Control of plasmon emission and dynamics at the transition from classical to quantum coupling
Reviews and Highlights | Quantum Science | Molecular and Soft-matter | Ultrafast Nano-optics and Nanophotonics | Mineralogy and Geochemistry |
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Vasily Kravtsov, Samuel Berweger, Joanna M. Atkin, and Markus B. Raschke
Nano Lett. 14, 5270 (2014).
DOI PDF
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With nanosecond radiative lifetimes, quenching dominates over enhancement for conventional fluorescence emitters near metal interfaces. We explore the fundamentally distinct behavior of photoluminescence (PL) with few-femtosecond radiative lifetimes of a coupled plasmonic emitter. Controlling the emitter−surface distance with subnanometer precision by combining atomic force and scanning tunneling distance control, we explore the unique behavior of plasmon dynamics at the transition from long-range classical resonant energy transfer to quantum coupling. Because of the ultrafast radiative plasmon emission, classical quenching is completely suppressed. Field-enhanced behavior dominates until the onset of quantum coupling dramatically reduces emission intensity and field enhancement, as verified in concomitant tip-enhanced Raman measurements. The entire distance behavior from tens of nanometers to subnanometers can be described using a phenomenological rate equation model and highlights the new degrees of freedom in radiation control enabled by an ultrafast radiative emitter near surfaces.