Nanocavities for Molecular Optomechanics: Their Fundamental Description and Applications.

Vibrational Raman scattering-a process where light exchanges energy with a molecular vibration through inelastic scattering-is most fundamentally described in a quantum framework where both light and vibration are quantized. When the Raman scatterer is embedded inside a plasmonic nanocavity, as in some sufficiently controlled implementations of surface-enhanced Raman scattering (SERS), the coupled system realizes an optomechanical cavity where coherent and parametrically amplified light-vibration interaction becomes a resource for vibrational state engineering and nanoscale nonlinear optics. The purpose of this Perspective is to clarify the connection between the languages and parameters used in the fields of molecular cavity optomechanics (McOM) versus its conventional, "macroscopic" counterpart and to summarize the main results achieved so far in McOM and the most pressing experimental and theoretical challenges.

Optomechanical realization of the bosonic Kitaev chain.

The fermionic Kitaev chain is a canonical model featuring topological Majorana zero modes. We report the experimental realization of its bosonic analogue in a nano-optomechanical network, in which the parametric interactions induce beam-splitter coupling and two-mode squeezing among the nanomechanical modes, analogous to hopping and p-wave pairing in the fermionic case, respectively. This specific structure gives rise to a set of extraordinary phenomena in the bosonic dynamics and transport.

Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement.

Plasmon resonances at the surface of metallic antennas allow for extreme enhancement of Raman scattering. Intrinsic to plasmonics, however, is that extreme field confinement lacks precise spectral control, which would hold great promise in shaping the optomechanical interaction between light and molecular vibrations. We demonstrate an experimental platform composed of a plasmonic nanocube-on-mirror antenna coupled to an open, tunable Fabry-Perot microcavity for selective addressing of individual vibrational lines of molecules with strong Raman scattering enhancement.

Enhanced nonlinear optomechanics in a coupled-mode photonic crystal device.

The nonlinear component of the optomechanical interaction between light and mechanical vibration promises many exciting classical and quantum mechanical applications, but is generally weak. Here we demonstrate enhancement of nonlinear optomechanical measurement of mechanical motion by using pairs of coupled optical and mechanical modes in a photonic crystal device. In the same device we show linear optomechanical measurement with a strongly reduced input power and reveal how both enhancements are related.

On-chip distribution of quantum information using traveling phonons.

Distributing quantum entanglement on a chip is a crucial step toward realizing scalable quantum processors. Using traveling phonons-quantized guided mechanical wave packets-as a medium to transmit quantum states is now gaining substantial attention due to their small size and low propagation speed compared to other carriers, such as electrons or photons. Moreover, phonons are highly promising candidates to connect heterogeneous quantum systems on a chip, such as microwave and optical photons for long-distance transmission of quantum states via optical fibers.

Non-Hermitian chiral phononics through optomechanically induced squeezing.

Imposing chirality on a physical system engenders unconventional energy flow and responses, such as the Aharonov-Bohm effect and the topological quantum Hall phase for electrons in a symmetry-breaking magnetic field. Recently, great interest has arisen in combining that principle with broken Hermiticity to explore novel topological phases and applications. Here we report phononic states with unique symmetries and dynamics that are formed when combining the controlled breaking of time-reversal symmetry with non-Hermitian dynamics.

Integrated Molecular Optomechanics with Hybrid Dielectric-Metallic Resonators.

Molecular optomechanics describes surface-enhanced Raman scattering using the formalism of cavity optomechanics as a parametric coupling of the molecule's vibrational modes to the plasmonic resonance. Most of the predicted applications require intense electric field hotspots but spectrally narrow resonances, out of reach of standard plasmonic resonances. The Fano lineshapes resulting from the hybridization of dielectric-plasmonic resonators with a broad-band plasmon and narrow-band cavity mode allow reaching strong Raman enhancement with high- resonances, paving the way for sideband resolved molecular optomechanics.

Continuous-wave frequency upconversion with a molecular optomechanical nanocavity.

