Issue

Vol. 17 (2025)

Grain Boundaries Contribute to the Performance of Perovskite Solar Cells by Promoting Charge Separations

https://doi.org/10.1007/s40820-025-01795-0
Peng Xu
Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, People’s Republic of China
Pengfei Wang
Key Laboratory of Materials Modification By Laser, Ion and Electron Beams (Ministry of Education), School of Physics, Dalian University of Technology, Dalian 116024, People’s Republic of China
Minhuan Wang
Key Laboratory of Materials Modification By Laser, Ion and Electron Beams (Ministry of Education), School of Physics, Dalian University of Technology, Dalian 116024, People’s Republic of China
Fengke Sun
State Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
Jing Leng
State Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
Yantao Shi
State Key Laboratory of Fine Chemicals, School of Chemistry, Frontier Science Center for Smart Materials, Dalian University of Technology, Dalian 116024, People’s Republic of China
Shengye Jin
Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, People’s Republic of China
Wenming Tian
State Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China

Corresponding Author: Wenming Tian

tianwm@dicp.ac.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 285

Abstract

Historically seen as a limitation, grain boundaries (GBs) within polycrystalline metal halide perovskite (MHP) films are thought to impede charge transport, adversely impacting the efficiency of perovskite solar cells (PSCs). In this study, we employ home-built confocal photoluminescence microscopy, combined with photocurrent detection modules, to directly visualize the carrier dynamics in the MHP film of PSCs under real operating conditions. Our findings suggest that GBs in high-efficiency PSCs function as carrier transport channels, where a notable enhancement in photocurrent is observed. Femtosecond transient absorption and Kelvin probe force microscopy measurements further validate the existence of a built-in electric field in the vicinity of GBs, offering additional driving force for charge separation and establishing channels for swift carrier transport along the GBs, thereby expediting subsequent charge collection processes. This study elucidates the pivotal role of GBs in operational PSCs and provides valuable insights for the fabrication of high-efficiency PSCs.


Highlights:
1 Sub-micrometer-resolved photocurrent mapping in operational perovskite solar cells, achieved through our home-built photoluminescence and photocurrent imaging microscopy, reveals enhanced photocurrent at grain boundaries compared to grain interiors.
2 Local pump-probe femtosecond transient absorption and Kelvin probe force microscopy measurements corroborate the presence of a built-in electric field in the vicinity of grain boundaries that promotes electron–hole separation and the subsequent charge collection, thereby contributing to the performance of perovskite solar cells.

