and their application in n-i-p perovskite solar cells. Opt. Mater. 136, 113453 (2023). https://doi.org/10.1016/j.optmat.2023.113453
  186. J. Hu, I.W.H. Oswald, S.J. Stuard, M.M. Nahid, N. Zhou et al., Synthetic control over orientational degeneracy of spacer cations enhances solar cell efficiency in two-dimensional perovskites. Nat. Commun. 10, 1276 (2019). https://doi.org/10.1038/s41467-019-08980-x
  187. L. Sun, X. Cao, J. Wang, X. Tan, H. Huang et al., Synergistic effect of dual anions for efficient and stable quasi 2D perovskite solar cell. J. Alloy. Compd. 918, 165725 (2022). https://doi.org/10.1016/j.jallcom.2022.165725
  188. G. Yan, G. Sui, W. Chen, K. Su, Y. Feng et al., Selectively fluorinated benzylammonium-based spacer cation enables graded quasi-2D perovskites for efficient and stable solar cells. Chem. Mater. 34, 3346–3356 (2022). https://doi.org/10.1021/acs.chemmater.2c00146
  189. H. Lai, Z. Xu, Z. Shao, B. Cui, B. Tian et al., Rational regulation of organic spacer cations for quasi-2D perovskite solar cells. Sol. RRL 7, 2300132 (2023). https://doi.org/10.1002/solr.202300132
  190. Q. Li, Y. Dong, G. Lv, T. Liu, D. Lu et al., Fluorinated aromatic formamidinium spacers boost efficiency of layered Ruddlesden-Popper perovskite solar cells. ACS Energy Lett. 6, 2072–2080 (2021). https://doi.org/10.1021/acsenergylett.1c00620
  191. F. Zhang, D.H. Kim, H. Lu, J.-S. Park, B.W. Larson et al., Enhanced charge transport in 2D perovskites via fluorination of organic cation. J. Am. Chem. Soc. 141, 5972–5979 (2019). https://doi.org/10.1021/jacs.9b00972
  192. T. Niu, J. Lu, X. Jia, Z. Xu, M.-C. Tang et al., Interfacial engineering at the 2D/3D heterojunction for high-performance perovskite solar cells. Nano Lett. 19, 7181–7190 (2019). https://doi.org/10.1021/acs.nanolett.9b02781
  193. L. Wang, Q. Zhou, Z. Zhang, W. Li, X. Wang et al., A guide to use fluorinated aromatic bulky cations for stable and high-performance 2D/3D perovskite solar cells: The more fluorination the better? J. Energy Chem. 64, 179–189 (2022). https://doi.org/10.1016/j.jechem.2021.04.063
  194. J. Hu, I.W.H. Oswald, H. Hu, S.J. Stuard, M.M. Nahid et al., Aryl-perfluoroaryl interaction in two-dimensional organic–inorganic hybrid perovskites boosts stability and photovoltaic efficiency. ACS Mater. Lett. 1, 171–176 (2019). https://doi.org/10.1021/acsmaterialslett.9b00102
  195. X. Dong, Y. Tang, Y. Li, X. Li, Y. Zhao et al., Boosting MA-based two-dimensional Ruddlesen-Popper perovskite solar cells by incorporating a binary spacer. J. Energy Chem. 95, 348–356 (2024). https://doi.org/10.1016/j.jechem.2024.03.047
  196. B.-E. Cohen, M. Wierzbowska, L. Etgar, High efficiency quasi 2D lead bromide perovskite solar cells using various barrier molecules. Sustain. Energy Fuels 1, 1935–1943 (2017). https://doi.org/10.1039/C7SE00311K
  197. H. Xiang, P. Liu, R. Ran, W. Wang, W. Zhou et al., Two-dimensional Dion-Jacobson halide perovskites as new-generation light absorbers for perovskite solar cells. Renew. Sust. Energy Rev. 166, 112614 (2022). https://doi.org/10.1016/j.rser.2022.112614
  198. J. Meng, D. Song, D. Huang, Y. Li, Y. Li et al., Enhanced Voc of two-dimensional ruddlesden–popper perovskite solar cells using binary synergetic organic spacer cations. Phys. Chem. Chem. Phys. 22, 54–61 (2020). https://doi.org/10.1039/C9CP04018H
  199. P. Cheng, Z. Xu, J. Li, Y. Liu, Y. Fan et al., Highly efficient Ruddlesden-Popper halide perovskite PA2MA4Pb5I16 solar cells. ACS Energy Lett. 3, 1975–1982 (2018). https://doi.org/10.1021/acsenergylett.8b01153
  200. Y. Chen, Y. Sun, J. Peng, W. Zhang, X. Su et al., Tailoring organic cation of 2D air-stable organometal halide perovskites for highly efficient planar solar cells. Adv. Energy Mater. 7, 1700162 (2017). https://doi.org/10.1002/aenm.201700162
  201. H. Lai, D. Lu, Z. Xu, N. Zheng, Z. Xie et al., Organic-salt-assisted crystal growth and orientation of quasi-2D Ruddlesden-Popper perovskites for solar cells with efficiency over 19%. Adv. Mater. 32, 2001470 (2020). https://doi.org/10.1002/adma.202001470
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