α-Helix-Driven Regulation of Aqueous Circularly Polarized Luminescence in Homopolypeptide Self-Assembly

Jinhui Jiang , Ziyue Ye , Siwei Zhang , Fulong Ma , Lin Lu , Zijie Qiu , Jianwei Sun , Yu Xiong , Zheng Zhao , Jacky W. Y. Lam , Ben Zhong Tang

Aggregate ›› 2025, Vol. 6 ›› Issue (10) : e70123

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Aggregate ›› 2025, Vol. 6 ›› Issue (10) : e70123 DOI: 10.1002/agt2.70123
RESEARCH ARTICLE

α-Helix-Driven Regulation of Aqueous Circularly Polarized Luminescence in Homopolypeptide Self-Assembly

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Abstract

Biopolymer-driven supramolecular chirality in aqueous media has gained significant advancements in hierarchical chiral nanostructures. However, researches on the aqueous circularly polarized luminescence (CPL) induced by supramolecular self-assembly and its mechanism have been rarely reported. Herein, we explore the hierarchical chirality transfer in self-assembled fluorescent homopolypeptide systems showing aqueous CPL, and unveil an α-helix-dominated CPL regulation mechanism. A relationship is established between molecular structure (degree of polymerization, DP), supramolecular assembly (self-assembly temperature, TSA), and resulting CPL properties. The stabilization for the homopolypeptide α-helix by increasing DP and decreasing TSA enables efficient chirality transfer from the polypeptide backbone to its terminal chromophore, thereby improving CPL properties. Our work elucidates the critical role of α-helix control in aqueous CPL systems, providing insights for designing biocompatible and tunable CPL-active nanomaterials.

Keywords

aqueous circularly polarized luminescence / chiral homopolypeptide / self-assembly / α-helix

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Jinhui Jiang, Ziyue Ye, Siwei Zhang, Fulong Ma, Lin Lu, Zijie Qiu, Jianwei Sun, Yu Xiong, Zheng Zhao, Jacky W. Y. Lam, Ben Zhong Tang. α-Helix-Driven Regulation of Aqueous Circularly Polarized Luminescence in Homopolypeptide Self-Assembly. Aggregate, 2025, 6(10): e70123 DOI:10.1002/agt2.70123

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References

[1]

a) Y. Wang, J. Xu, Y. Wang, and H. Chen, “Emerging Chirality in Nanoscience,” Chemical Society Reviews 42 (2013): 2930-2962. b) M. Liu, L. Zhang, and T. Wang, “Supramolecular Chirality in Self-Assembled Systems,” Chemical Reviews 115 (2015): 7304-7397.

[2]

C. Bai and M. Liu, “From Chemistry to Nanoscience: Not Just a Matter of Size,” Angewandte Chemie International Edition 52 (2013): 2678-2683.

[3]

a) J. Kim, J. Lee, W. Y. Kim, et al., “Induction and Control of Supramolecular Chirality by Light in Self-Assembled Helical Nanostructures,” Nature Communications 6 (2015): 6959. b) J. S. Kang, S. Kang, J.-M. Suh, et al., “Circularly Polarized Light Can Override and Amplify Asymmetry in Supramolecular Helices,” Journal of the American Chemical Society 144 (2022): 2657-2666.

[4]

S. Huang, H. Yu, and Q. Li, “Supramolecular Chirality Transfer Toward Chiral Aggregation: Asymmetric Hierarchical Self-Assembly,” Advanced Science 8 (2021): 2002132.

[5]

a) R. Xiong, J. Luan, S. Kang, C. Ye, S. Singamaneni, and V. V. Tsukruk, “Biopolymeric Photonic Structures: Design, Fabrication, and Emerging Applications,” Chemical Society Reviews 49 (2020): 983-1031. b) G. Zhang, X. Cheng, Y. Wang, and W. Zhang, “Supramolecular Chiral Polymeric Aggregates: Construction and Applications,” Aggregate 4 (2023): e262.

[6]

Z.-L. Gong, X. Zhu, Z. Zhou, et al., “Frontiers in Circularly Polarized Luminescence: Molecular Design, Self-Assembly, Nanomaterials, and Applications,” Science China Chemistry 64 (2021): 2060-2104.

[7]

a) H. Zhong, X. Gao, B. Zhao, and J. Deng, ““Matching Rule” for Generation, Modulation and Amplification of Circularly Polarized Luminescence,” Accounts of Chemical Research 57 (2024): 1188-1201. b) Y. Wu, M. Li, Z.-g. Zheng, Z.-Q. Yu, and W.-H. Zhu, “Liquid Crystal Assembly for Ultra-Dissymmetric Circularly Polarized Luminescence and Beyond,” Journal of the American Chemical Society 145 (2023): 12951-12966. c) B.-H. Liu, Y. Zong, N. Liu, and Z.-Q. Wu, “Advances in Self-Assembly-Based Circularly Polarized Luminescent Materials,” Science China Chemistry 67 (2024): 3247-3257. d) H. Yan, Y. He, D. Wang, T. Han, and B. Z. Tang, “Aggregation-Induced Emission Polymer Systems With Circularly Polarized Luminescence,” Aggregate 4 (2023): e331. e) Y. Zhong, Z. Wu, Y. Zhang, B. Dong, and X. Bai, “Circularly Polarized Luminescence of Lanthanide Complexes: From Isolated Individuals, Discrete Oligomers, to Hierarchical Assemblies,” InfoMat 5 (2023): e12392. f) S. Jiang and N. A. Kotov, “Circular Polarized Light Emission in Chiral Inorganic Nanomaterials,” Advanced Materials 35 (2023): 2108431.