Keywords

Perovskite solar cells Grain boundary Photocurrent mapping Stark effect Carrier dynamics
Xu, Peng, Pengfei Wang, Minhuan Wang, Fengke Sun, Jing Leng, Yantao Shi, Shengye Jin, and Wenming Tian. 2025. “Grain Boundaries Contribute to the Performance of Perovskite Solar Cells by Promoting Charge Separations”. Nano-Micro Letters 17 (June):285. https://doi.org/10.1007/s40820-025-01795-0.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. M. Köhler, M. Pomaska, P. Procel, R. Santbergen, A. Zamchiy et al., A silicon carbide-based highly transparent passivating contact for crystalline silicon solar cells approaching efficiencies of 24%. Nat. Energy 6(5), 529–537 (2021). https://doi.org/10.1038/s41560-021-00806-9
  2. J. Zheng, Z. Ying, Z. Yang, Z. Lin, H. Wei et al., Polycrystalline silicon tunnelling recombination layers for high-efficiency perovskite/tunnel oxide passivating contact tandem solar cells. Nat. Energy 8(11), 1250–1261 (2023). https://doi.org/10.1038/s41560-023-01382-w
  3. Y. Chen, N. Yang, G. Zheng, F. Pei, W. Zhou et al., Nuclei engineering for even halide distribution in stable perovskite/silicon tandem solar cells. Science 385(6708), 554–560 (2024). https://doi.org/10.1126/science.ado9104
  4. C. Yu, Q. Zou, Q. Wang, Y. Zhao, X. Ran et al., Silicon solar cell with undoped tin oxide transparent electrode. Nat. Energy 8(10), 1119–1125 (2023). https://doi.org/10.1038/s41560-023-01331-7
  5. E. Aydin, E. Ugur, B.K. Yildirim, T.G. Allen, P. Dally et al., Enhanced optoelectronic coupling for perovskite/silicon tandem solar cells. Nature 623, 732–738 (2023). https://doi.org/10.1038/s41586-023-06667-4
  6. W.K. Metzger, S. Grover, D. Lu, E. Colegrove, J. Moseley et al., Exceeding 20% efficiency with in situ group V doping in polycrystalline CdTe solar cells. Nat. Energy 4(10), 837–845 (2019). https://doi.org/10.1038/s41560-019-0446-7
  7. J. Kwon, M. Seol, J. Yoo, H. Ryu, D.-S. Ko et al., 200-mm-wafer-scale integration of polycrystalline molybdenum disulfide transistors. Nat. Electron. 7(5), 356–364 (2024). https://doi.org/10.1038/s41928-024-01158-4
  8. Y. Magari, T. Kataoka, W. Yeh, M. Furuta, High-mobility hydrogenated polycrystalline In2O3 (In2O3: H) thin-film transistors. Nat. Commun. 13(1), 1078 (2022). https://doi.org/10.1038/s41467-022-28480-9
  9. Y.-S. Shiah, K. Sim, Y. Shi, K. Abe, S. Ueda et al., Mobility–stability trade-off in oxide thin-film transistors. Nat. Electron. 4(11), 800–807 (2021). https://doi.org/10.1038/s41928-021-00671-0
  10. H. Wu, Q. Wang, A. Zhang, G. Niu, M. Nikl et al., One-dimensional scintillator film with benign grain boundaries for high-resolution and fast X-ray imaging. Sci. Adv. 9(30), eadh1789 (2023). https://doi.org/10.1126/sciadv.adh1789
  11. D. Yang, X.L. Shi, M. Li, M. Nisar, A. Mansoor et al., Flexible power generators by Ag2Se thin films with record-high thermoelectric performance. Nat. Commun. 15(1), 923 (2024). https://doi.org/10.1038/s41467-024-45092-7
  12. D. Wang, J. Ding, Y. Ma, C. Xu, Z. Li et al., Multi-heterojunctioned plastics with high thermoelectric figure of merit. Nature 632(8025), 528–535 (2024). https://doi.org/10.1038/s41586-024-07724-2
  13. O. Auciello, D.M. Aslam, Review on advances in microcrystalline, nanocrystalline and ultrananocrystalline diamond films-based micro/nano-electromechanical systems technologies. J. Mater. Sci. 56(12), 7171–7230 (2021). https://doi.org/10.1007/s10853-020-05699-9
  14. L. Zhao, P. Tang, D. Luo, M.I. Dar, F.T. Eickemeyer et al., Enabling full-scale grain boundary mitigation in polycrystalline perovskite solids. Sci. Adv. 8(35), eabo3733 (2022). https://doi.org/10.1126/sciadv.abo3733
