Abstract
Confinement effect at microscale level is ubiquitous in biosystems and microreactors, but its mechanism remains debated. Herein we discovered that the multimode competition of molecular vibrational strong coupling (VSC) with optical resonators can well account for the confinement effects as reflected by the efficacy of enzymatic ATP hydrolysis. As O-H stretching vibration coupling with 6th cavity mode, the VSC effect on ATP hydrolysis shows significant enhancement, while VSC with higher cavity modes will gradually reduce such effect due to the multimodal competition. The higher the cavity mode coupled with, the closer to the outside of Fabry-Pérot cavity. Moreover, the underlying mechanism of VSC effect on ATP hydrolysis could be originated from the Rabi splitting of hydrogen bond landscape, mainly altering the binding affinity between Ca2+ and ATPase. This research deepens our understanding of the microscale confinement effect on reactions from the aspect of quantum mechanism, which can guide the rational design of microreactors.
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