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Plasmon resonance biosensors provide ultimate sensitivity at the single-molecule level. This sensitivity is, however, associated with a nanometer-sized confined hotspot, and molecular transport toward the sensor relies on inefficient diffusion. Here, we combine a plasmonic nanoantenna with a solid-state nanopore and demonstrate that single DNA molecules can be efficiently delivered to the plasmonic hotspots and detected in a label-free manner at submillisecond acquisition rates by monitoring the backscattered light intensity from the plasmonic nanoantennas. Our method realizes a better than 200 μs temporal resolution together with a down to subsecond waiting time, which is orders of magnitude better than traditional single-molecule plasmonic resonance sensing methods. Furthermore, the electric field applied to the nanopore can actively drive biomolecules away from the hotspot, preventing molecules to permanently bind to the gold sensor surface and allowing efficient reuse of the sensor. Our plasmonic nanopore sensor thus significantly outperforms conventional plasmon resonance sensors and provides great opportunities for high-throughput optical single-molecule-sensing assays.

Active Delivery of Single DNA Molecules into a Plasmonic Nanopore for Label-Free Optical Sensing