Coherent Electron-Vibron Interactions in Surface-Enhanced Raman Scattering (SERS).

In this Letter we identify coherent electron-vibron interactions between near-resonant and nonresonant electronic levels that contribute beyond standard optomechanical models for off-resonant or resonance surface-enhanced Raman scattering (SERS). By developing an open-system quantum model using first molecular interaction principles, we show how the Raman interference of both resonant and nonresonant contributions can provide several orders of magnitude modifications of the SERS peaks with respect to former optomechanical models and over the fluorescence backgrounds. This cooperative optomechanical mechanism allows for generating an enhancement of nonclassical photon pair correlations between Stokes and anti-Stokes photons, which can be detected by photon-counting measurements. Our results demonstrate Raman enhancements and suppressions of coherent nature that significantly impact the standard estimations of the optomechanical contribution from SERS spectra and their quantum mechanical observable effects.

Engineering Long-Lived Vibrational States for an Organic Molecule.

The optomechanical character of molecules was discovered by Raman about one century ago. Today, molecules are promising contenders for high-performance quantum optomechanical platforms because their small size and large energy-level separations make them intrinsically robust against thermal agitations. Moreover, the precision and throughput of chemical synthesis can ensure a viable route to quantum technological applications. The challenge, however, is that the coupling of molecular vibrations to environmental phonons limits their coherence to picosecond time scales. Here, we improve the optomechanical quality of a molecule by several orders of magnitude through phononic engineering of its surrounding. By dressing a molecule with long-lived high-frequency phonon modes of its nanoscopic environment, we achieve storage and retrieval of photons at millisecond timescales and allow for the emergence of single-photon strong coupling in optomechanics. Our strategy can be extended to the realization of molecular optomechanical networks.

Single-Molecule Vacuum Rabi Splitting: Four-Wave Mixing and Optical Switching at the Single-Photon Level.

A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this Letter, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generation and all-optical switching. Our work promotes the use of molecules for applications such as integrated photonic circuits operating at very low powers.

Quantum Metamaterials with Magnetic Response at Optical Frequencies.

We propose novel quantum antennas and metamaterials with a strong magnetic response at optical frequencies. Our design is based on the arrangement of natural quantum emitters with only electric dipole transition moments at distances smaller than a wavelength of light but much larger than their physical size. In particular, we show that an atomic dimer can serve as a magnetic antenna at its antisymmetric mode to enhance the decay rate of a magnetic transition in its vicinity by several orders of magnitude. Furthermore, we study metasurfaces composed of atomic bilayers with and without cavities and show that they can fully reflect the electric and magnetic fields of light, thus, forming nearly perfect electric or magnetic mirrors. The proposed metamaterials will embody the intrinsic quantum functionalities of natural emitters such as atoms, ions, color center, or molecules and can be fabricated with available state-of-the-art technologies, promising several applications both in classical optics and quantum engineering.

Small slot waveguide rings for on-chip quantum optical circuits.

Nanophotonic interfaces between single emitters and light promise to enable new quantum optical technologies. Here, we use a combination of finite element simulations and analytic quantum theory to investigate the interaction of various quantum emitters with slot-waveguide rings. We predict that for rings with radii as small as 1.44 µm, with a Q-factor of 27,900, near-unity emitter-waveguide coupling efficiencies and emission enhancements on the order of 1300 can be achieved. By tuning the ring geometry or introducing losses, we show that realistic emitter-ring systems can be made to be either weakly or strongly coupled, so that we can observe Rabi oscillations in the decay dynamics even for micron-sized rings. Moreover, we demonstrate that slot waveguide rings can be used to directionally couple emission, again with near-unity efficiency. Our results pave the way for integrated solid-state quantum circuits involving various emitters.

Large suppression of quantum fluctuations of light from a single emitter by an optical nanostructure.

We investigate the reduction of the electromagnetic field fluctuations in resonance fluorescence from a single emitter coupled to an optical nanostructure. We find that such hybrid systems can lead to the creation of squeezed states of light, with quantum fluctuations significantly below the shot-noise level. Moreover, the physical conditions for achieving squeezing are strongly relaxed with respect to an emitter in free space. A high degree of control over squeezed light is feasible both in the far and near fields, opening the pathway to its manipulation and applications on the nanoscale with state-of-the-art setups.

Conformal surface plasmons propagating on ultrathin and flexible films.

Surface plasmon polaritons (SPPs) are localized surface electromagnetic waves that propagate along the interface between a metal and a dielectric. Owing to their inherent subwavelength confinement, SPPs have a strong potential to become building blocks of a type of photonic circuitry built up on 2D metal surfaces; however, SPPs are difficult to control on curved surfaces conformably and flexibly to produce advanced functional devices. Here we propose the concept of conformal surface plasmons (CSPs), surface plasmon waves that can propagate on ultrathin and flexible films to long distances in a wide broadband range from microwave to mid-infrared frequencies. We present the experimental realization of these CSPs in the microwave regime on paper-like dielectric films with a thickness 600-fold smaller than the operating wavelength. The flexible paper-like films can be bent, folded, and even twisted to mold the flow of CSPs.

Waveguided spoof surface plasmons with deep-subwavelength lateral confinement.

We present a new type of waveguide scheme for terahertz circuitry based on the concept of spoof surface plasmons. This structure is composed of a one-dimensional array of L-shaped metallic elements horizontally attached to a metal surface. The dispersion relation of the surface electromagnetic modes supported by this system presents a very weak dependence with the lateral dimension and the modes are very deep-subwavelength confined with a long-enough propagation length.

Resonance energy transfer and superradiance mediated by plasmonic nanowaveguides.

We show how both the subwavelength confinement associated with surface plasmons and the one-dimensional character of plasmonic waveguides can be exploited to enhance the coupling between quantum emitters. Resonance energy transfer and the phenomenon of superradiance are investigated in three different waveguiding schemes (wires, wedges, and channels) by means of the Finite Element Method. We also develop a simplified model that is able to capture the main features of the numerical results.