Coherent upconversion of terahertz and mid-infrared signals into visible light opens new horizons for spectroscopy, imaging, and sensing but represents a challenge for conventional nonlinear optics. Here, we used a plasmonic nanocavity hosting a few hundred molecules to demonstrate optomechanical transduction of submicrowatt continuous-wave signals from the mid-infrared (32 terahertz) onto the visible domain at ambient conditions. The incoming field resonantly drives a collective molecular vibration, which imprints a coherent modulation on a visible pump laser and results in upconverted Raman sidebands with subnatural linewidth.

Floquet Phonon Lasing in Multimode Optomechanical Systems.

Dynamical radiation pressure effects in cavity optomechanical systems give rise to self-sustained oscillations or 'phonon lasing' behavior, producing stable oscillators up to GHz frequencies in nanoscale devices. Like in photonic lasers, phonon lasing normally occurs in a single mechanical mode. We show here that mode-locked, multimode phonon lasing can be established in a multimode optomechanical system through Floquet dynamics induced by a temporally modulated laser drive.

Roadmap on quantum nanotechnologies.

Quantum phenomena are typically observable at length and time scales smaller than those of our everyday experience, often involving individual particles or excitations. The past few decades have seen a revolution in the ability to structure matter at the nanoscale, and experiments at the single particle level have become commonplace. This has opened wide new avenues for exploring and harnessing quantum mechanical effects in condensed matter.

Direct quantification of topological protection in symmetry-protected photonic edge states at telecom wavelengths.

Topological on-chip photonics based on tailored photonic crystals (PhCs) that emulate quantum valley-Hall effects has recently gained widespread interest owing to its promise of robust unidirectional transport of classical and quantum information. We present a direct quantitative evaluation of topological photonic edge eigenstates and their transport properties in the telecom wavelength range using phase-resolved near-field optical microscopy. Experimentally visualizing the detailed sub-wavelength structure of these modes propagating along the interface between two topologically non-trivial mirror-symmetric lattices allows us to map their dispersion relation and differentiate between the contributions of several higher-order Bloch harmonics.

Super-Resolution without Imaging: Library-Based Approaches Using Near-to-Far-Field Transduction by a Nanophotonic Structure.

Super-resolution imaging is often viewed in terms of engineering narrow point spread functions, but nanoscale optical metrology can be performed without real-space imaging altogether. In this paper, we investigate how partial knowledge of scattering nanostructures enables extraction of nanoscale spatial information from far-field radiation patterns. We use principal component analysis to find patterns in calibration data and use these patterns to retrieve the position of a point source of light.

Direct observation of topological edge states in silicon photonic crystals: Spin, dispersion, and chiral routing.

Topological protection in photonics offers new prospects for guiding and manipulating classical and quantum information. The mechanism of spin-orbit coupling promises the emergence of edge states that are helical, exhibiting unidirectional propagation that is topologically protected against back scattering. We directly observe the topological states of a photonic analog of electronic materials exhibiting the quantum spin Hall effect, living at the interface between two silicon photonic crystals with different topological order.

Synthetic gauge fields for phonon transport in a nano-optomechanical system.

Gauge fields in condensed matter physics give rise to nonreciprocal and topological transport phenomena and exotic electronic states. Nanomechanical systems are applied as sensors and in signal processing, and feature strong nonlinearities. Gauge potentials acting on such systems could induce quantum Hall physics for phonons at the nanoscale.

State Preparation and Tomography of a Nanomechanical Resonator with Fast Light Pulses.

Pulsed optomechanical measurements enable squeezing, nonclassical state creation, and backaction-free sensing. We demonstrate pulsed measurement of a cryogenic nanomechanical resonator with record precision close to the quantum regime. We use these to prepare thermally squeezed and purified conditional mechanical states, and to perform full state tomography.

Optomechanically Induced Birefringence and Optomechanically Induced Faraday Effect.

