Achieving strong coupling between excitons of colloidal semiconductor quantum dots (QDs) and localized surface plasmon polaritons (LSPs) is critical for advanced room-temperature quantum emitter and sensing applications. A key challenge is to have precise control of the emitters position with respect to an individual plasmonic nanostructure. Here, we present room temperature strong coupling between QDs and a single gold nano-bipyramid (BPs). The selection of the bipyramid plasmonic nanocavity offers access to a single hotspot with a very small mode volume. The localization of QDs at a single hotspot is achieved via plasmon-triggered two-photon polymerization. This technique exploits the enhanced electric field at the BP tip to selectively polymerize a photosensitive QD-containing formulation. Room-temperature scattering spectra of a 3-QD-BP system reveal Rabi splitting of 349.3 meV and a coupling strength of 175.68 meV. The with distinct anti-crossing behavior is confirmed by simulations. This approach simplifies QD integration for strong coupling systems compared to previous methods. These results indicate a scalable platform for solid-state quantum technologies with colloidal QDs, enabling explora-tion of exciton-plasmon interactions and further advance-ment of applications in quantum optics and quantum sensing under ambient conditions.
Comments
8 pages, 4 figures and extra supplementary material
Achieving strong coupling between excitons of colloidal semiconductor quantum dots (QDs) and localized surface plasmon polaritons (LSPs) is critical for advanced room-temperature quantum emitter and sensing applications. A key challenge is to have precise control of the emitters position with respect to an individual plasmonic nanostructure. Here, we present room temperature strong coupling between QDs and a single gold nano-bipyramid (BPs). The selection of the bipyramid plasmonic nanocavity offers access to a single hotspot with a very small mode volume. The localization of QDs at a single hotspot is achieved via plasmon-triggered two-photon polymerization. This technique exploits the enhanced electric field at the BP tip to selectively polymerize a photosensitive QD-containing formulation. Room-temperature scattering spectra of a 3-QD-BP system reveal Rabi splitting of 349.3 meV and a coupling strength of 175.68 meV. The with distinct anti-crossing behavior is confirmed by simulations. This approach simplifies QD integration for strong coupling systems compared to previous methods. These results indicate a scalable platform for solid-state quantum technologies with colloidal QDs, enabling explora-tion of exciton-plasmon interactions and further advance-ment of applications in quantum optics and quantum sensing under ambient conditions.
Strong light–matter interaction is at the heart of modern quantum technological applications and is the basis for a wide range of rich optical phenomena. Coupling a single quantum emitter strongly with electromagnetic fields provides an unprecedented control over its quantum states and enables high-fidelity quantum operations. However, single-emitter strong coupling is exceptionally fragile and has been realized mostly at cryogenic temperatures. Recent experiments have, however, demonstrated that single-emitter strong coupling can be realized at room temperature by using plasmonic nanocavities that confine optical fields via surface plasmons strongly on metal surfaces and facilitate sub-picosecond light–matter interaction. Here, we outline recent theoretical developments and experimental demonstrations of room-temperature strong coupling in the plasmonic platform, from emitter ensembles down to the single emitter limit, before placing a focus on selective studies that explore and provide insight into applications of plexcitonic strong coupling including sensing of single biological molecules, qubit entanglement generation, and reconfigurable single-photon sources and provide an outline of research directions in quantum sensing, quantum information processing, and ultrafast spectroscopy.
Quantum strong coupling between emitters and cavities generates hybrid modes which provide a platform for quantum devices. The atom based systems require precise control over the position of atoms within the cavity and are difficult to be integrated on a chip. The quantum dots-photonic crystal system is limited to the cryogenic temperature. On the contrary, the molecule-plasmonic cavity is a good candidate for chip scale, room temperature operating strong coupling units due to the extremely small mode volume of plasmonic nanocavities. However, to precisely position a single or a few molecules into a plasmonic nanocavity is challenging. In this work, a few molecules are integrated into the nanocavity through oligonucleotides. The clear Rabi splitting is observed and the anti-crossing curve shows a clear verification of coupling. The number of fluorophore integrated into the nanocavity is estimated to be one. The deterministic strong coupling may be realized based on this configuration.
Quantum technologies are widely expected to bring a revolution in communications and information technologies in the coming decade allowing, for example, un-paralleled levels of secure communications. For quantum communication, photonic quantum effects have played a central role, but most photonic solutions and systems based on light-matter interaction also require cryogenic environments. Strong coupling of light and matter at the single emitter level is a fundamental quantum resource offering deterministic energy exchange between single photons and a two-level system, and the possibility to achieve single-photon nonlinearities via the anharmonicity of the Jaynes-Cummings ladder. Until recently, however, the conditions for achieving strong-coupling were most commonly met at cryogenic temperatures such that de-coherence processes are suppressed. As a major step forward, we have recently demonstrated room-temperature strong coupling of single molecules [1] and single quantum dots [2] to ultra-confined light fields in plasmonic resonators at ambient conditions. The fact that strong-coupling conditions may be reached at room temperature is of immense interest because it represents a clear route to a practical implementation and use of quantum behaviour in nanophotonic systems and its application in bio-sensing [3]. The talk will discuss how nanoplasmonics can be an enabler of ultrafast room-temperature quantum nanophotonic networks via strong coupling and ultrafast quantum dynamics [4]. We will highlight the physics associated with recently demonstrated room-temperature strong coupling of single molecules in a plasmonic nano-cavity [1] and near-field generated strong coupling of single quantum dots [2] and single quantum emitter Dicke enhancement [5] paving the road towards single-photon quantum nonlinearities. The presentation will also explain near-field enhanced single-photon emission in near-zero index materials [6] and ultrafast multi-partite quantum entanglement [7]. This provides the foundation for unprecedented control over photon number, single photon dynamics, and dynamic multi-photon coherence. These properties are all imperative for the development of next-generation, nanoscale building blocks in ambient-temperature photonic quantum communication technologies.
Abstract 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.
Abstract Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g (2) (0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.
Light-matter superposition states obtained via strong coupling play a decisive role in quantum information processing, but the deleterious effects of material dissipation and environment-induced decoherence inevitably destroy coherent light-matter polaritons over time. Here, we propose the use of coherent perfect absorption under near-field driving to prepare and protect the polaritonic states of a single quantum emitter interacting with a plasmonic nanocavity at room temperature. Our scheme of quantum nanoplasmonic coherent perfect absorption leverages an inherent frequency specificity to selectively initialize the coupled system in a chosen plasmon-emitter dressed state, while the coherent, unidirectional and non-perturbing near-field energy transfer from a proximal plasmonic waveguide can in principle render the dressed state robust against dynamic dissipation under ambient conditions. Our study establishes a previously unexplored paradigm for quantum state preparation and coherence preservation in plasmonic cavity quantum electrodynamics, offering compelling prospects for elevating quantum nanophotonic technologies to ambient temperatures.