Asynchronous locking in metamaterials of fluids of light and sound.

Lattices of exciton-polariton condensates represent an attractive platform for the study and implementation of non-Hermitian bosonic quantum systems with strong non-linear interactions. The possibility to actuate on them with a time dependent drive could provide for example the means to induce resonant inter-level transitions, or to perform Floquet engineering or Landau-Zener-Stückelberg state preparation. Here, we introduce polaromechanical metamaterials, two-dimensional arrays of µm-sized traps confining zero-dimensional light-matter polariton fluids and GHz phonons. A strong exciton-mediated polariton-phonon interaction induces a time-dependent inter-site polariton coupling J(t) with remarkable consequences for the dynamics. When locally perturbed by continuous wave optical excitation, a mechanical self-oscillation sets-in and polaritons respond by locking the energy detuning between neighbor sites at integer multiples of the phonon energy, evidencing asynchronous locking involving the polariton and phonon fields. These results open the path for the coherent control of dissipative quantum light fluids with hypersound in a scalable platform.

Polariton-driven phonon laser.

Efficient generation of phonons is an important ingredient for a prospective electrically-driven phonon laser. Hybrid quantum systems combining cavity quantum electrodynamics and optomechanics constitute a novel platform with potential for operation at the extremely high frequency range (30-300 GHz). We report on laser-like phonon emission in a hybrid system that optomechanically couples polariton Bose-Einstein condensates (BECs) with phonons in a semiconductor microcavity. The studied system comprises GaAs/AlAs quantum wells coupled to cavity-confined optical and vibrational modes. The non-resonant continuous wave laser excitation of a polariton BEC in an individual trap of a trap array, induces coherent mechanical self-oscillation, leading to the formation of spectral sidebands displaced by harmonics of the fundamental 20 GHz mode vibration frequency. This phonon "lasing" enhances the phonon occupation five orders of magnitude above the thermal value when tunable neighbor traps are red-shifted with respect to the pumped trap BEC emission at even harmonics of the vibration mode. These experiments, supported by a theoretical model, constitute the first demonstration of coherent cavity optomechanical phenomena with exciton polaritons, paving the way for new hybrid designs for quantum technologies, phonon lasers, and phonon-photon bidirectional translators.

Optomechanical properties of GaAs/AlAs micropillar resonators operating in the 18 GHz range.

Recent experiments demonstrated that GaAs/AlAs based micropillar cavities are promising systems for quantum optomechanics, allowing the simultaneous three-dimensional confinement of near-infrared photons and acoustic phonons in the 18-100 GHz range. Here, we investigate through numerical simulations the optomechanical properties of this new platform. We evidence how the Poisson's ratio and semiconductor/vacuum boundary conditions lead to very distinct features in the mechanical and optical three-dimensional confinement. We find a strong dependence of the mechanical quality factor and strain distribution on the micropillar radius, in great contrast to what is predicted and observed in the optical domain. The derived optomechanical coupling constants g0 reach ultra-large values in the 106 rad/s range.

Micropillar Resonators for Optomechanics in the Extremely High 19-95-GHz Frequency Range.

Strong confinement, in all dimensions, and high mechanical frequencies are highly desirable for quantum optomechanical applications. We show that GaAs/AlAs micropillar cavities fully confine not only photons but also extremely high frequency (19-95 GHz) acoustic phonons. A strong increase of the optomechanical coupling upon reducing the pillar size is observed, together with record room-temperature Q-frequency products of 10^{14}. These mechanical resonators can integrate quantum emitters or polariton condensates, opening exciting perspectives at the interface with nonlinear and quantum optics.

Multiple Quantum Wells for PT-Symmetric Phononic Crystals.

We demonstrate that the parity-time symmetry for sound is realized in laser-pumped multiple-quantum-well structures. Breaking of the parity-time symmetry for the phonons with wave vectors corresponding to the Bragg condition makes the structure a highly selective acoustic wave amplifier. Single-mode distributed feedback phonon lasing is predicted for structures with realistic parameters.

Towards GHz-THz cavity optomechanics in DBR-based semiconductor resonators.

Resonators based on acoustic distributed Bragg reflectors (DBRs) were optimized to work in the GHz-THz regime, and grown by molecular beam epitaxy. We show that in structures made of GaAlAs alloys a simultaneous optimal confinement of light in the visible range and phonons in the tens of GHz range can be achieved. We report time resolved differential optical reflectivity experiments performed with fs-ps laser pulses. The experimental results are in excellent agreement with simulations based on standard transfer matrix methods. The resonant behavior of the photoelastic coefficient is discussed. The perfect optic-acoustic mode overlapping, added to a strongly enhanced coupling mechanism, implies that these DBR-based cavities could be the base of highly efficient optomechanical resonators.

Polariton Resonances for Ultrastrong Coupling Cavity Optomechanics in GaAs/AlAs Multiple Quantum Wells.

Polariton-mediated light-sound interaction is investigated through resonant Brillouin scattering experiments in GaAs/AlAs multiple-quantum wells. Photoelastic coupling enhancement at exciton-polariton resonance reaches 10(5) at 30 K as compared to a typical bulk solid room temperature transparency value. When applied to GaAs based cavity optomechanical nanodevices, this result opens the path to huge displacement sensitivities and to ultrastrong coupling regimes in cavity optomechanics with couplings g(0) in the range of 100 GHz.

