Solid-state continuous time crystal in a polariton condensate with a built-in mechanical clock.

Time crystals (TCs) are many-body systems that display spontaneous breaking of time translation symmetry. We demonstrate a TC by using driven-dissipative condensates of microcavity exciton-polaritons, spontaneously formed from an incoherent particle bath. The TC phases are controlled by the power of a continuous-wave nonresonant optical drive exciting the condensate and the interaction with cavity phonons.

Microcavity phonoritons - a coherent optical-to-microwave interface.

Optomechanical systems provide a pathway for the bidirectional optical-to-microwave interconversion in (quantum) networks. These systems can be implemented using hybrid platforms, which efficiently couple optical photons and microwaves via intermediate agents, e.g.

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.

Optics in South America: introduction.

South American optics research has seen remarkable growth over the past 50 years, with significant contributions in areas such as quantum optics, holography, spectroscopy, nonlinear optics, statistical optics, nanophotonics and integrated photonics. The research has driven economic development in sectors like telecom, biophotonics, biometrics, and agri-sensing. This joint feature issue between JOSA A and JOSA B exhibits cutting-edge optics research from the region, fostering a sense of community and promoting collaboration among researchers.

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 lifetime of interlayer breathing modes of few-layer 2H-MoSe membranes.

A time-resolved observation of coherent interlayer longitudinal acoustic phonons in thin layers of 2H-MoSe2 is reported. A femtosecond pump-probe technique is used to investigate the evolution of the energy loss of these vibrational modes in a wide selection of MoSe2 flakes with different thicknesses ranging from bilayer up to the bulk limit. By directly analysing the temporal decay of the modes, we can clearly distinguish an abrupt crossover related to the acoustic mean free path of the phonons in a layered system, and the constraints imposed on the acoustic decay channels when reducing the dimensionality.

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.

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}.

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.

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.

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.

Silver nanoparticle-mesoporous oxide nanocomposite thin films: a platform for spatially homogeneous SERS-active substrates with enhanced stability.

We introduce a nanoparticle-mesoporous oxide thin film composite (NP-MOTF) as low-cost and straightforward sensing platforms for surface-enhanced Raman Spectroscopy (SERS). Titania, zirconia, and silica mesoporous matrices templated with Pluronics F-127 were synthesized via evaporation-induced self-assembly and loaded with homogeneously dispersed Ag nanoparticles by soft reduction or photoreduction. Both methods give rise to uniform and reproducible Raman signals using 4-mercaptopyridine as a probe molecule.

Fabry-Pérot-multichannel spectrometer tandem for ultra-high resolution Raman spectroscopy.

We present a novel ultra-high resolution Raman spectroscopy technique based in a Fabry-Pérot/triple spectrometer tandem with multichannel acquisition. We describe the system, detail the calibration process, and experimentally test the technique, showing that effective finesses in excess of 1000 are possible. The technique is specifically tailored for low intensity, complex and spectrally extended Raman spectra, providing shorter acquisition times with respect to similar tandem systems with monochannel detectors.

Strong correlation between molecular configurations and charge-transfer processes probed at the single-molecule level by surface-enhanced Raman scattering.

Single-molecule (SM) electrochemistry studied by surface-enhanced Raman scattering (SERS) with high spectral resolution reveals a picture in which the frequency of Raman modes is correlated with the electrochemical process through the interaction with the surface. Previously unexplored phenomena can be revealed by the synergy of electrochemistry and SM-SERS, which explores in this case subtler spectroscopic aspects (like the frequency of a vibration within the inhomogeneous broadening of a many-molecules Raman peak) to gain the information. We demonstrate, among other things, that the interaction with the surface is correlated both with the molecule vibrational frequencies and with the ability of single molecules to be reduced/oxidized at different potentials along the electrochemical cycle.

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.

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.

Self-assembly of thiolated cyanine aggregates on Au(111) and Au nanoparticle surfaces.

Heptamethinecyanine J-aggregates display sharp, intense fluorescence emission making them attractive candidates for developing a variety of chem-bio-sensing applications. They have been immobilized on planar thiol-covered Au surfaces and thiol-capped Au nanoparticles by weak molecular interactions. In this work the self-assembly of novel thiolated cyanine (CNN) on Au(111) and citrate-capped AuNPs from solutions containing monomers and J-aggregates has been studied by using STM, XPS, PM-IRRAS, electrochemical techniques and Raman spectroscopy.

From single to multiple Ag-layer modification of Au nanocavity substrates: a tunable probe of the chemical surface-enhanced Raman scattering mechanism.

We present experimental and computational results that enlighten the mechanisms underlying the chemical contribution to surface-enhanced Raman scattering (SERS). Gold void metallic arrays electrochemically covered either by a Ag monolayer or 10-100 Ag layers were modified with a self-assembled monolayer of 4-mercaptopyridine as a molecular Raman probe displaying a rich and unexpected Raman response. A resonant increase of the Raman intensity in the red part of the spectrum is observed that cannot be related to plasmon excitations of the cavity-array.

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.

Monitoring the electrochemistry of single molecules by surface-enhanced Raman spectroscopy.

Coherent control of chemical species in complex systems is always subject to intrinsic inhomogeneities from the environment. For example, slight chemical modifications can decisively affect transport properties of molecules on surfaces. Hence, single-molecule (SM) studies are the best solution to avoid these problems and to study diverse phenomena in biology, physics, and chemistry.

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.

Electrochemical modulation for signal discrimination in surface enhanced Raman scattering (SERS).

Electrochemical modulation to induce controlled fluctuations in SERS signals is introduced as a method to discriminate and isolate different contributions to the spectra. The modulation--which can be changed in potential range, amplitude, and frequency--acts as a controllable "switch" to turn on, off, or change specific Raman signals which can then be correlated within the spectra by different fluctuation analysis techniques. Principal component analysis (PCA), either by itself or assisted by fast fourier transform (FFT) prefiltering, are shown to provide viable tools to isolate the different components of the spectra.

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.

Ag-modified Au nanocavity SERS substrates.

The engineering of cavity void metallic arrays allows to vary the plasmon-polariton mode energies from the near infrared to the ultraviolet through the tuning of the void height and diameter, and the selection of the appropriate material. Typically Au nanocavity substrates can be grown with better reproducibility, homogeneity, and stability, while Ag structures display significantly larger SERS enhancements. To exploit these two apparently excluding aspects, quality and enhancement, we report a detailed study of 500 nm Au-nanocavity templates modified by the controlled electrochemical deposition of 100 Ag layers, a thickness similar to the visible light skin-depth of bulk Ag.

Redox molecule based SERS sensors.

We describe a general framework to design nanobiosensors based on a wired enzyme coupled to a redox molecule and integrated with SERS Au core-shell nanoparticles and ordered nanocavities. The response of the proposed sensor is based on the different electronic resonant Raman behavior of the oxidized or reduced electronic states of the molecular wire, and on the surface plasmon amplification induced by the tailored metallic substrate. The nanobiosensors can be interrogated remotely through the resonant Raman scattering intensity recovery or spectral variation of the redox molecule, an Os-complex, when the latter varies its oxidation state.