RESUMEN

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. Those phases are, for increasing power, Larmor-like precession of the condensate pseudo-spins-a signature of continuous TC; locking of the frequency of precession to self-sustained coherent phonons-stabilized TC; and doubling of TC's period by phonons-a discrete TC with continuous excitation. These results establish microcavity polaritons as a platform for the investigation of time-broken symmetry in nonhermitian systems.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

RESUMEN

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.

Asunto(s)

Técnicas Biosensibles/métodos , Glucosa Oxidasa/química , Glucosa/química , Oro/química , Nanopartículas del Metal/química , Calibración , Técnicas Electroquímicas/métodos , Flavina-Adenina Dinucleótido/análogos & derivados , Flavina-Adenina Dinucleótido/química , Flavina-Adenina Dinucleótido/metabolismo , Glucosa/metabolismo , Glucosa Oxidasa/metabolismo , Microscopía de Fuerza Atómica , Microscopía Electrónica de Transmisión , Nanocables/química , Osmio/química , Espectrofotometría Ultravioleta , Espectrometría Raman/métodos

RESUMEN

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.

RESUMEN

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.

RESUMEN

We present a detailed structural and surface-enhanced Raman scattering (SERS) study of poly(allylamine) modified with Os(byp)2ClPyCHO (PAH-Os) and gold nanoparticles self-assembled multilayers [PAH-Os+(Au-nanoparticlesPAH-Os)n, n=1 and 5]. Atomic force microscopy and variable-angle spectroscopic ellipsometry measurements indicate that the first nanoparticle layer grows homogenously by partially covering the substrate without clustering. Analyzing the sample thickness and roughness we infer that the growth process advances thereafter by filling with nanoparticles the interstitial spaces between the previously adsorbed nanoparticles. After five immersion steps the multilayers reach a more compact structure. The interaction between plasmons of near-gold nanoparticles provides a new optical absorption around 650 nm which, in addition, allows a more effective SERS process in that spectral region than at the single-plasmon resonance (approximately 530 nm). We compare the electronic resonance Raman and SERS amplification mechanisms in these self-assembled multilayers analyzing Raman resonance scans and Raman intensity micromaps. As a function of nanoparticle coverage we observe large changes in the Raman intensity scans, with maxima that shift from the electronic transitions, to the plasmon resonance, and finally to the coupled-plasmon absorption. The Raman micromaps, on the other hand, evidence huge intensity inhomogeneities which we relate to "hot spots." Numerical discrete dipole approximation calculations including the interaction between gold nanoparticles are presented, providing a qualitative model for the coupled-plasmon absorption and redshifted Raman hot spots in these samples.

RESUMEN

We present a resonant Raman scattering study of (PAH--Os/PVS)n and (PAH--Os/GOx)m self-assembled multilayers (n=1-11 and m=1-3). These Os polymer multilayers can be used in electrodes as efficient molecular wires for biomolecular recognition. The Raman intensity dependence on the number of self-assembly cycles provides information on the deposition process. The spectra are identical to that observed for PAH--Os in aqueous solution, indicating that the PAH--Os metal complex structure is conserved in the multilayers. We observe at approximately 500 nm incoming and outgoing Raman resonances of osmium and bipyridine vibrational modes. These resonances are associated to the metal-to-ligand charge transfer (MLCT) transition. We study the evolution of these Raman modes as a function of the Os oxidation state during in situ electrochemistry. During the oxidation process, Os(II)-->Os(III), the Raman resonance related to the MLCT disappears and the bipyridine related modes harden by approximately 10 cm(-1). These results are correlated with optical transmission measurements which show the disappearance of the visible region absorption when the Os complex is oxidized. We also find partial quenching of the Raman mode intensity after in situ voltamperometric cycles which demonstrates the existence of photo-electro-chemical processes.

RESUMEN

Extending the idea of optical microcavities to sound waves, we propose a phonon cavity consisting of two semiconductor superlattices enclosing a spacer layer. We show that acoustical phonons can be confined in such layered structures when the spacer thickness is an integer multiple of the acoustic half-wavelength at the center of one of the superlattice folded minigaps. We report Raman scattering experiments that, taking profit of an optical microcavity geometry, demonstrate unambiguously the observation of a phonon-cavity confined acoustical vibration in a GaAs/AlAs based structure. The experimental results compare precisely with photoelastic model calculations of the Raman spectra.

RESUMEN

We report optical double resonant enhancement of Raman scattering in a new double microcavity geometry. The design allows almost backscattering geometries, providing easy access to the excitations' in-plane dispersion. The cavity is used to study the phonon spectra of a finite GaAs/AlAs superlattice. A new type of "standing optical vibration" is demonstrated involving the GaAs confined phonons with a standing wave envelope determined by the superlattice thickness. A strong dispersion of the first order standing wave mode is observed, as well as its anticrossing with higher order confined modes of the same symmetry.