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Nature volume 652, pages 1204–1210 (2026)
Non-geminate recombination in organic photovoltaics (OPVs) forms low-energy spin-triplet excitons (T1) that are known to result in irreversible, non-radiative relaxations1,2,3,4,5. Here we experimentally show in an OPV system incorporating a non-fullerene acceptor with a narrowed singlet–triplet gap that T1 excitons can be redissociated through the interfacial charge-transfer state to form free carriers. We corroborate this by identifying the increased population of free carriers following triplet sensitization of the acceptor in an OPV blend, and illustrate the way in which this mechanism alters the evolution of T1 and free carrier populations. We reveal how the distribution of orbitals in the molecule and exciton delocalization in aggregates affect the singlet–triplet energetics of the acceptor in the condensed phase, rendering the traffic between T1 and the spin-triplet charge-transfer state controllable. By introducing this acceptor as a ternary component into other host OPV systems, we manage to recover the triplet-mediated losses and improve OPV efficiencies by maximizing the number of extractable photocarriers. This study deepens our understanding of the fundamentals of OPVs, and shows how to develop future organic optoelectronics by demonstratating the recovery of low-energy T1 excitons into usable charges for electricity or light generation instead of heat.
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The data supporting the findings of this study are available from the corresponding authors on reasonable request.
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A.K.Y.J. is grateful for sponsorship by the Lee Shau-Kee Chair Professorship in Materials Science, and support from APRC grants (grant nos. 9380086, 9610419, 9610440, 9610492, 9610508) of the City University of Hong Kong; MHKJFS, TCFS and MRP (grant nos. MHP/054/23, GHP/121/22SZ, MRP/040/21X, respectively) grants from the Innovation and Technology Commission of Hong Kong; and GRF (grant nos. 11307621, 11316422, 11308625) and CRS (grant nos. CRS_CityU104/23 and CRS_HKUST203/23) grants from the Research Grants Council of Hong Kong. This work was partially financially supported by City University of Hong Kong (grant no. 9610739) via the ‘Fostering Innovation for Resilience and Sustainable Transformation’ project, which is officially endorsed by the United Nations Educational, Scientific and Cultural Organization, under the International Decade of Sciences for Sustainable Development (2024–2033). D.L. is grateful for support from the Collaborative Research Equipment Grant (grant no. C1015-21EF) via the Research Grants Council of Hong Kong. C.S.L. is grateful for support from the General Research Fund from the Research Grants Council of the Hong Kong Special Administrative Region (grant no. CityU 11303923). S.W.T. is grateful for the support from the National Natural Science Foundation of China (grant no. 62474151). X.K.C. gratefully acknowledges financial support from the National Key Research and Development Program of China (grant no. 2022YFB4200600), the National Natural Science Foundation of China (grant nos. W2511063 and 52473190), the Natural Science Foundation of Jiangsu Province (grant no. BK20240042), the Science and Technology Project of Suzhou (grant no. ZXL2024394), the Suzhou Key Laboratory of Functional Nano and Soft Materials, Collaborative Innovation Center of Suzhou Nano Science and Technology, and the 111 Project. We also gratefully acknowledge Y. Li, Y. Wang, Z. Yue and T. Xia from the City University of Hong Kong for their assistance with ultraviolet photoelectron spectroscopy, photoluminescence and electroluminescence measurements, and cell characterizations; M. Yan from the Nanjing University for their assistance with spectroscopic measurements; R. Walia from the Soochow University for their assistance with theoretical calculations; and S.-H. Jang from the University of Washington for their assistance with writing the manuscript.
These authors contributed equally: Qian Li, Lingchen Kong, Le Mei
Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong SAR
Qian Li (李谦), Lingchen Kong (孔令晨), Shanchao Ouyang (欧阳汕超), Huanhuan Gao (高欢欢), Wei Gao (高威), Nan Zhang (张楠), Hin-Lap Yip (葉軒立), Dangyuan Lei (雷党愿), Sai-Wing Tsang (曾世榮), Francis R. Lin (林均叡) & Alex K.-Y. Jen (任廣禹)
Hong Kong Institute for Clean Energy, City University of Hong Kong, Kowloon, Hong Kong SAR
Qian Li (李谦), Lingchen Kong (孔令晨), Shanchao Ouyang (欧阳汕超), Nan Zhang (张楠), Hin-Lap Yip (葉軒立), Dangyuan Lei (雷党愿), Sai-Wing Tsang (曾世榮), Francis R. Lin (林均叡) & Alex K.-Y. Jen (任廣禹)
Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong SAR
Le Mei (梅乐), Baobing Fan (樊宝兵), Feng Qi (齐峰), Zhiqiang Guan (官志强), Chun-Sing Lee (李振聲), Francis R. Lin (林均叡) & Alex K.-Y. Jen (任廣禹)
Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou, China
Le Mei (梅乐) & Xian-Kai Chen (陈先凯)
State Key Laboratory of Bioinspired interfacial Materials Science, Soochow University, Suzhou, China
Le Mei (梅乐) & Xian-Kai Chen (陈先凯)
School of Physics and Technology, University of Jinan, Jinan, China
Yiwen Ji (季艺闻)
State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, China
Baobing Fan (樊宝兵)
School of Materials Science and Engineering, Shandong University of Technology, Zibo, China
Huanhuan Gao (高欢欢)
Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Institute of Luminescent Materials and Information Displays, College of Materials Science and Engineering, Huaqiao University, Xiamen, China
Wei Gao (高威)
College of Materials Science and Engineering, Qingdao University, Qingdao, China
Feng Qi (齐峰)
Center of Super-Diamond and Advanced Films, City University of Hong Kong, Kowloon, Hong Kong SAR
Zhiqiang Guan (官志强), Hin-Lap Yip (葉軒立), Chun-Sing Lee (李振聲), Sai-Wing Tsang (曾世榮) & Alex K.-Y. Jen (任廣禹)
National Laboratory of Solid State Microstructures, School of Physics, and Collaborative Innovation Center for Advanced Microstructures, Nanjing University, Nanjing, China
Chunfeng Zhang (张春峰)
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Q.L., X.K.C., F.R.L. and A.K.Y.J. conceived the idea. Q.L. and F.R.L. designed the experiments and wrote the manuscript. Q.L. performed the TAS, TR-2PPE and other spectroscopic measurements. L.K. fabricated the OPV cells and conducted relevant characterizations. L.M., Y.J. and X.K.C. performed the theoretical calculations and simulations. S.O. and S.W.T. conducted the electroabsorption measurements and assisted with the photoluminescence and electroluminescence measurements. B.F., H.G., W.G. and F.Q. provided the materials. D.L. and C.Z. assisted with the spectroscopic measurements. Z.G. and C.S.L. contributed to the establishment of the TR-2PPE and ultraviolet photoelectron spectroscopy systems, and the sample measurements. N.Z. and H.L.Y. contributed to optimizing the TR-2PPE and cell characterizations.
