Due to the large chemical composition and bandgap tunability of both perovskite and organic semiconductors, perovskite/organic tandem solar cells are attractive for next-generation thin-film photovoltaics. However, their efficiency is limited by the open-circuit voltage loss of wide-bandgap perovskite subcells and the non-ideal interconnecting layers. Here we report that the passivation of nickel oxide hole-transporting layers with benzylphosphonic acid leads to the suppression of interfacial recombination, boosting the voltage up to 1.26 V in a 1.79-eV-bandgap perovskite subcell. Then, we develop an optimized interconnecting layer structure based on a 4-nm-thick sputtered indium zinc oxide layer inserted between organic bathocuproine and molybdenum oxide with enhanced electrical properties and transmittance in the near-infrared region. Through these improvements, we achieve a maximum efficiency of 23.60% (22.95% certified) in the perovskite/organic tandem solar cell. In addition, the tandem device retained 90% initial efficiency after 500 h maximum power point tracking under continuous one sun illumination.
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Anaya, M., Lozano, G., Calvo, M. E. & Míguez, H. ABX3 perovskites for tandem solar cells. Joule 1, 769–793 (2017).
Leijtens, T., Bush, K. A., Prasanna, R. & McGehee, M. D. Opportunities and challenges for tandem solar cells using metal halide perovskite semiconductors. Nat. Energy 3, 828–838 (2018).
Bush, K. A. et al. 23.6%-efficient monolithic perovskite/silicon tandem solar cells with improved stability. Nat. Energy 2, 17009 (2017).
Hou, Y. et al. Efficient tandem solar cells with solution-processed perovskite on textured crystalline silicon. Science 367, 1135–1140 (2020).
Eperon, G. E. et al. Perovskite-perovskite tandem photovoltaics with optimized band gaps. Science 354, 861–865 (2016).
McMeekin, D. P. et al. A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells. Science 351, 151–155 (2016).
Best Research-Cell Efficiency Chart. NREL https://www.nrel.gov/pv/assets/pdfs/best-research-cell-efficiencies-rev210726.pdf (Assessed April 2021).
Al-Ashouri, A. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).
Li, H. & Zhang, W. Perovskite tandem solar cells: from fundamentals to commercial deployment. Chem. Rev. 120, 9835–9950 (2020).
Yan, C. et al. Non-fullerene acceptors for organic solar cells. Nat. Rev. Mater. 3, 18003 (2018).
Yuan, J. et al. Single-junction organic solar cell with over 15% efficiency using fused-ring acceptor with electron-deficient core. Joule 3, 1140–1151 (2019).
Zhang, M. et al. Single-layered organic photovoltaics with double cascading charge transport pathways: 18% efficiencies. Nat. Commun. 12, 309 (2021).
Yao, H., Wang, J., Xu, Y., Zhang, S. & Hou, J. Recent progress in chlorinated organic photovoltaic materials. Acc. Chem. Res. 53, 822–832 (2020).
Xie, Y. M. et al. Monolithic perovskite/organic tandem solar cells: developments, prospects, and challenges. Nano Sel. 2, 1266–1276 (2021).
Meng, L. et al. Organic and solution-processed tandem solar cells with 17.3% efficiency. Science 361, 1094–1098 (2018).
Chen, X. et al. Efficient and reproducible monolithic perovskite/organic tandem solar cells with low-loss interconnecting layers. Joule 4, 1594–1606 (2020).
Lin, R. et al. Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(ii) oxidation in precursor ink. Nat. Energy 4, 864–873 (2019).
Al-Ashouri, A. et al. Conformal monolayer contacts with lossless interfaces for perovskite single junction and monolithic tandem solar cells. Energy Environ. Sci. 12, 3356–3369 (2019).
Peña-Camargo, F. et al. Halide segregation versus interfacial recombination in bromide-rich wide-gap perovskite solar cells. ACS Energy Lett. 5, 2728–2736 (2020).
Mahesh, S. et al. Revealing the origin of voltage loss in mixed-halide perovskite solar cells. Energy Environ. Sci. 13, 258–267 (2020).
Ko, Y., Park, H., Lee, C., Kang, Y. & Jun, Y. Recent progress in interconnection layer for hybrid photovoltaic tandems. Adv. Mater. 32, e2002196 (2020).
De Bastiani, M. et al. Recombination junctions for efficient monolithic perovskite-based tandem solar cells: physical principles, properties, processing and prospects. Mater. Horiz. 7, 2791–2809 (2020).