  15. W.D. Callister Jr., D.G. Rethwisch, Materials science and engineering: an introduction (John wiley & sons, Hoboken, 2020), pp.106–109
  16. Y. Zou, X. Bai, S. Kahmann, L. Dai, S. Yuan et al., A practical approach toward highly reproducible and high-quality perovskite films based on an aging treatment. Adv. Mater. 36(1), 2307024 (2024). https://doi.org/10.1002/adma.202307024
  17. Z. Chu, M. Yang, P. Schulz, D. Wu, X. Ma et al., Impact of grain boundaries on efficiency and stability of organic-inorganic trihalide perovskites. Nat. Commun. 8(1), 2230 (2017). https://doi.org/10.1038/s41467-017-02331-4
  18. Y. Zhou, O.S. Game, S. Pang, N.P. Padture, Microstructures of organometal trihalide perovskites for solar cells: their evolution from solutions and characterization. J. Phys. Chem. Lett. 6(23), 4827–4839 (2015). https://doi.org/10.1021/acs.jpclett.5b01843
  19. M.U. Rothmann, J.S. Kim, J. Borchert, K.B. Lohmann, C.M. O’Leary et al., Atomic-scale microstructure of metal halide perovskite. Science 370(6516), 5940 (2020). https://doi.org/10.1126/science.abb5940
  20. S. Palei, G. Murali, C.-H. Kim, I. In, S.-Y. Lee et al., A review on interface engineering of MXenes for perovskite solar cells. Nano-Micro Lett. 15(1), 123 (2023). https://doi.org/10.1007/s40820-023-01083-9
  21. T. Xiao, M. Hao, T. Duan, Y. Li, Y. Zhang et al., Elimination of grain surface concavities for improved perovskite thin-film interfaces. Nat. Energy 9(8), 999–1010 (2024). https://doi.org/10.1038/s41560-024-01567-x
  22. J. Zhuang, J. Wang, F. Yan, Review on chemical stability of lead halide perovskite solar cells. Nano-Micro Lett. 15(1), 84 (2023). https://doi.org/10.1007/s40820-023-01046-0
  23. D.W. DeQuilettes, S.M. Vorpahl, S.D. Stranks, H. Nagaoka, G.E. Eperon et al., Impact of microstructure on local carrier lifetime in perovskite solar cells. Science 348(6235), 683–686 (2015). https://doi.org/10.1126/science.aaa5333
  24. Z. Zhang, W. Chen, X. Jiang, J. Cao, H. Yang et al., Suppression of phase segregation in wide-bandgap perovskites with thiocyanate ions for perovskite/organic tandems with 25.06% efficiency. Nat. Energy 9(5), 592–601 (2024). https://doi.org/10.1038/s41560-024-01491-0
  25. Y. Zhou, L.M. Herz, A.K. Jen, M. Saliba, Advances and challenges in understanding the microscopic structure–property–performance relationship in perovskite solar cells. Nat. Energy 7(9), 794–807 (2022). https://doi.org/10.1038/s41560-022-01096-5
  26. L. Zhang, L. Mei, K. Wang, Y. Lv, S. Zhang et al., Advances in the application of perovskite materials. Nano-Micro Lett. 15(1), 177 (2023). https://doi.org/10.1007/s40820-023-01140-3
  27. K. Almasabi, X. Zheng, B. Turedi, A.Y. Alsalloum, M.N. Lintangpradipto et al., Hole-transporting self-assembled monolayer enables efficient single-crystal perovskite solar cells with enhanced stability. ACS Energy Lett. 8(2), 950–956 (2023). https://doi.org/10.1021/acsenergylett.2c02333
  28. N. Tsvetkov, D. Koo, D. Kim, H. Park, H. Min, Advances in single-crystal perovskite solar cells: from materials to performance. Nano Energy 130, 110069 (2024). https://doi.org/10.1016/j.nanoen.2024.110069
  29. W. Li, Y. Ma, S. Yang, J. Gong, S. Zhang et al., Nanoscopic study of the compositions, structures, and electronic properties of grain boundaries in Cu(InGa)Se2 photovoltaic thin films. Nano Energy 33, 157–167 (2017). https://doi.org/10.1016/j.nanoen.2017.01.041
  30. D.-Y. Son, J.-W. Lee, Y.J. Choi, I.-H. Jang, S. Lee et al., Self-formed grain boundary healing layer for highly efficient CH3NH3PbI3 perovskite solar cells. Nat. Energy 1, 16081 (2016). https://doi.org/10.1038/nenergy.2016.81
