Physical Review Letters · 2015 · 543 citations · 47 references
Quantum PhotonicsOptical MaterialsNano-opticsEngineeringPlasmon-enhanced PhotovoltaicsStrong Light-matter InteractionsQuantum MetamaterialsPolariton DynamicOptical PropertiesPlasmonic NanocavitiesNanophotonicsPlasmonic MaterialPhotonicsQuantum SciencePhysicsAmbient ConditionsNanotechnologyPhotonic MaterialsLight–matter InteractionMolecular ExcitonsPlasmonicsRoom TemperatureApplied PhysicsPlasmon ResonancesQuantum DevicesNanofabrication
Strong light‑matter interactions between two‑level systems and resonant cavities enable single‑photon optical nonlinearities, yet achieving them has required cryogenic temperatures and ultrahigh vacuum, and room‑temperature plasmonic attempts have not yet succeeded at the single‑nanoparticle level. The study aims to realize strong coupling between a single silver nanoprism’s plasmons and excitons in molecular J aggregates at ambient conditions. This is accomplished by confining plasmons within a single silver nanoprism and coupling them to excitons in molecular J aggregates under room‑temperature conditions. The resulting sub‑wavelength mode volume and high quality factor yield a strong‑coupling figure of merit Q/√V ≈ 6×10³ μm⁻³ᐟ², comparable to state‑of‑the‑art photonic crystal and microring resonators, demonstrating that silver nanoprisms can enable room‑temperature quantum optics.
Realizing strong light-matter interactions between individual two-level systems and resonating cavities in atomic and solid state systems opens up possibilities to study optical nonlinearities on a single-photon level, which can be useful for future quantum information processing networks. However, these efforts have been hampered by unfavorable experimental conditions, such as cryogenic temperatures and ultrahigh vacuum, required to study such systems and phenomena. Although several attempts to realize strong light-matter interactions at room temperature using plasmon resonances have been made, successful realizations on the single-nanoparticle level are still lacking. Here, we demonstrate the strong coupling between plasmons confined within a single silver nanoprism and excitons in molecular J aggregates at ambient conditions. Our findings show that deep subwavelength mode volumes V together with quality factors Q that are reasonably high for plasmonic nanostructures result in a strong-coupling figure of merit-Q/sqrt[V] as high as ∼6×10^{3} μm^{-3/2}, a value comparable to state-of-the-art photonic crystal and microring resonator cavities. This suggests that plasmonic nanocavities, and specifically silver nanoprisms, can be used for room temperature quantum optics.
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