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Nature Communications

Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity

Oluwafemi Stephen Ojambati, Rohit Chikkaraddy, William Deacon, Matthew J. Horton, Dean Kos, Vladimir A. Turek, Ulrich F. Keyser, Jeremy J. Baumberg

Published Mar 5, 2019• 174 citations
Publisher

Abstract

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.

DOI
10.1038/s41467-019-08611-5

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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.
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.
The coherent interaction between quantum emitters and photonic modes in cavities underlies many of the current strategies aiming at generating and controlling photonic quantum states. A plasmonic nanocavity provides a powerful solution for reducing the effective mode volumes down to nanometre scale, but spatial control at the atomic scale of the coupling with a single molecular emitter is challenging. Here we demonstrate sub-nanometre spatial control over the coherent coupling between a single molecule and a plasmonic nanocavity in close proximity by monitoring the evolution of Fano lineshapes and photonic Lamb shifts in tunnelling electron-induced luminescence spectra. The evolution of the Fano dips allows the determination of the effective interaction distance of ∼1 nm, coupling strengths reaching ∼15 meV and a giant self-interaction induced photonic Lamb shift of up to ∼3 meV. These results open new pathways to control quantum interference and field-matter interaction at the nanoscale.
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.
Quantum plasmonics extends cavity quantum electrodynamics (cQED) concepts to the nanoscale, benefiting from the strongly subwavelength confinement of the plasmon modes supported by metal nanostructures. In this work, we describe in detail collective strong coupling to a plasmonic nanocavity. Similarities and differences to cQED are emphasized. We notably observe that the Rabi splitting can strongly deviate from the standard NeΔΩ1 law, where Ne is the number of emitters and ΔΩ1 is the Rabi splitting for a single emitter. In addition, we discuss the collective Lamb shift and the role of quantum corrections to the emission spectra.
Abstract In the light–matter strong coupling regime, the excited state of quantum emitters is inextricably linked to a photonic mode, leading to hybrid states that are part light and part matter. Recently, there has been a huge effort to realize strong coupling with nanoplasmonics, since it provides a versatile environment to study and control molecules in ambient conditions. Among the most promising designs are plasmonic nanocavities that confine light to unprecedentedly small volumes. Such nanocavities, though, support multiple types of modes, with different field profiles and radiative decay rates (bright and dark modes). Here, we show theoretically that the different nature of these modes leads to mode beating within the nanocavity and the Rabi oscillations, which alters the spatiotemporal dynamics of the hybrid system. By specifically designing the illumination setup, we decompose and control the dark and bright plasmon mode excitation and therefore their coupling with quantum emitters. Hence, this work opens new routes for dynamically dressing emitters, to tailor their hybrid states with external radiation.