Correspondence to Xian-Kai Chen (陈先凯), Francis R. Lin (林均叡) or Alex K.-Y. Jen (任廣禹).
The authors declare no competing interests.
Nature thanks the anonymous reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available.
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a, Normalized TAS dynamics of T1 excitons (1560 nm) in D18:Sensi-FTh-4F and Sensi-FTh-4F films at different pump power densities. b, Representative schematics of TTA and TCA processes in OPVs. In TTA, e.g., two T1 excitons interact, causing one to return to the GS and the other to be excited to a high energy state (Sn). In TCA, e.g., a T1 exciton interacts with a charge (CS), causing the T1 exciton to return to the GS, transferring thermal energy to the charge. TTA and TCA are both bimolecular processes, which are sensitive to the pump density. In contrast, the transfer from T1 to interfacial 3CT is a unimolecular process, which is not affected by the pump density. In the case of D18:Sensi-FTh-4F (Supplementary Fig. 6) and D18:FTh-4F (Supplementary Fig. 4) films at relatively low excitation densities, the first-order T1 → 3CT transfer process dominates the T1 decay dynamics as the T1 population is rather low. However, as the T1 population increases at higher excitation densities, the bimolecular TTA and TCA pathways become more dominant so that the power dependence becomes more significant. In Sensi-FTh-4F, due to the absence of T1 → 3CT transfer process, the bimolecular processes are consistently dominant, as evidenced by the significant power dependence across different excitation densities (Supplementary Fig. 7).
The Jablonski diagram illustrates the states and the processes involved. (1) CS undergoes non-geminate recombination (NGR) to form 1CT/3CT in 1:3 ratio; (2) 1CT re-separates into CS or relaxes to GS; (3) 3CT re-separates into CS or undergoes BCT to T1 in NFA; (4) T1 in NFA transfers to reform 3CT or relaxes to GS directly or through TCA. The rate equations used for simulation are also provided.
a,b, fs-TAS colour plots and spectra of Sensi-BrQx-4BO (6:1), c,d neat BrQx-4BO, e,f, Sensi-FTh-4F (6:1) and g,h, neat FTh-4F films.
a,b, TR-2PPE spectra of Sensi-BrQx-4BO (6:1) and Sensi-FTh-4F (6:1) films. c,d, TR-2PPE spectra of neat BrQx-4BO and neat FTh-4F films.
The molecular orbitals on the thienyl side-chains are circled by the blue dashed lines. The weights of the HOMO → LUMO transition in the S1 and T1 excitations and the spatial HOMO-LUMO overlap (θH-L) are provided.
a, Illustration of core and terminal groups in NFAs. b, Statistics of the dimers packed in different configurations (i.e., terminal-to-terminal, core-to-terminal, and core-to-core) obtained from MD simulations. c, Average spatial distances of dimers with different packing configurations. d, Average CT percentages of S1 states calculated from dimers packed in different configurations.
Second harmonic EA spectra (transmission mode) and 1st/2nd derivatives of absorption spectra of a, BrQx-4BO and b, FTh-4F films. The excited-state polarizability change (Δp) is related to spatial distribution of electron wavefunction. The dipole moment change (Δμ) is related to electron-hole separation in neat NFA films. The EA spectrum of BrQx-4BO film resembles the 1st derivative of its absorption spectrum, suggesting the dominant proportion of Δp relative to Δμ. In contrast, the EA spectrum of FTh-4F film shows a combined features of the 1st and 2nd derivatives of its absorption spectrum, implying an improved contribution from Δμ.
a, J − V curves and b, EQE spectra of D18:Y6-4BO (1:1.3) and ternary (D18:Y6-4BO:FTh-4F = 1:1.2:0.15) OPV cells.
Supplementary Methods, Notes, Figures, Tables and References.
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Li, Q., Kong, L., Mei, L. et al. Recycling of spin-triplet excitons in organic photovoltaics. Nature 652, 1204–1210 (2026). https://doi.org/10.1038/s41586-026-10419-5
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