Version 2 2023-12-15, 23:33Version 2 2023-12-15, 23:33
Version 1 2023-12-11, 22:00Version 1 2023-12-11, 22:00
journal contribution
posted on 2023-12-15, 23:33authored byXiaomei 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, Xiang Lan
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 DNA-templated 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.