Optical cavities can enhance and control light-matter interactions. This level of control has recently been extended to the nanoscale with single emitter strong coupling even at room temperature using plasmonic nanostructures. However, emitters in static geometries, limit the ability to tune the coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) with a nanocavity formed between a scanning plasmonic antenna tip and the substrate. By reversibly and dynamically addressing single quantum dots, we observe mode splitting up to 160 meV and anticrossing over a detuning range of ~100 meV, and with subnanometer precision over the deep subdiffraction-limited mode volume. Thus, TESC enables previously inaccessible control over emitter-nanocavity coupling and mode volume based on near-field microscopy. This opens pathways to induce, probe, and control single-emitter plasmon hybrid quantum states for applications from optoelectronics to quantum information science at room temperature.

H, O, and F functionalized 2D Te. H-β-Te becomes indirect semiconductor, O-β-Te becomes metallic (both stable). Investigated binding to substrate.

Quantum state control of two‐level emitters is fundamental for many information processing, metrology, and sensing applications. However, quantum‐coherent photonic control of solid‐state emitters has traditionally been limited to cryogenic environments, which are not compatible with implementation in scalable, broadly distributed technologies. In contrast, plasmonic nano‐cavities with deep sub‐wavelength mode volumes have recently emerged as a path toward room temperature quantum control. However, optimization, control, and modeling of the cavity mode volume are still in their infancy. Here recent demonstrations of plasmonic tip‐enhanced strong coupling (TESC) with a configurable nano‐tip cavity are extended to perform a systematic experimental investigation of the cavity‐emitter interaction strength and its dependence on tip position, augmented by modeling based on both classical electrodynamics and a quasinormal mode framework. Based on this work, a perspective for nano‐cavity optics is provided as a promising tool for room temperature control of quantum coherent interactions that could spark new innovations in fields from quantum information and quantum sensing to quantum chemistry and molecular opto‐mechanics.