Zhao, D. et al. Low-bandgap mixed tin–lead iodide perovskite absorbers with long carrier lifetimes for all-perovskite tandem solar cells. Nat. Energy 2, 17018 (2017).
Li, C. et al. Low-bandgap mixed tin–lead iodide perovskites with reduced methylammonium for simultaneous enhancement of solar cell efficiency and stability. Nat. Energy 5, 768–776 (2020).
Yu, Z. et al. Simplified interconnection structure based on C60/SnO2–x for all-perovskite tandem solar cells. Nat. Energy 5, 657–665 (2020).
Yang, Z. et al. Enhancing electron diffusion length in narrow-bandgap perovskites for efficient monolithic perovskite tandem solar cells. Nat. Commun. 10, 4498 (2019).
Palmstrom, A. F. et al. Enabling flexible all-perovskite tandem solar cells. Joule 3, 2193–2204 (2019).
Zhao, D. et al. Efficient two-terminal all-perovskite tandem solar cells enabled by high-quality low-bandgap absorber layers. Nat. Energy 3, 1093–1100 (2018).
Xiao, K. et al. All-perovskite tandem solar cells with 24.2% certified efficiency and area over 1 cm2 using surface-anchoring zwitterionic antioxidant. Nat. Energy 5, 870–880 (2020).
Li, Z. et al. Hybrid perovskite-organic flexible tandem solar cell enabling highly efficient electrocatalysis overall water splitting. Adv. Energy Mater. 10, 2000361 (2020).
Lang, K. et al. High performance tandem solar cells with inorganic perovskite and organic conjugated molecules to realize complementary absorption. J. Phys. Chem. Lett. 11, 9596–9604 (2020).
Chen, C.-C. et al. Perovskite/polymer monolithic hybrid tandem solar cells utilizing a low-temperature, full solution process. Mater. Horiz. 2, 203–211 (2015).
Xie, S. et al. Efficient monolithic perovskite/organic tandem solar cells and their efficiency potential. Nano Energy 78, 105238–105245 (2020).
Zeng, Q. et al. A two-terminal all-inorganic perovskite/organic tandem solar cell. Sci. Bull. 64, 885–887 (2019).
Kim, S. & Lee, J.-L. Design of dielectric/metal/dielectric transparent electrodes for flexible electronics. J. Photon. Energy 2, 021215–021211 (2012).
Axelevitch, A., Gorenstein, B. & Golan, G. Investigation of optical transmission in thin metal films. Phys. Procedia 32, 1–13 (2012).
Di Girolamo, D. et al. Progress, highlights and perspectives on NiO in perovskite photovoltaics. Chem. Sci. 11, 7746–7759 (2020).
Ali, F., Roldán-Carmona, C., Sohail, M. & Nazeeruddin, M. K. Applications of self-assembled monolayers for perovskite solar cells interface engineering to address efficiency and stability. Adv. Energy Mater. 10, 2002989 (2020).
Bi, H. et al. Interfacial defect passivation and stress release by multifunctional KPF6 modification for planar perovskite solar cells with enhanced efficiency and stability. Chem. Eng. J. 418, 129375 (2021).
Zhang, J. et al. Obstructing interfacial reaction between NiOx and perovskite to enable efficient and stable inverted perovskite solar cells. Chem. Eng. J. 426, 131357 (2021).
Du, Y. et al. Polymeric surface modification of NiOx-based inverted planar perovskite solar cells with enhanced performance. ACS Sustain. Chem. Eng. 6, 16806–16812 (2018).
Tress, W. Perovskite solar cells on the way to their radiative efficiency limit – insights into a success story of high open-circuit voltage and low recombination. Adv. Energy Mater. 7, 1602358 (2017).
Wang, Q. et al. Effects of self-assembled monolayer modification of nickel oxide nanoparticles layer on the performance and application of inverted perovskite solar cells. ChemSusChem 10, 3794–3803 (2017).
Chen, W. et al. Molecule-doped nickel oxide: verified charge transfer and planar inverted mixed cation perovskite solar cell. Adv. Mater. 30, 1800515 (2018).
Liu, L., Xiao, Z., Zuo, C. & Ding, L. Inorganic perovskite/organic tandem solar cells with efficiency over 20%. J. Semicond. 42, 020501 (2021).
