Vibrational strong coupling (VSC) has been an emerging tool to regulate the energy landscape of chemical bonds. VSC can be achieved by tuning the optical mode of Fabry-Peŕot (FP) cavities to resonantly couple with molecular vibrations, which generates new light-molecule hybrid states and energy levels, thereby directly influencing chemical reactions. Herein, VSC with FP cavities can significantly reduce the melting temperature (T m ) of dsDNA, which can be precisely measured using DNA origami coassembly, benefiting from the precise hybridization-dependent origami conformation. An 8.5-μm-spaced FP cavity can strongly couple with the vibration of the pyridine bases, exhibiting the most optimized enhancing effect on directly driving the coassembly of DNA origami in FP cavities. This work sheds light on the quantum mechanism in life and in turn holds great promise to develop innovative techniques to regulate life.

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