Strong optical-mechanical coupling in a vertical GaAs/AlAs microcavity for subterahertz phonons and near-infrared light.

We show that distributed Bragg reflector GaAs/AlAs vertical cavities designed to confine photons are automatically optimal to confine phonons of the same wavelength, strongly enhancing their interaction. We study the impulsive generation of intense coherent and monochromatic acoustic phonons by following the time evolution of the elastic strain in picosecond-laser experiments. Efficient optical detection is assured by the strong phonon backaction on the high-Q optical cavity mode. Large optomechanical factors are reported (~THz/nm range). Pillar cavities based in these structures are predicted to display picogram effective masses, almost perfect sound extraction, and threshold powers for the stimulated emission of phonons in the range µW-mW, opening the way for the demonstration of phonon "lasing" by parametric instability in these devices.

Magneto-optical enhancement by plasmon excitations in nanoparticle/metal structures.

Coupling magnetic materials to plasmonic structures provides a pathway to dramatically increase the magneto-optical response of the resulting composite architecture. Although such optical enhancement has been demonstrated in a variety of systems, some basic aspects are scarcely known. In particular, reflectance/transmission modulations and electromagnetic field intensification, both triggered by plasmon excitations, can contribute to the magneto-optical enhancement. However, a quantitative evaluation of the impact of both factors on the magneto-optical response is lacking. To address this issue, we have measured magneto-optical Kerr spectra on corrugated gold/dielectric interfaces with magnetic (nickel and iron oxide) nanoparticles. We find that the magneto-optical activity is enhanced by up to an order of magnitude for wavelengths that are correlated to the excitation of propagating or localized surface plasmons. Our work sheds light on the fundamental principles for the observed optical response and demonstrates that the outstanding magneto-optical performance is originated by the increase of the polarization conversion efficiency, whereas the contribution of reflectance modulations is negligible.

Bi-analyte single molecule SERS technique with simultaneous spatial resolution.

The simultaneous combination on CCD detectors of both spectral and spatial information is used in the framework of the single molecule (SM) bi-analyte Surface-Enhanced Raman Scattering (SERS) technique, to provide a new level of understanding on the origins of SM-spectra, as well as reveal the advantages and limitations of the statistical identification of SM-events. A new and deeper interpretation of the roots of the inhomogeneous broadening of single molecule Raman peaks can be uncovered, as well as the origin of Surface-Enhanced Fluorescence (SEF) emission by single molecules. In this manner, subtler aspects of SM-SERS spectroscopy can be revealed by the additional presence of spatial information on the localization of single molecules producing the signal. The spatial information is normally lost through the standard binning of CCD cameras for spectroscopy, which only emphasizes the spectral dimension of the problem. This novel extension of the bi-analyte SM-SERS method should contribute to the furtherance of the technique, and several of its fundamental aspects are discussed in detail.

Bloch oscillations of THz acoustic phonons in coupled nanocavity structures.

Nanophononic Bloch oscillations and Wannier-Stark ladders have been recently predicted to exist in specifically tailored structures formed by coupled nanocavities. Using pump-probe coherent phonon generation techniques we demonstrate that Bloch oscillations of terahertz acoustic phonons can be directly generated and probed in these complex nanostructures. In addition, by Fourier transforming the time traces we had access to the proper eigenmodes in the frequency domain, thus evidencing the related Wannier-Stark ladder. The observed Bloch oscillation dynamics are compared with simulations based on a model description of the coherent phonon generation and photoelastic detection processes.

Enhancement and inhibition of coherent phonon emission of a Ni film in a BaTiO3/SrTiO3 cavity.

We report pump-probe time resolved reflectivity experiments in a hybrid air-Ni metal-BaTiO(3)/SrTiO(3) oxide mirror phonon cavity. We demonstrate that the generated coherent acoustic phonon spectra of the impulsively excited metallic film can be inhibited or enhanced in the phonon cavity with respect to a Ni film directly grown on a SrTiO(3) substrate. The experiments are compared with simulations that highlight the role of the phonon density of states in the coherent acoustic emission, extending concepts at the base of the optical Purcell effect to the field of phononics.

Lifetime of THz acoustic nanocavity modes.

We present an ultrahigh resolution Raman study of the lifetime of 1 THz acoustic phonons confined in nanocavities. We demonstrate that the cavity Q factor can be controlled by design. Anharmonicity contributes only marginally to limit the cavity phonon lifetime, even at room temperature, while thickness fluctuations in the scale of 1/10 of a unit cell are the main limitation for the performance of THz phonon cavities.

Ferroelectricity-induced coupling between light and terahertz-frequency acoustic phonons in BaTiO3/SrTiO3 superlattices.

