Mo, XiaomeiLi, HuachengTang, PanHao, YayaDong, BingqianMarazuela Lamata, María DoloresGómez Gómez, María MilagrosZhu, XianfengLi, QianLora Maroto, BeatrizJiang, ShuoxingFan, ChunhaiLan, Xiang2024-01-102024-01-102023DNA-Modulated and Mechanoresponsive Excitonic Couplings Reveal Chiroptical Correlation of Conformation, Tension, and Dynamics of DNA Self-Assembly Xiaomei Mo, Huacheng Li, Pan Tang, Yaya Hao, Bingqian Dong, M. Dolores Marazuela, M. Milagros Gomez-Gomez, Xianfeng Zhu, Qian Li, Beatriz L. Maroto, Shuoxing Jiang, Chunhai Fan, and Xiang Lan Nano Letters 2023 23 (24), 11734-11741 DOI: 10.1021/acs.nanolett.3c036521530-698410.1021/acs.nanolett.3c03652https://hdl.handle.net/20.500.14352/92251Study of the conformational and mechanical behaviors of biomolecular assemblies is vital to the rational design and realization of artificial molecular architectures with biologically relevant functionality. Here, we revealed DNA-modulated and mechanoresponsive excitonic couplings between organic chromophores and verified strong correlations between the excitonic chiroptical responses and the conformational and mechanical states of DNA self-assemblies irrespective of fluorescence background interference. Besides, the excitonic chiroptical effect allowed sensitive monitoring of DNA self-assembled nanostructures due to small molecule bindings or DNA strand displacement reactions. Moreover, we developed a new chiroptical reporter, a DNAtemplated dimer of an achiral cyanine5 and an intrinsically chiral BODIPY, that exhibited unique multiple-split spectral line shape of exciton-coupled circular dichroism, largely separated response wavelengths, and enhanced anisotropy dissymmetry factor (g-factor). These results shed light on a promising chiroptical spectroscopic tool for studying biomolecular recognition and binding, conformation dynamics, and soft mechanics in general.engjournal article1530-6992https://doi.org/10.1021/acs.nanolett.3c03652open access543Química2301 Química Analítica