Zuo, L., Shi, X., Fu, W. & Jen, A. K. Highly efficient semitransparent solar cells with selective absorption and tandem architecture. Adv. Mater. 31, e1901683 (2019).
Bush, K. A. et al. Thermal and environmental stability of semi-transparent perovskite solar cells for tandems enabled by a solution-processed nanoparticle buffer layer and sputtered ITO electrode. Adv. Mater. 28, 3937–3943 (2016).
Fu, F. et al. High-efficiency inverted semi-transparent planar perovskite solar cells in substrate configuration. Nat. Energy 2, 16190 (2016).
Schloemer, T. H. et al. The molybdenum oxide interface limits the high-temperature operational stability of unencapsulated perovskite solar cells. ACS Energy Lett. 5, 2349–2360 (2020).
Heumueller, T. et al. Disorder-induced open-circuit voltage losses in organic solar cells during photoinduced burn-in. Adv. Energy Mater. 5, 1500111 (2015).
Chen, W., Xu, L., Feng, X., Jie, J. & He, Z. Metal acetylacetonate series in interface engineering for full low-temperature-processed, high-performance, and stable planar perovskite solar cells with conversion efficiency over 16% on 1 cm2 scale. Adv. Mater. 29, 1603923 (2017).
Chen, C. et al. Arylammonium-assisted reduction of the open-circuit voltage deficit in wide-bandgap perovskite solar cells: the role of suppressed ion migration. ACS Energy Lett. 5, 2560–2568 (2020).
Ying, Z. et al. Sputtered indium-zinc oxide for buffer layer free semitransparent perovskite photovoltaic devices in perovskite/silicon 4T-tandem solar cells. Adv. Mater. Interfaces 8, 2001604 (2020).
Ma, R. et al. Adding a third component with reduced miscibility and higher LUMO level enables efficient ternary organic solar cells. ACS Energy Lett. 5, 2711–2720 (2020).
Chen, W. et al. Interfacial stabilization for inverted perovskite solar cells with long-term stability. Sci. Bull. 66, 991–1002 (2021).
Tan, H. Q., Zhao, X., Birgersson, E., Lin, F. & Xue, H. Optoelectronic modeling and sensitivity analysis of a four-terminal all-perovskite tandem solar cell – identifying pathways to improve efficiency. Sol. Energy 216, 589–600 (2021).
Xue, H., Fu, K., Wong, L. H., Birgersson, E. & Stangl, R. Modelling and loss analysis of meso-structured perovskite solar cells. J. Appl. Phys. 122, 083105 (2017).
Zhang, T. et al. Analysis of a device model for organic pseudo-bilayer solar cells. J. Appl. Phys. 112, 084511 (2012).
Hurkx, G. A. M., Klaassen, D. B. M. & Knuvers, M. P. G. A new recombination model for device simulation including tunneling. IEEE Trans. Electron Dev. 39, 331–338 (1992).
This work is supported by the National Natural Science Foundation of China (nos 61775091 and U2001216); the Science, Technology and Innovation Commission of Shenzhen Municipality (no. JCYJ20180504165851864); the Shenzhen Key Laboratory Project (no. ZDSYS201602261933302); and the Natural Science Foundation of Shenzhen Innovation Committee (nos JCYJ20150529152146471 and JCYJ20170818141216288). A.B.D. acknowledges support from the Research Grants Council Collaborative Research Fund grants C5037-18G and C7018-20G, Seed Funding for Strategic Interdisciplinary Research Scheme of the University of Hong Kong and Shenzhen Science and Technology Innovation Commission Projects no. JCYJ20170818141216288. Y. Hou acknowledges the support from the National University of Singapore Presidential Young Professorship (R-279-000-617-133 and R-279-001-617-133). Seven of the authors of this paper are affiliated with the Solar Energy Research Institute of Singapore (SERIS), a research institute at the National University of Singapore. SERIS is supported by the National University of Singapore, the National Research Foundation Singapore, the Energy Market Authority of Singapore and the Singapore Economic Development Board. We thank the Materials Characterization and Preparation Center and the Pico Center of SUSTech for some characterizations in this work.
The authors declare no competing interests.
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Chen, W., Zhu, Y., Xiu, J. et al. Monolithic perovskite/organic tandem solar cells with 23.6% efficiency enabled by reduced voltage losses and optimized interconnecting layer. Nat Energy 7, 229–237 (2022). https://doi.org/10.1038/s41560-021-00966-8
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