Tunable Interferometric Effects between Single-Molecule Suzuki-Miyaura Cross-Couplings.

Abstract

Parallel two molecular bridges loaded with a palladium catalyst were integrated into separate pairs of graphene electrodes in the same device. Based on the complete description of the one-palladium catalytic pathway by single-molecule electrical spectroscopy, this setup enables the mapping of the cross-correlation between different catalysts and demonstrates the emergent complexity in the extrapolation from single molecule to ensemble. The anticorrelation behaviors at the time scale of two individual catalysts in sufficiently close proximity were revealed in the Suzuki-Miyaura cross-coupling. Further experimental evidence demonstrates that the long-range electric dipole-dipole interaction induced by solvent leads to the destructive interferometric effect of two catalysts. In contrast, the cooperative coupling of the elementary step between two catalysts affords a local acceleration. This new form of reaction dynamics measurement via focusing on multiple molecules with single-event resolution holds great promise to build a bridge between single molecule and ensemble.