  31. T.-X. Qin, E.-M. You, M.-X. Zhang, P. Zheng, X.-F. Huang et al., Quantification of electron accumulation at grain boundaries in perovskite polycrystalline films by correlative infrared-spectroscopic nanoimaging and Kelvin probe force microscopy. Light Sci. Appl. 10(1), 84 (2021). https://doi.org/10.1038/s41377-021-00524-7
  32. V.L. Pool, B. Dou, D.G. Van Campen, T.R. Klein-Stockert, F.S. Barnes et al., Thermal engineering of FAPbI3 perovskite material via radiative thermal annealing and in situ XRD. Nat. Commun. 8, 14075 (2017). https://doi.org/10.1038/ncomms14075
  33. X. Wang, Y. Sun, Y. Wang, X.-C. Ai, J.-P. Zhang, Lewis base plays a double-edged-sword role in trap state engineering of perovskite polycrystals. J. Phys. Chem. Lett. 13(6), 1571–1577 (2022). https://doi.org/10.1021/acs.jpclett.2c00167
  34. Y. Wang, Y. Cheng, C. Yin, J. Zhang, J. You et al., Manipulating crystal growth and secondary phase PbI2 to enable efficient and stable perovskite solar cells with natural additives. Nano-Micro Lett. 16(1), 183 (2024). https://doi.org/10.1007/s40820-024-01400-w
  35. Y. Kutes, Y. Zhou, J.L. Bosse, J. Steffes, N.P. Padture et al., Mapping the photoresponse of CH3NH3PbI3 hybrid perovskite thin films at the nanoscale. Nano Lett. 16(6), 3434–3441 (2016). https://doi.org/10.1021/acs.nanolett.5b04157
  36. M.I. Saidaminov, K. Williams, M. Wei, A. Johnston, R. Quintero-Bermudez et al., Multi-cation perovskites prevent carrier reflection from grain surfaces. Nat. Mater. 19(4), 412–418 (2020). https://doi.org/10.1038/s41563-019-0602-2
  37. W. Tian, R. Cui, J. Leng, J. Liu, Y. Li et al., Limiting perovskite solar cell performance by heterogeneous carrier extraction. Angew. Chem. Int. Ed. 55(42), 13067–13071 (2016). https://doi.org/10.1002/anie.201606574
  38. P. Jia, L. Qin, D. Zhao, Y. Tang, B. Song et al., The trapped charges at grain boundaries in perovskite solar cells. Adv. Funct. Mater. 31(49), 2107125 (2021). https://doi.org/10.1002/adfm.202107125
  39. L. Zhang, B. Lv, H. Yang, R. Xu, X. Wang et al., Quantum-confined stark effect in the ensemble of phase-pure CdSe/CdS quantum dots. Nanoscale 11(26), 12619–12625 (2019). https://doi.org/10.1039/C9NR03061A
  40. S. Wang, J. Leng, Y. Yin, J. Liu, K. Wu et al., Ultrafast dopant-induced exciton auger-like recombination in Mn-doped perovskite nanocrystals. ACS Energy Lett. 5(1), 328–334 (2020). https://doi.org/10.1021/acsenergylett.9b02678
  41. K. Wu, G. Liang, Q. Shang, Y. Ren, D. Kong et al., Ultrafast interfacial electron and hole transfer from CsPbBr3 perovskite quantum dots. J. Am. Chem. Soc. 137(40), 12792–12795 (2015). https://doi.org/10.1021/jacs.5b08520
  42. C. Chakraborty, K.M. Goodfellow, S. Dhara, A. Yoshimura, V. Meunier et al., Quantum-confined stark effect of individual defects in a van der waals heterostructure. Nano Lett. 17(4), 2253–2258 (2017). https://doi.org/10.1021/acs.nanolett.6b04889
  43. X. Chen, R.T. Pekarek, J. Gu, A. Zakutayev, K.E. Hurst et al., Transient evolution of the built-in field at junctions of GaAs. ACS Appl. Mater. Interfaces 12(36), 40339–40346 (2020). https://doi.org/10.1021/acsami.0c11474
  44. X. Yan, B. Wu, C. Chen, F. Sun, H. Bao et al., Elucidating the impact of electron accumulation in quantum-dot light-emitting diodes. Nano Lett. 24(42), 13374–13380 (2024). https://doi.org/10.1021/acs.nanolett.4c03967
  45. J. Leng, J. Liu, J. Zhang, S. Jin, Decoupling interfacial charge transfer from bulk diffusion unravels its intrinsic role for efficient charge extraction in perovskite solar cells. J. Phys. Chem. Lett. 7(24), 5056–5061 (2016). https://doi.org/10.1021/acs.jpclett.6b02309
Read More
Author biographies are not available.
Download this PDF file
PDF SUPPLEMENTARY FILE
Statistic
Read Counter : 1890 Download : 1414

Most read articles by the same author(s)