We demonstrate an optomechanical platform where optical mode conversion mediated by mechanical motion enables the arbitrary tailoring of polarization states of propagating light fields. Optomechanical interactions are realized in a Fabry-Pérot resonator, which naturally supports two polarization-degenerate states while an optical control field induces rotational symmetry breaking. Applying such principles, the entire Poincaré sphere is spanned by just optical control of the driving field, realizing reciprocal and nonreciprocal optomechanically induced birefringence for linearly polarized and circularly polarized control driving.

Controlling Nanoantenna Polarizability through Backaction via a Single Cavity Mode.

The polarizability α determines the absorption, extinction, and scattering by small particles. Beyond being purely set by scatterer size and material, in fact polarizability can be affected by backaction: the influence of the photonic environment on the scatterer. As such, controlling the strength of backaction provides a tool to tailor the (radiative) properties of nanoparticles.

Optical circulation in a multimode optomechanical resonator.

Breaking the symmetry of electromagnetic wave propagation enables important technological functionality. In particular, circulators are nonreciprocal components that can route photons directionally in classical or quantum photonic circuits and offer prospects for fundamental research on electromagnetic transport. Developing highly efficient circulators thus presents an important challenge, especially to realise compact reconfigurable implementations that do not rely on magnetic fields to break reciprocity.

Integrated nano-opto-electro-mechanical sensor for spectrometry and nanometrology.

Spectrometry is widely used for the characterization of materials, tissues, and gases, and the need for size and cost scaling is driving the development of mini and microspectrometers. While nanophotonic devices provide narrowband filtering that can be used for spectrometry, their practical application has been hampered by the difficulty of integrating tuning and read-out structures. Here, a nano-opto-electro-mechanical system is presented where the three functionalities of transduction, actuation, and detection are integrated, resulting in a high-resolution spectrometer with a micrometer-scale footprint.

Nonlinear cavity optomechanics with nanomechanical thermal fluctuations.

Although the interaction between light and motion in cavity optomechanical systems is inherently nonlinear, experimental demonstrations to date have allowed a linearized description in all except highly driven cases. Here, we demonstrate a nanoscale optomechanical system in which the interaction between light and motion is so large (single-photon cooperativity C≈10) that thermal motion induces optical frequency fluctuations larger than the intrinsic optical linewidth. The system thereby operates in a fully nonlinear regime, which pronouncedly impacts the optical response, displacement measurement and radiation pressure backaction.

The Origin and Limit of Asymmetric Transmission in Chiral Resonators.

We observe that the asymmetric transmission (AT) through photonic systems with a resonant chiral response is strongly related to the far-field properties of eigenmodes of the system. This understanding can be used to predict the AT for any resonant system from its complex eigenmodes. We find that the resonant chiral phenomenon of AT is related to, and is bounded by, the nonresonant scattering properties of the system.

Coherent Atom-Phonon Interaction through Mode Field Coupling in Hybrid Optomechanical Systems.

We propose a novel type of optomechanical coupling which enables a tripartite interaction between a quantum emitter, an optical mode, and a macroscopic mechanical oscillator. The interaction uses a mechanism we term mode field coupling: a mechanical displacement modifies the spatial distribution of the optical mode field, which, in turn, modulates the emitter-photon coupling rate. In properly designed multimode optomechanical systems, we can achieve situations in which mode field coupling is the only possible interaction pathway for the system.

Nonreciprocity and magnetic-free isolation based on optomechanical interactions.

Nonreciprocal components, such as isolators and circulators, provide highly desirable functionalities for optical circuitry. This motivates the active investigation of mechanisms that break reciprocity, and pose alternatives to magneto-optic effects in on-chip systems. In this work, we use optomechanical interactions to strongly break reciprocity in a compact system.

Perturbing Open Cavities: Anomalous Resonance Frequency Shifts in a Hybrid Cavity-Nanoantenna System.

The influence of a small perturbation on a cavity mode plays an important role in fields like optical sensing, cavity quantum electrodynamics, and cavity optomechanics. Typically, the resulting cavity frequency shift directly relates to the polarizability of the perturbation. Here, we demonstrate that particles perturbing a radiating cavity can induce strong frequency shifts that are opposite to, and even exceed, the effects based on the particles' polarizability.