We report a UV-Raman study of folded acoustic vibrations in epitaxial ferroelectric BaTiO3/SrTiO3 superlattices. The folded acoustic doublets show an anomalous temperature dependence disappearing above the ferroelectric transition, which is tuned by varying the thickness of the BaTiO3 and SrTiO3 layers. A mechanism involving the acoustic phonon modulation of the spatially periodic ferroelectric polarization explains the observed temperature dependence. These results demonstrate the strong coupling between sound, charge, and light in these multifunctional nanoscale ferroelectrics.

Wired-enzyme core-shell Au nanoparticle biosensor.

We report a fully integrated core-shell nanoparticle system responsive to glucose. The system is comprised of self-assembled glucose oxidase and an osmium molecular wire on core-shell Au nanoparticles. Characterization of the functional nanoparticles by spectroscopy, quartz crystal microbalance and electrochemical techniques has shown that the catalytically active shell has a structure as designed and all components are active in the self-assembled multilayer shell. Furthermore, amperometric reagentless detection of glucose and contactless photonic biosensing by the Os(II) resonant Raman signal have been demonstrated. The enzymatic reduction of FAD by glucose and further reduction of the Raman silent Os(III) by FADH 2 yields a characteristic enzyme-substrate calibration curve in the millimolar range. Furthermore, coupling of electronic resonant Raman of the osmium complex with the SERS amplification by Au NPs plasmon resonance has been demonstrated which leads to an extra enhancement of the biosensor signal. We present a proof of concept extending the work done with planar surfaces to core-shell NPs as an advance in the design of glucose-responsive chemistry detected by SERS-like methods.

Selective optical generation of coherent acoustic nanocavity modes.

Femtosecond pump-probe experiments on a Ga0.85In0.15As nanocavity enclosed by two Ga(0.85)In(0.15)As/AlAs phonon Bragg mirrors reveal selective generation of terahertz confined acoustic modes and regular folded phonons. Selective generation of the confined modes alone is achievable for laser excitation at certain energies below the mirror absorption edges, corresponding to electronic transitions within the cavity layer only. Calculations based on the photoelastic effect explain the experimental results. Decay times of cavity and regular modes evidence longer decay times and anharmonic effects for the cavity mode.

Restricted surface mobility of thiolate-covered metal surfaces: a simple strategy to produce high-area functionalized surfaces.

We have studied the self-assembly of thiol monolayers on high-area nanostructured gold surfaces. These surfaces are highly irregular with a fractal dimension close to 2.5. Auger electron spectroscopy and voltammetric data indicate that thiol self-assembly with a maximum surface coverage approximately 1/3 takes place, the same result as that found for smooth gold surfaces. Therefore, neither curvature effects, which would promote higher coverage, nor excluded volume effects, which would result in lower coverage, are present in these irregular surfaces. The high surface area of the bare electrodes exhibits a rapid surface decay in different liquid media that is hindered by alkanethiolate chemisorption. The presence of thiolate SAMs reduces markedly the mass transport surface diffusion of gold adatoms, hindering surface area decay and freezing the system in a metastable state for days. This effect cannot be explained by considering only hydrocarbon-hydrocarbon chain interactions, because it is also observed for ordered arrays of adsorbed S atoms. Therefore, interactions between ordered chemisorbed species at high coverage seem to be responsible for the observed behavior. The thiol-covered high-area metallic substrates can be used to efficiently anchor a large number of molecules, biomolecules, or nanostructures, improving the performance of SAM-based optical and electrochemical devices.

Coherent generation of acoustic phonons in an optical microcavity.

Ultrafast coherent generation of acoustic phonons is studied in a semiconductor optical microcavity. The confinement of the light pulse amplifies both the generation and the detection of phonons. In addition, the standing wave character of the photon field modifies the generation and detection phonon bandwidth. Coherent generation experiments in an acoustic nanocavity embedded in an optical microcavity are reported as a function of laser energy and incidence angle to evidence the separate role of the optical and exciton resonances. Amplified signals and phonon spectra modified by the optical confinement are demonstrated.

Subterahertz phonon dynamics in acoustic nanocavities.

We report a direct determination of the dynamic behavior of confined acoustic phonons in nanocavities by picosecond acoustics. We provide the broadband, high resolution transmission amplitude curve in the subterahertz range, and we give evidence of resonant transmission peaks in three successive stop bands, in quantitative agreement with acoustic simulations. We furthermore demonstrate transit times in the nanosecond range at the cavity peaks reflecting the strong confinement of resonant phonons within the cavity layer. On the other hand, picosecond transit times are measured in the stop band, shorter than in any of the constituting materials, a tunneling effect well known both in photonic crystals and in macroscopic phononic systems.

Probing nanoscale ferroelectricity by ultraviolet Raman spectroscopy.

We demonstrated that ultraviolet Raman spectroscopy is an effective technique to measure the transition temperature (Tc) in ferroelectric ultrathin films and superlattices. We showed that one-unit-cell-thick BaTiO3 layers in BaTiO3/SrTiO3 superlattices are not only ferroelectric (with Tc as high as 250 kelvin) but also polarize the quantum paraelectric SrTiO3 layers adjacent to them. Tc was tuned by approximately 500 kelvin by varying the thicknesses of the BaTiO3 and SrTiO3 layers, revealing the essential roles of electrical and mechanical boundary conditions for nanoscale ferroelectricity.