%0 Journal Article
%A Mo, Xiaomei
%A Li, Huacheng
%A Tang, Pan
%A Hao, Yaya
%A Dong, Bingqian
%A Marazuela Lamata, María Dolores
%A Gómez Gómez, María Milagros
%A Zhu, Xianfeng
%A Li, Qian
%A Lora Maroto, Beatriz
%A Jiang, Shuoxing
%A Fan, Chunhai
%A Lan, Xiang
%T DNA-Modulated and Mechanoresponsive Excitonic Couplings Reveal Chiroptical Correlation of Conformation, Tension, and Dynamics of DNA Self-Assembly
%D 2023
%@ 1530-6984
%U https://hdl.handle.net/20.500.14352/92251
%X Study 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.
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