[8]

a) J. Jiang, F. Ma, R. Dong, et al., “Aqueous Circularly Polarized Luminescence Induced by Homopolypeptide Self-Assembly,” Journal of the American Chemical Society 145 (2023): 27282-27294. b) Q. Jiang, X. Xu, P.-A. Yin, et al., “Circularly Polarized Luminescence of Achiral Cyanine Molecules Assembled on DNA Templates,” Journal of the American Chemical Society 141 (2019): 9490-9494. c) Y. Shi, G. Yin, Z. Yan, et al., “Helical Sulfono-γ-AApeptides With Aggregation-Induced Emission and Circularly Polarized Luminescence,” Journal of the American Chemical Society 141 (2019): 12697-12706. d) Y. An, Z. Shen, F. Zhang, et al., “Inversion of Circularly Polarized Luminescence in the Left-Handed Chitosan-Templated Co-Assemblies,” Advanced Science 12 (2025): 2415260.

[9]

a) M. S. Ganewatta, Z. Wang, and C. Tang, “Chemical Syntheses of Bioinspired and Biomimetic Polymers Toward Biobased Materials,” Nature Reviews Chemistry 5 (2021): 753-772. b) A. Rasines Mazo, S. Allison-Logan, F. Karimi, et al., “Ring Opening Polymerization of α-Amino Acids: Advances in Synthesis, Architecture and Applications of Polypeptides and Their Hybrids,” Chemical Society Reviews 49 (2020): 4737-4834. c) Y. Wu, K. Chen, J. Wang, M. Chen, W. Dai, and R. Liu, “Recent Advances and Future Developments in the Preparation of Polypeptides via N -Carboxyanhydride (NCA) Ring-Opening Polymerization,” Journal of the American Chemical Society 146 (2024): 24189-24208.

[10]

X. Liu, J. Huang, J. Wang, et al., “Accelerated and Controlled Polymerization of N-Carboxyanhydrides Assisted by Acids,” CCS Chemistry (2024),

[11]

a) T. Miyazawa and E. R. Blout, “The Infrared Spectra of Polypeptides in Various Conformations: Amide I and II Bands 1,” Journal of the American Chemical Society 83 (1961): 712-719. b) J. Jiang, H. Sun, P. Wei, et al., “π–π Interlocking Effect for Designing Biodegradable Nanorods With Controlled Lateral Surface Curvature,” Chemistry of Materials 34 (2022): 4937-4945.

[12]

a) B. F. Levine and C. G. Bethea, “Second Order Hyperpolarizability of a Polypeptide α-Helix: Poly-γ-Benzyl-L Glutamate,” Journal of Chemical Physics 65 (1976): 1989-1993. b) A. Wada and H. Kihara, “On the Rigidity of the α-Helix as Measured by Dielectric Studies,” Polymer Journal 3 (1972): 482-487. c) B. Lin, A. Hung, W. Singleton, et al., “Inside Back Cover: The Effect of Tailing Lipidation on the Bioactivity of Antimicrobial Peptides and Their Aggregation Tendency,” Aggregate 4 (2023): e329.

[13]

C. M. Barratt, T. K. Haraniya, S. J. Iwamasa, et al., “Synthesis and Conformational Studies of Hyperbranched-Core Star Polymers With Poly(γ-Benzyl-l-Glutamate) Arms,” European Polymer Journal 186 (2023): 111859.

[14]

C. Wang, W. Chi, Q. Qiao, D. Tan, Z. Xu, and X. Liu, “Twisted Intramolecular Charge Transfer (TICT) and Twists Beyond TICT: From Mechanisms to Rational Designs of Bright and Sensitive Fluorophores,” Chemical Society Reviews 50 (2021): 12656-12678.

[15]

C. Cai, J. Lin, X. Zhu, S. Gong, X.-S. Wang, and L. Wang, “Superhelices With Designed Helical Structures and Temperature-Stimulated Chirality Transitions,” Macromolecules 49 (2016): 15-22.

[16]

Y.-b. Lim, K.-S. Moon, and M. Lee, “Stabilization of an α Helix by β-Sheet-Mediated Self-Assembly of a Macrocyclic Peptide,” Angewandte Chemie International Edition 48 (2009): 1601-1605.

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2025 The Author(s). Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.

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